Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Bimetallic metal–organic frameworks (MOFs) offer unique synergistic properties and improved conductivity due to the integration of multiple metal components. However, their electrical and dielectric properties remain underexplored, and their charge transport mechanisms are not fully understood. This study investigates the electrical and dielectric properties of Mn‐BTC (BTC = benzene‐1,3,5‐tricarboxylic acid), Co‐BTC, and bimetallic Mn–Co BTC MOFs with varying Mn/Co ratios. Charge transport in these MOFs occurs via hopping at low frequencies, transitioning to lattice response at higher frequencies. While Mn incorporation typically reduces alternating current (AC) conductivity, the 1:2 Mn:Co MOF exhibits a unique conduction mechanism, enhancing AC conductivity by 25%. As electrocatalysts for oxygen evolution reaction (OER), the 1:2 Mn:Co MOF outperforms Mn‐BTC, Co‐BTC, and other Mn‐Co BTC variants, achieving a lower overpotential (359 mV) and Tafel slope (71 mV dec⁻¹). The correlation between AC conductivity and electrocatalytic performance underscores the critical role of electrical properties in MOF functionality. This study highlights the potential of tailoring the electrical properties of bimetallic MOFs to optimize their electrocatalytic performance, offering valuable insights for future catalyst design.

DOI： 10.1002/aesr.202300301

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1038/s44221-025-00391-1

Other Link： https://www.nature.com/articles/s44221-025-00391-1

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Tin halide perovskites are promising candidates for lead‐free perovskite solar cells due to their ideal bandgap and high charge‐carrier mobility. However, poor crystal quality and rapid degradation in ambient conditions severely limit their stability and practical applications. This study demonstrates that incorporating UiO‐66, a zirconium‐based MOF, significantly enhances the performance and stability of tin halide perovskite solar cells (TPSCs). The unique porous structure and abundant carboxylate groups of UiO‐66 improve the crystallinity and film quality of FASnI₃, reduce defect density, and prolong charge carrier lifetimes. Consequently, the power conversion efficiency (PCE) of UiO‐66‐integrated TPSCs increases from 11.43% to 12.64%, and the devices maintain over 90% of their initial PCE after 100 days in a nitrogen glovebox. These findings highlight the potential of UiO‐66 in addressing the efficiency and stability challenges of tin halide perovskites.

DOI： 10.1002/smll.202411346

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1038/s41557-024-01727-2

Other Link： https://www.nature.com/articles/s41557-024-01727-2

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Copper‐based electrocatalysts are recognized as crucial catalysts for CO₂ electroreduction into multi‐carbon products. However, achieving copper‐based electrocatalysts with adjustable valences via one‐step facile synthesis remains a challenge. In this study, Cu/Cu₂O heterostructure is constructed by adjusting the anion species of the Cu ions‐containing electrolyte during electrodeposition synthesis. Then, Cu/Cu₂O with tuned nanoarchitectures ranging from dendrites to polyhedrons is achieved by introducing transition metal ions as additives, leading to an adjustable interfacial microenvironment for CO₂/H₂O adsorption on the Cu/Cu₂O electrodes. Additionally, the polyhedral Cu/Cu₂O catalysts are used as templates for depositing Ag single atoms (Ag_SA), which are known as synergistic active sites for promoting ^*CO to ^*COH toward C₂₊ products. The prepared Ag_SA‐Cu/Cu₂O catalyst is evaluated in a flow cell and exhibited a FE_C2+ of 90.2% and a partial current density (jc₂₊) of 426.6 mA cm⁻² for CO₂ electroreduction. As revealed by in situ Raman spectra and density functional theory calculations, the introduction of Ag single atoms slows down the reduction of Cu⁺ during CO₂ electroreduction, especially at a high current density. This work provides a promising paradigm for diverse control of the compositions and hydrophobicity of Cu‐based catalysts for selective CO₂ electroreduction to C₂₊ products.

DOI： 10.1002/adma.202411498

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Oxford University Press (OUP)  

Abstract

Incorporating mesoporous structures into various materials can provide abundant active sites and facilitate smooth diffusion, and their effectiveness has been demonstrated across a range of material types. However, despite the development of numerous mesoporous materials, first-generation mesoporous materials (e.g., silica-based compositions) have limited applications due to their poor electrical conductivity and limited compositional diversity, necessitating additional processing for widespread utilization. Our group first proposed the synthesis of mesoporous metals using a solution-based soft-templating method based on self-assembly of micelles, marking a significant advancement in mesoporous materials. This effective process has recently been extended to the synthesis of mesoporous metals and chalcogenides. Chalcogenides have garnered significant attention due to their intriguing optical, electrical, and electrochemical properties arising from their distinctive electronic structures. Mesoporous chalcogenides have been found to effectively enhance these properties. This paper provides a comprehensive review of the synthesis of mesoporous metals and chalcogenides—representing second-generation mesoporous materials (mesoporous materials 2.0)—with specific examples. Our goal is to inform readers about second-generation mesoporous materials and provide insights for further research.

DOI： 10.1093/bulcsj/uoae136

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acselectrochem.4c00056

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.ccr.2024.216199

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.matchemphys.2024.130120

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Chinese Chemical Society  

DOI： 10.31635/ccschem.024.202404641

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2025.159270

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.ccr.2024.216264

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Unique mesoporous Au NPs improved the capacitance, electrical conductivity, cycling stability and photocurrent response of MXene-based film electrodes.

DOI： 10.1039/d4ta06043a

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

In this work, a unique 2D hollow turtle shell‐like mesoporous carbon (HTMC) synthesized via a ternary heterostructuring strategy to alleviate the restacking tendency of 2D materials is presented. The ternary 2D heterostructuring is achieved via an in situ growth of zeolitic imidazolate framework‐8 (ZIF‐8) on graphene oxide (GO) and a subsequent mesostructured polydopamine (mPDA) coating to obtain ternary heterostructured GO@ZIF‐8@mPDA, which is then converted to the hierarchically porous HTMC having macro‐, meso‐, and micropores via direct carbonization. Additionally, 2D turtle shell‐like microporous carbon (TMC) and 2D mesoporous carbon (MPC) derived from binary heterostructured GO@ZIF‐8 and GO@mPDA, respectively, are synthesized to investigate the porosity effect on alleviating the loss of accessible surface area of restacked 2D carbons. Among them, HTMC demonstrates superior structural advantages for alleviating the negative effects of restacking in 2D materials, exhibiting by far the highest specific capacitance (C_sp) across all scan rates (93.7 F g⁻¹ at 500 mV s⁻¹ to 334.47 F g⁻¹ at 1 mV s⁻¹) in 1 M H₂SO₄. Furthermore, HTMC demonstrates outstanding rate capability while maintaining the greatest charge storage capacity over all scan rates.

DOI： 10.1002/smll.202406174

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Dry reforming of methane (DRM) represents an important way to convert both CO₂ and CH₄ to reduce greenhouse effects and produce valuable chemical products. Owing to the strong bonding energies of both CO₂ and CH₄ molecules, DRM usually proceeds at a high temperature, which inevitably causes catalyst sintering, leading to catalyst deactivation. This work develops a highly stable sub‐nanometer Ru catalyst on a Ni‐doped MgO support using Mg²⁺ vacancies as anchors. The optimized Ru_1.5/Ni₁‐MgO‐R catalyst displays 90% CH₄ conversion and 92% CO₂ conversion to syngas in DRM at 800 °C. More importantly, it exhibits strong durability and can run continuously for more than 1200 h. Both the characterizations and the density functional theory (DFT) calculations demonstrate that the Ni²⁺ substituted Mg²⁺ in the MgO matrix produces Mg²⁺ vacancies (Mg_V), which can stabilize sub‐nanometer Ru clusters of ≈0.9 nm. Moreover, the presence of Mg_v‐Ru₈ clusters strongly stabilizes sub‐nanometer Ru. This study contributes valuable insights into the design of sub‐nanometer metal catalysts with strong sintering resistance at high temperatures.

DOI： 10.1002/aenm.202404936

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Uranium extraction from seawater (UES) is crucial for ensuring the sustainable development of nuclear power and has seen significant advancements in recent years. However, natural seawater is a highly complex biogeochemical system, characterized by an extremely low uranium (U) concentration (≈3.3 µg L⁻¹), abundant competitive ions, and significant marine biological pollution, making UES a formidable challenge. This review addresses the challenges encountered in UES and explores potential methods for enhancing the industrial UES system, including membrane separation, electrochemistry, photocatalysis, and biosorption. Additionally, several representative marine tests are summarized and restrictive factors of large‐scale UES are analyzed. Finally, the further development of UES from laboratory to industry applications is promoted, with a focus on technological innovation. The goal is to stimulate innovative ideas and provide fresh insights for the future development of the UES system, bridging the gap between laboratory research and industrial implementation.

DOI： 10.1002/smtd.202401598

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Rare‐earth‐doped all‐inorganic perovskite applications for near‐infrared (NIR) emission are crucial for the construction of the next generation of intelligent lighting sources. However, the preparation of rare‐earth‐doped all‐inorganic perovskite is complex, and difficult to control, and the issue of thermal quenching poses significant challenges to its practical application. Here, in order to address these issues, a convenient photo‐induced synthesis method for CsPbCl₃:Mn/Yb nanocrystals (NCs) is proposed by decomposing carbon tetrachloride with 365 nm light to provide chloride ions and regulate the formation of perovskite at room temperature. The negative thermal quenching in the NIR emission is achieved through the energy transfer between Mn and Yb. The emission intensity of Yb enhances 3.2 times when the temperature rises to ≈427 K. Furthermore, with the help of the orange emission from the Mn²⁺ ions and the NIR emission from the Yb³⁺ ions, visible to NIR light emitting diode (LED) devices are constructed and applied in orange light illumination and night vision imaging. This study enriches the preparation methods and chemical research on perovskite doping, which may open up new opportunities for the widespread application of perovskite‐based materials or device engineering.

DOI： 10.1002/advs.202408927

PubMed

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.ccr.2024.216100

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.nanoen.2024.110244

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.nanoms.2024.01.010

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1038/s44221-024-00340-4

Other Link： https://www.nature.com/articles/s44221-024-00340-4

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The remarkable properties of 2D nanomaterials are well known. However, their high interfacial adhesion energy often leads to restacking issues, limiting their potential in various applications. A strategic synthetic approach is presented to overcome this challenge. Specifically, the study first demonstrates the use of layered aluminosilicate as a sacrificial 2D template to allow the growth of highly ordered meso‐holey polymeric layers, which can be subsequently exfoliated upon the removal of aluminosilicate and thermally converted to perpendicularly open meso‐holey carbon (POMC). On the other hand, perpendicularly blocked meso‐holey carbon (PBMC) is obtained with non‐sacrificial 2D template of graphene oxide. When both POMC and PBMC are evaluated by operando hydrodynamic electrochemical impedance spectroscopy and transmission line model analysis for electrochemical reduction of oxygen, POMC achieves a remarkable improvement of charge transfer and mass transfer by up to 4.1 and 7.9 times, respectively, as compared to PBMC. This study therefore highlights the importance of perpendicularly open 2D nanoarchitectures in circumventing the restacking effect, offering valuable insights for leveraging 2D nanomaterials with open meso‐holes in various applications.

DOI： 10.1002/advs.202409546

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1038/s41467-024-53174-9

Other Link： https://www.nature.com/articles/s41467-024-53174-9

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsanm.4c04249

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Covalent organic frameworks (COFs) are promising high-performance capacitive deionization (CDI) materials. Strategies to optimize CDI performance of COFs focus largely on hybridization with conductive substrates, to improve their their intrinsically poor conductivity. A new structure-function relationship between COFs and their substrates is proposed here based on substrate-induced surface curvature. Graphene (zero-curvature) and carbon nanotubes (CNT, curved) are selected as COF growthsubstrates to assess the effect of curvature engineering effect on CDI performance of TpPa-SO3H-COF. Ultrahigh ion (Na+) adsorption capacity (58.74 mg g−1) is achieved by CNT-COF hybrid (cf. compared to graphene-COF hybrid 34.20 mg g−1), demonstrating the significance of curvature engineering. Notably, the corresponding salt (NaCl) adsorption capacity of CNT-COF hybrid reaches 149.25 mg g−1 in 1000 ppm at 1.2 V, representing state-of-the-art CDI performance, and the highest value among organic CDI electrodes. X-ray photoelectron spectroscopy and theoretical calculations subsequently reveal that substrate curvature can induce local strain, which regulates charge distribution within the COF skeleton, causing a lower binding energy state for Na+ adsorption. Electrochemical quartz crystal microbalance measurements revealed faster Na+ adsorption kinetics of CNT-COF due to regulated charge distribution within COF skeleton induced by substrate curvature. This work gives new insight into design of COF materials based on curvature engineering.

DOI： 10.1002/adfm.202407479

Scopus

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：AIP Publishing  

This review aims to offer strategic synthesis of new carbon materials under the thematic concept of “nanoarchitectonics” applied to metal-organic framework (MOF)-derived porous carbons. The background tracing of carbon materials in terms of the development of carbon microstructure is outlined first to offer the microstructural level of understanding of traditional carbons as well as recent MOF-derived porous carbons. Subsequently, we present the discussion on the effect of nanopore size on the formation of an electrical double layer, and justify the electrochemical rationale behind the need for nanoarchitecturing of porous carbon materials. Traditional synthetic strategies of template-free and template-based methods and the previous porous carbon materials are also discussed as the potential synthetic methods and approaches available for nanoarchitecturing of MOF-derived porous carbons. Various examples of nanoarchitectured MOF-derived porous carbons are then presented and discussed based on the careful categorization into template-free methods including bottom–up and top–down approaches and template-based methods including hard- and soft-template approaches. This review therefore aims to summarize and extend the current knowledge of nanoarchitectured MOF-derived porous carbons to offer intuitions and innovations toward future carbon materials. We also offer future directions with considerations on the challenges and innovations in the current field of nanoarchitectured MOF-derived porous carbons.

DOI： 10.1063/5.0213150

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2024.156429

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cclet.2024.110659

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.ccr.2024.215923

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jallcom.2024.175215

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Oxford University Press (OUP)  

Abstract

Mesoporous alumina spherical particles, synthesized via spray-drying with the self-assembly of EOnPOmEOn, have been utilized for the development of clinical-grade molybdenum-99/technetium-99 m (99Mo/99mTc) generators. When evaluated as molybdenum (Mo) adsorbents, the mesoporous alumina spherical particles are useful for effective adsorption of Mo ions rather than commercially available particulate alumina. The effects of surfactant removal methods on the Mo adsorption property are also systematically investigated using the batch method. Batch adsorption studies reveal practical adsorption capacities ranging from 45.9 to 91.2 mg Mo g−1 in a Mo solution (1000 mg Mo L−1) at pH 3. The experimental results indicate the following trend in Mo adsorption capacity: solvent extraction >calcination (400 °C and 800 °C) >commercially available alumina (Medical Al2O3 used as is). To explore the feasibility of developing a clinical-scale generator, a novel tandem column generator concept is employed. Using the spray-dried and extracted mesoporous alumina, 99mTc eluted from the generator exhibits high radionuclidic, radiochemical, and chemical purity, making it suitable for the preparation of 99mTc-labeled radiopharmaceuticals.

DOI： 10.1093/bulcsj/uoae099

Other Link： https://academic.oup.com/bcsj/article-pdf/97/10/uoae099/60626749/uoae099.pdf

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The interlayer stacking modes of 2D covalent‐organic frameworks (COFs) directly influence their structural features, ultimately determining their functional output. However, controllably modulating the interlayer stacking structure in traditional 2D metal‐free COFs, based on the same building blocks, remains challenging. Here, two trinuclear copper organic frameworks are synthesized successfully with different interlayer stacking structures: eclipsed AA stacking in Cu₃‐PA‐COF‐AA and staggered ABC stacking in Cu₃‐PA‐COF‐ABC, using the same monomers. Remarkably, various functionalities, including porosity and electronic and optical properties, can be effectively regulated by interlayer stacking. As a result, Cu₃‐PA‐COF‐AA and Cu₃‐PA‐COF‐ABC exhibit significantly different activities toward the photoreduction of U(VI), presenting a promising strategy for removing radioactive uranium pollution. Due to its broader visible‐light absorption range and superior photogenerated carrier migration and separation efficiency, Cu₃‐PA‐COF‐AA achieves a U(VI) removal ratio of 93.6% without additional sacrificial agents in an air atmosphere—≈2.2 times higher than that of Cu₃‐PA‐COF‐ABC (42.0%). To the best of the knowledge, this is the first study to elucidate the effect of interlayer stacking in COFs on the photocatalytic activity of U(VI) reduction. This finding may inspire further exploration of the structure‐function relationship in COFs as photocatalysts and their potential for photoinduced removal of radionuclides.

DOI： 10.1002/advs.202406530

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

High-entropy alloys (HEAs) are promising materials for electrochemical energy applications due to their excellent catalytic performance and durability. However, the controlled synthesis of HEAs with a well-defined structure and a uniform composition distribution remains a challenge. Herein, a soft template-assisted electrodeposition technique is used to fabricate a mesoporous HEA (m-HEA) film with a uniform composition distribution of Pt, Pd, Rh, Ru, and Cu, providing a suitable platform for investigating structure-performance relationships. Electrochemical deposition enables the uniform nucleation and grain growth of m-HEA, which can be deposited onto many conductive substrates. The m-HEA film exhibits an enhanced mass activity of 4.2 A mgPt-1 toward methanol oxidation reaction (MOR), which is 7.2-fold and 35-fold higher than a mesoporous Pt film and commercial Pt black, respectively. Experimental characterization indicates that structural defects and a low work function of the m-HEA film offer sufficient active sites and fast electron-transfer kinetics. Furthermore, theoretical calculations demonstrate that the variety of favorable adsorption sites on multimetallic elements of HEA reduces the barriers for dehydration pathways and *CO species removal, ensuring optimal performance for complex MOR reactions. This work provides an effective approach to designing a variety of HEA catalysts with well-controlled porous structures for targeted electrocatalytic applications.

DOI： 10.1021/acsnano.4c08929

Scopus

PubMed

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Perovskite oxides are considered highly promising candidates for oxygen evolution reaction (OER) catalysts due to their low cost and adaptable electronic structure. However, modulating the electronic structure of catalysts without altering their nanomorphology is crucial for understanding the structure‐property relationship. In this study, a simple plasma bombardment strategy is developed to optimize the catalytic activity of perovskite oxides. Experimental characterization of plasma‐treated LaCo_0.9Fe_0.1O₃ (P‐LCFO) reveals abundant oxygen vacancies, which expose numerous active sites. Additionally, X‐ray photoelectron spectroscopy and X‐ray absorption fine structure analyses indicate a low Co valence state in P‐LCFO, likely due to the presence of these oxygen vacancies, which contributes to an optimized electronic structure that enhances OER performance. Consequently, P‐LCFO exhibits significantly improved OER catalytic activity, with a low overpotential of 294 mV at a current density of 10 mA cm⁻², outperforming commercial RuO₂. This work underscores the benefits of plasma engineering for studying structure‐property relationships and developing highly active perovskite oxide catalysts for water splitting.

DOI： 10.1002/smll.202404239

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2024.153714

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.apcatb.2024.123902

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.4c02036

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsami.4c09747

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.4c01416

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Oxford University Press (OUP)  

Abstract

Capacitive deionization is an efficient and cost-effective technology for ion removal from brackish water. Here, we demonstrate a sulfonate-functionalized covalent organic framework as a novel faradaic cathode material for capacitive deionization applications. Due to its orderly arranged adsorption units in the covalent organic framework, the resulting covalent organic framework demonstrates a superior sodium cations removal capacity of 19.56 mg g−1 and a maximum desalination rate of 3.15 mg g−1 s−1 in a 500 ppm NaCl solution at 1.2 V.

DOI： 10.1093/bulcsj/uoae074

Other Link： https://academic.oup.com/bcsj/article-pdf/97/9/uoae074/59068833/uoae074.pdf

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

High Entropy Alloys (HEAs) are a versatile material with unique properties, tailored for various applications. They enable pH‐sensitive electrocatalytic transformations like hydrogen evolution reaction (HER) and hydrogen oxidation reactions (HOR) in alkaline media. Mesoporous nanostructures with high surface area are preferred for these electrochemical reactions, but designing mesoporous HEA sis challenging. To overcome this challenge, a low‐temperature triblock copolymer‐assisted wet‐chemical approach is developed to produce mesoporous HEA nanospheres composed of PtPdRuMoNi systems with sufficient entropic mixing. Owing to active sites with inherent entropic effect, mesoporous features, and increased accessibility, optimized HEA nanospheres promote strong HER/HOR performance in alkaline medium. At 30 mV nominal overpotential, it exhibits a mass activity of ≈167 (HER) and 151 A g_Pt⁻¹ (HOR), far exceeding commercial Pt‐C electrocatalysts (34 and 48 A g_Pt⁻¹) and many recently reported various alloys. The Mott‐Schottky analysis reveals HEA nanospheres inherit high charge carrier density, positive flat band potential, and smaller charge transfer barrier, resulting in better activity and faster kinetics. This micelle‐assisted synthetic enable the exploration of the compositional and configurational spaces of HEAs at relatively low temperature, while simultaneously facilitating the introduction of mesoporous nanostructures for a wide range of catalytic applications.

DOI： 10.1002/advs.202402518

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Flexible porous materials have gained considerable interest for their potential applications in selective absorption and controlled release/storage of specific molecules or compounds. Here, nanoscrolls are proposed as a type of inorganic solids with reversibly flexible mesopores. Nanoscrolls exhibit a rolled‐up structure composed of nanosheets with a 1D rod‐like morphology, possessing two distinct nanospaces. The first space comprises 1D tubular mesopores located at the center of the rod, while the second space exists in the interlayer regions on the wall of the mesopore, resulting from the layer stacking caused by the scrolling of nanosheets. By replacing the interlayer cations on the nanoscroll walls with other cations, a drastic alteration in the size of the 1D mesopores is observed. For instance, exchanging bulky dodecylammonium cations with small NH₄⁺ cations leads to a substantial change in pore size, with differences ranging from 10 to 20 nm—a notably larger variation compared to previous reports on flexible porous materials. Importantly, the alteration of pore size induced by the exchange reaction is found to be reversible. This reversible alteration in pore size holds promise for applications in host–guest chemistry involving large moieties such as nanoparticles and enzymes.

DOI： 10.1002/smll.202403814

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.nanolett.4c02178

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Osmotic energy, often referred to as “blue energy”, is the energy generated from the mixing of solutions with different salt concentrations, offering a vast, renewable, and environmentally friendly energy resource. The efficacy of osmotic power production considerably relies on the performance of the transmembrane process, which depends on ionic conductivity and the capability to differentiate between positive and negative ions. Recent advancements have led to the development of membrane materials featuring precisely tailored ion transport nanochannels, enabling high‐efficiency osmotic energy harvesting. In this review, ion diffusion in confined nanochannels and the rational design and optimization of membrane architecture are explored. Furthermore, structural optimization of the membrane to mitigate transport resistance and the concentration polarization effect for enhancing osmotic energy harvesting is highlighted. Finally, an outlook on the challenges that lie ahead is provided, and the potential applications of osmotic energy conversion are outlined. This review offers a comprehensive viewpoint on the evolving prospects of osmotic energy conversion.

DOI： 10.1002/adma.202404418

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Electrocatalytic water splitting driven by sustainable energy is a clean and promising water‐chemical fuel conversion technology for the production of high‐purity green hydrogen. However, the sluggish kinetics of anodic oxygen evolution reaction (OER) pose challenges for large‐scale hydrogen production, limiting its efficiency and safety. Recently, the anodic OER has been replaced by a nucleophilic oxidation reaction (NOR) with biomass as the substrate and coupled with a hydrogen evolution reaction (HER), which has attracted great interest. Anode NOR offers faster kinetics, generates high‐value products, and reduces energy consumption. By coupling NOR with hydrogen evolution reaction, hydrogen production efficiency can be enhanced while yielding high‐value oxidation products or degrading pollutants. Therefore, NOR‐coupled HER hydrogen production is another new green electrolytic hydrogen production strategy after electrolytic water hydrogen production, which is of great significance for realizing sustainable energy development and global decarbonization. This review explores the potential of nucleophilic oxidation reactions as an alternative to OER and delves into NOR mechanisms, guiding future research in NOR‐coupled hydrogen production. It assesses different NOR‐coupled production methods, analyzing reaction pathways and catalyst effects. Furthermore, it evaluates the role of electrolyzers in industrialized NOR‐coupled hydrogen production and discusses future prospects and challenges. This comprehensive review aims to advance efficient and economical large‐scale hydrogen production.

DOI： 10.1002/adma.202404806

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Constructing dual‐site catalysts consisting of atomically dispersed metal single atoms and metal atomic clusters (MACs) is a promising approach to further boost the catalytic activity for oxygen reduction reaction (ORR). Herein, a porous Co_SA‐AC@SNC featuring the coexistence of Co single‐atom sites (CoN₄) and S‐coordinated Co atomic clusters (SCo₆) in S, N co‐doped carbon substrate is successfully synthesized by using porphyrinic metal‐organic framework (Co‐TPyP MOF) as the precursor. The introduction of the sulfur source creates abundant microstructural defects to anchor Co metal clusters, thus modulating the electronic structure of its surrounding carbon substrate. The synergistic effect between the two types of active sites and structural advantages, in turn, results in high ORR performance of Co_SA‐AC@SNC with half‐wave potential (E_1/2) of 0.86 V and Tafel slope of 50.17 mV dec⁻¹. Density functional theory (DFT) calculations also support the synergistic effect between CoN₄ and SCo₆ by detailing the catalytic mechanism for the improved ORR performance. The as‐fabricated Zn–air battery (ZAB) using Co_SA‐AC@SNC demonstrates impressive peak power density of 174.1 mW cm⁻² and charge/discharge durability for 148 h. This work provides a facile synthesis route for dual‐site catalysts and can be extended to the development of other efficient atomically dispersed metal‐based electrocatalysts.

DOI： 10.1002/smll.202402323

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/jacs.4c02321

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.4c04174

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Mesoporous materials find widespread applications due to their high specific surface area, contributing to enhanced performance. Scanning electron microscopy (SEM) observation of mesoporous materials provides valuable insights into their mesostructures. However, direct observation of the outermost surfaces, which often dictate material properties, remains challenging, especially for highly insulating and fragile compounds. In this study, utilizing SEM observation with ultra‐low‐voltage acceleration directed by Gemini column is proposed to achieve direct surface imaging of mesoporous organic materials with highly insulating and fragile characteristics. By observing mesostructured polymers obtained through a soft‐templating method without washing, stuffed pores are identified allowing the differentiation of micelle templates and polymer walls. Moreover, leveraging SEM measurements, a polymerization mechanism is proposed for dopamine on the polymer micelles adhered to the graphene oxide nanosheets. These findings demonstrate the potential of SEM measurements with ultra‐low accelerating voltage in facilitating surface observations of polymer‐derived nanomaterials characterized by high insulating properties and a fragile framework.

DOI： 10.1002/admi.202400247

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jma.2024.06.026

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2024.152124

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The rational design of efficient catalysts for uric acid (UA) electrooxidation, as well as the establishment of structure‐activity relationships, remains a critical bottleneck in the field of electrochemical sensing. To address these challenges, herein, a hybrid catalyst that integrates carbon‐supported Pt nanoparticles and nitrogen‐coordinated Mn single atoms (Pt_NPs/MnNC) is developed. The metal‐metal interaction during annealing affords the construction of metallic‐bonded Pt−Mn pairs between Pt_NPs and Mn single atoms, facilitating the electron transfer from Pt_NPs to the support and thereby optimizing the electronic structure of catalysts. More importantly, experiments and theoretical calculations provide visual proof for the ‘incipient hydrous oxide adatom mediator’ mechanism for UA oxidation. The Pt−Mn pairs first adsorb OH* to construct the bridged Pt−OH−Mn mediators to serve as a highly active intermediate for N−H bond dissociation and proton transfer. Benefiting from the unique electronic and geometric structure of the catalytic center and reactive intermediates, Pt_NPs/MnNC exhibits superior electrooxidation performance. The electrochemical sensor based on Pt_NPs/MnNC enables sensitive detection and discrimination of UA and dopamine in serum samples. This work offers new insights into the construction of novel electrocatalysts for sensitive sensing platforms.

DOI： 10.1002/ange.202405571

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Association for the Advancement of Science (AAAS)  

Atomically dispersed Pt-group metals are promising as nanocatalysts because of their unique geometric structures and ultrahigh atomic utilization. However, loading isolated Pt-group metals in single-atom alloys (SAAs) with distinctive bimetallic sites is challenging. In this study, we present amorphous mesoporous Ni boride (Ni-B) as an ideal substrate to uniformly disperse Pt atoms with tunable loadings (1.7 to 12.2 wt %). The effect of the morphology, composition, and crystal phase of the Ni-B host on the growth and dispersion of Pt atoms is discussed. The resulting amorphous Pt-Ni-B mesoporous nanospheres exhibit superior electrocatalytic H ₂ evolution performance in acidic media. This strategy holds the potential to synthesize a diverse library of mesoporous amorphous Pt-group SAAs, by leveraging functional amorphous nanostructured 3 d transition-metal borides as substrates, thereby proposing a comprehensive strategy to control atomically dispersed Pt-group metals.

DOI： 10.1126/sciadv.ado2442

Scopus

PubMed

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Nanotechnology‐inspired small‐sized water‐enabled electricity generation (WEG) has sparked widespread research interest, especially when applied as an electricity source for off‐grid low‐power electronic equipment and systems. Currently, WEG encompasses a wide range of physical phenomena, generator structures, and power generation environments. However, a systematic framework to clearly describe the connections and differences between these technologies is unavailable. In this review, a comprehensive overview of generator technologies and the typical mechanisms for harvesting water energy is provided. Considering the different roles of water in WEG processes, the related technologies are presented as two different scenarios. Moreover, a detailed analysis of the electrical potential formation in each WEG process is presented, and their similarities and differences are elucidated. Furthermore, a comprehensive compilation of advanced generator architectures and system designs based on hydrological cycle processes is presented, along with their respective energy efficiencies. These nanotechnology‐inspired small‐sized WEG devices show considerable potential for applications in the Internet of Things ecosystem (i.e., microelectronic devices, integrated circuits, and smart clothing). Finally, the prospects and future challenges of WEG devices are also summarized.

DOI： 10.1002/sus2.206

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acssensors.4c00192

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

Abstract

Low-cost detection systems are needed for the identification of microplastics (MPs) in environmental samples. However, their rapid identification is hindered by the need for complex isolation and pre-treatment methods. This study describes a comprehensive sensing platform to identify MPs in environmental samples without requiring independent separation or pre-treatment protocols. It leverages the physicochemical properties of macroporous-mesoporous silver (Ag) substrates templated with self-assembled polymeric micelles to concurrently separate and analyze multiple MP targets using surface-enhanced Raman spectroscopy (SERS). The hydrophobic layer on Ag aids in stabilizing the nanostructures in the environment and mitigates biofouling. To monitor complex samples with multiple MPs and to demultiplex numerous overlapping patterns, we develop a neural network (NN) algorithm called SpecATNet that employs a self-attention mechanism to resolve the complex dependencies and patterns in SERS data to identify six common types of MPs: polystyrene, polyethylene, polymethylmethacrylate, polytetrafluoroethylene, nylon, and polyethylene terephthalate. SpecATNet uses multi-label classification to analyze multi-component mixtures even in the presence of various interference agents. The combination of macroporous-mesoporous Ag substrates and self-attention-based NN technology holds potential to enable field monitoring of MPs by generating rich datasets that machines can interpret and analyze.

DOI： 10.1038/s41467-024-48148-w

Other Link： https://www.nature.com/articles/s41467-024-48148-w

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsanm.4c01350

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsami.4c01881

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Ammonia borane (AB) with 19.6 wt % H₂ content is widely considered a safe and efficient medium for H₂ storage and release. Co‐based nanocatalysts present strong contenders for replacing precious metal‐based catalysts in AB hydrolysis due to their high activity and cost‐effectiveness. However, precisely adjusting the active centers and surface properties of Co‐based nanomaterials to enhance their activity, as well as suppressing the migration and loss of metal atoms to improve their stability, presents many challenges. In this study, mesoporous‐silica‐confined bimetallic Co−Cu nanoparticles embedded in nitrogen‐doped carbon (Co_xCu_1−x@NC@mSiO₂) were synthesized using a facile mSiO₂‐confined thermal pyrolysis strategy. The obtained product, an optimized Co_0.8Cu_0.2@NC@mSiO₂ catalyst, exhibits enhanced performance with a turnover frequency of 240.9 mol_H2 ⋅ mol_metal ⋅ min⁻¹ for AB hydrolysis at 298 K, surpassing most noble‐metal‐free catalysts. Moreover, Co_0.8Cu_0.2@NC@mSiO₂ demonstrates magnetic recyclability and extraordinary stability, with a negligible decline of only 0.8 % over 30 cycles of use. This enhanced performance was attributed to the synergistic effect between Co and Cu, as well as silica confinement. This work proposes a promising method for constructing noble‐metal‐free catalysts for AB hydrolysis.

DOI： 10.1002/ange.202404505

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Tailoring the surface structure of the mesoporous metal catalysts is pivotal for influencing both the catalytic activity and selectivity. Through the dealloying of bimetallic alloys, surface modification is achieved by dissolving unstable components, thereby forming a multitude of catalytically active sites. In this study, highly enhanced electrocatalysts are fabricated via chemical etching of mesoporous AuCu alloy nanoparticles prepared through the self‐assembly of micelles. The presence of large mesoporosity (>10 nm) with rich defect sites on the surface, along with the synergistic effect arising from the AuCu bimetallic alloy, effectively boosts electrocatalytic performance for the ethanol oxidation reaction. This strategy demonstrates a promising strategy to further enhance the catalytic performance of Au‐based mesoporous nanoparticles by eliminating the unstable metal component and refining the mesoporous structure with an abundance of various active sites.

DOI： 10.1002/sstr.202400021

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The chemical/physical properties and reliable performance of nanoporous materials are strongly influenced by the particle size and corresponding distribution. Among many types of MOFs, ZIF‐8, is still widely used and many studies have been conducted to control the particle size and uniformity of ZIF‐8 using surfactants and organic solvents. However, the use of surfactants and organic solvents process is expensive and may cause environmental pollution. For the first time, in this paper, a surfactant‐free, size‐controllable, and scalable green synthesis method of ZIF‐8 particles is reported using four reaction parameters (temperature, concentration, pouring time, and reactant ratio) that affect the formation of nuclei and growth of ZIF‐8 crystals. The as‐synthesized ZIF‐8 nanoparticles show great uniformity and controllable particle sizes in the wide range of 147–915 nm. In addition, a 2 L large‐scale synthesis of ZIF‐8 with narrow size distribution is developed by finely tuned particle size in water without any additives. To demonstrate the efficient utilization of nanopores according to the particle size and size distribution, an adsorption test is conducted on the ZIF‐8 nanoparticles. This study will support the synthesis of size‐controlled ZIF‐8 with narrow size distribution and their composites for achieving high performance in the emerging applications.

DOI： 10.1002/smtd.202400236

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Understanding the growth of mesoporous crystalline materials, such as mesoporous metals, on different substrates can provide valuable insights into the crystal growth dynamics and the redox reactions that influence their electrochemical sensing performance. Herein, it is demonstrated how the amorphous nature of the glass substrate can suppress the typical <111> oriented growth in mesoporous Au (mAu) films. The suppressed <111> growth is manifested as an accumulation of strain, leading to the generation of abundant surface defects, which are beneficial for enhancing the electrochemical activity. The fine structuring attained enables dramatically accelerated diffusion and enhances the electrochemical sensing performance for disease‐specific biomolecules. As a proof‐of‐concept, the as‐fabricated glass‐grown mAu film demonstrates high sensitivity in electrochemical detection of SARS‐CoV‐2‐specific RNA with a limit of detection (LoD) as low as 1 attomolar (aM).

DOI： 10.1002/smll.202311645

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c11547

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The utilization of solar‐thermal energy and universal cold energy has led to many innovative designs that achieve effective temperature regulation in different application scenarios. Numerous studies on passive solar heating and radiation cooling often operate independently (or actively control the conversion) and lack a cohesive framework for deep connections. This work provides a concise overview of the recent breakthroughs in solar heating and radiation cooling by employing a mechanism material in the application model. Furthermore, the utilization of dynamic Janus‐like behavior serves as a novel nexus to elucidate the relationship between solar heating and radiation cooling, allowing for the analysis of dynamic conversion strategies across various applications. Additionally, special discussions are provided to address specific requirements in diverse applications, such as optimizing light transmission for clothing or window glass. Finally, the challenges and opportunities associated with the development of solar heating and radiation cooling applications are underscored, which hold immense potential for substantial carbon emission reduction and environmental preservation. This work aims to ignite interest and lay a solid foundation for researchers to conduct in‐depth studies on effective and self‐adaptive regulation of cooling and heating.

DOI： 10.1002/smll.202309397

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c08486

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.apcatb.2023.123584

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2024.150112

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：MDPI AG  

The contributions of magnetohydrodynamic (MHD) vortexes to chiral electrodeposition in a vertical magnetic field were theoretically examined based on the three-generation model of the 2D nucleus, 3D nucleus, and screw dislocation; for the vortexes to rotate in the second and third-generation, the kinematic viscosity must be at least 10−18 and 10−30 times lower than the ordinary value in the first generation, i.e., almost equal to zero. This implies that the ionic vacancy created on the electrode surface works as an atomic-scale lubricant. At the same time, the vortexes played three roles: promotion and suppression of nucleation, and transport of the chirality from the upper generation to the lower generation through precessional motion. Then, the rule of the chirality transfer was established, and finally, the relationship between the chiral activity and magnetic field was clarified in the presence and absence of chloride ions.

DOI： 10.3390/magnetochemistry10040025

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsaem.4c00141

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

A paucity of redox centers, poor charge transport properties, and low structural stability of organic materials obstruct their use in practical applications. Herein, these issues have been addressed through the use of a redox‐active salen‐based framework polymer (RSFP) containing multiple redox‐active centers in π‐conjugated configuration for applications in lithium‐ion batteries (LIBs). Based on its unique architecture, RSFP exhibits a superior reversible capacity of 671.8 mAh g⁻¹ at 0.05 A g⁻¹ after 168 charge‐discharge cycles. Importantly, the lithiation/de‐lithiation performance is enhanced during operation, leading to an unprecedented reversible capacity of 946.2 mAh g⁻¹ after 3500 cycles at 2 A g⁻¹. The structural evolution of RSFP is studied ex situ using X‐ray photoelectron spectroscopy, revealing multiple active C═N, C─O, and C═O sites and aromatic sites such as benzene rings. Remarkably, the emergence of C═O originated from C─O is triggered by an electrochemical process, which is beneficial for improving reversible lithiation/delithiation behavior. Furthermore, the respective strong and weak binding interactions between redox centers and lithium ions, corresponding to theoretical capacities of 670.1 and 938.2 mAh g⁻¹, have been identified by density functional theory calculations manifesting 14‐electron redox reactions. This work sheds new light on routes for the development of redox‐active organic materials for energy storage applications.

DOI： 10.1002/smll.202309321

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Distinct from inorganic 2D nanomaterials (e.g., graphene, MoS₂, etc,), self‐assembled organic 2D materials are significant due to the unique advantages of fine structure tunability and functionality. Electronically and photofunctionally‐active compounds (e.g., pentacene, p‐sexiphenyl) are highly attractive for applications but are limited by difficult handling and the existence of only a few native structures of the compounds. Here, it is shown that a p‐sexiphenyl derivative incorporated into 2D multilamellar sheets with chromophores oriented in the layers exhibits a significant polarization of photoluminescence. Highly emissive, amphiphilic sexiphenyl with hydrophilic/hydrophobic groups self‐assembles at air–water interface with chromophore orientation in the resulting films being controlled by monolayer compression. Large‐area multilamellar structures with p‐sexiphenyl chromophores highly oriented against the 2D plane are prepared by consecutive film transfers. The 2D sheets exhibit significant polarization of photoluminescence with polarization ratio 0.8 between orthogonal in‐plane axes. Notably, multilamellar structures cannot be established for the same p‐sexiphenyl using thermotropic processing thus emphasizing the importance of the 2D sheet multilayer synthesis process. Amphiphile design can be applied for the tailored synthesis of large‐area multilayered 2D sheets and used to construct highly efficient light‐emitting devices.

DOI： 10.1002/adom.202400177

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Informa UK Limited  

DOI： 10.1080/14686996.2024.2322458

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c09159

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Methods to encode digital data items as strands of synthetic DNA followed by selective data retrieval have been demonstrated. However, these initially bio‐oriented processes remain slow and not optimized. DNA field‐effect transistor (DNA‐FET) is studied here as a possible random‐access memory (RAM) device for simple, selective and rapid ssDNA fragment retrieval used as data pool identifier. The DNA‐FET is based on a co‐planar Au‐gated fully organic transistor appended with short single‐stranded DNA (ssDNA) probes bearing a blocking molecule to prevent partial hybridization and achieve near perfect selectivity for short length ssDNA (up to 45 nt). Examination of transconductance of the novel active layer incorporating a DNA nanopore architecture reveals enhanced binding site accessibility. This, in turn, facilitates discriminatory hybridization, particularly in the physical retrieval of short‐length ssDNA from a competitive, concentrated ssDNA background pool consisting of nine different sequences, with at least one nucleotide difference. The DNA‐FET exhibits rapid operation (9 min) in the millivolt range, low detection limit (sub‐femtomolar), high selectivity and reusability. Considering the straightforward concept, near error‐free identification capacity and hypothetically outstanding scalability, the DNA‐FET described here has potential as a foundation for further exploration of advanced RAM technology in the DNA data storage process.

DOI： 10.1002/adsr.202300176

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.148456

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c09819

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Informa UK Limited  

DOI： 10.1080/14686996.2023.2292485

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

Abstract

Through a copper double bipolar magnetohydrodynamic (MHD) electrode (MHDE) producing twice the amounts of ionic vacancies than a conventional single MHDE, the molar excess heat of the pair annihilation of ionic vacancies, 702 kJ mol⁻¹ at 10 T on average was obtained in a copper redox reaction. It was about twice as large as that of a single MHDE, 387 kJ mol⁻¹ at the same magnetic field. This result strongly suggests that a multi-channel bipolar MHDE will produce much greater excess heat. To conserve the linear momentum and electric charge during electron transfer in an electrode reaction, ionic vacancies are created, storing the solvation energy in the polarized core of the order of 0.1 nm, and the pair annihilation of the vacancies with opposite charges liberates the energy as excess heat. The promoted excess heat by the double bipolar MHDE with a diffuser at 10 T was 710 ± 144 kJ mol⁻¹, whereas as mentioned above, 702 ± 426 kJ mol⁻¹ was obtained by the same electrode without such a diffuser. From the theoretical excess heat of 1140 kJ mol⁻¹, the collision efficiencies in pair annihilation were 0.623 ± 0.126 and 0.616 ± 0.374, respectively. From these results, the reproducibility of the thermal measurement was experimentally validated. At the same time, it was concluded that at magnetic fields beyond 10 T, the concentration of ionic vacancy and the collision efficiency take constant uppermost values.

DOI： 10.1038/s41598-024-51834-w

Other Link： https://www.nature.com/articles/s41598-024-51834-w

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acscentsci.3c01637

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c09386

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Minimally invasive procedures assisted by soft robots for surgery, diagnostics, and drug delivery have unprecedented benefits over traditional solutions from both patient and surgeon perspectives. However, the translation of such technology into commercialization remains challenging. The lack of perception abilities is one of the obstructive factors paramount for a safe, accurate and efficient robot‐assisted intervention. Integrating different types of miniature sensors onto robotic end‐effectors is a promising trend to compensate for the perceptual deficiencies in soft robots. For example, haptic feedback with force sensors helps surgeons to control the interaction force at the tool‐tissue interface, impedance sensing of tissue electrical properties can be used for tumor detection. The last decade has witnessed significant progress in the development of multimodal sensors built on the advancement in engineering, material science and scalable micromachining technologies. This review article provides a snapshot on common types of integrated sensors for soft medical robots. It covers various sensing mechanisms, examples for practical and clinical applications, standard manufacturing processes, as well as insights on emerging engineering routes for the fabrication of novel and high‐performing sensing devices.

DOI： 10.1002/smll.202308805

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.147990

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jma.2023.11.014

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A sub-nano interfacial catalytic structure is orchestrated by tailor-designing a hollow bowl-like porous carbon-confined Ru–MgO hetero-structured nanopair as a high-performance catalyst for ammonia borane hydrolysis.

DOI： 10.1039/d3mh01909h

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Graphene coating and N-doped graphene coating are not only good physical protective layers but also have efficient ORR catalytic activity on platinum surfaces, which is important for promoting high-performance fuel cell technology.

DOI： 10.1039/d4cp00269e

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

SiO₂ assisted abundant Cu⁰–Cu⁺–NH₂ composite interfaces enhance the adsorption and activation of CO₂ and H₂O, strengthen the adsorption of CO intermediates, and promote C–C coupling to produce C₂₊ products.

DOI： 10.1039/d3ta05652j

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Ultrafine MoC nanocrystals are confined within the MOF-derived NC matrix to generating NC/MoC. The NC/MoC based electrode achieves high CDI performance.

DOI： 10.1039/d4sc00971a

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

We demonstrate Mn-defected γ-MnO₂ as photocatalyst for synthesis of vanillin in aqueous environment under room temperature. The ˙OH species on Mn-defected γ-MnO₂ act as reactive oxygen species for oxidation of vanillyl alcohol into vanillin.

DOI： 10.1039/d3sc05654f

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Smectite-type clays with interlayer inorganic cations can be swollen and delaminated in water–polar organic mixed solvents.

DOI： 10.1039/d4dt00192c

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

This work reports the selective synthesis of monodisperse nickel–cobalt phosphate particles with different structures for battery-like supercapacitors.

DOI： 10.1039/d3ta06584g

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The Mn substitution and structure optimization via ppy connection confer enhanced ion/electron migration to NiHCF. This results in rapid redox kinetics, improves electrode integrity, and ultimately ensures high desalination performance.

DOI： 10.1039/d4sc00686k

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Nanoporous Ba_0.85Ca_0.15(Ti_0.9Zr_0.1)O₃ (BCZT) films, as lead-free piezoelectrics, exhibited a d₃₃ ∼10 times higher than nonporous BCZT, making them promising for high-density dielectric capacitors and energy harvesters.

DOI： 10.1039/d3sc06712b

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The potential of materials informatics in designing lithium extraction materials for capacitive deionization have been discussed.

DOI： 10.1039/d3ta07069g

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

B, N-doped porous carbon confined MoC quantum dots were engineered as a facile carrier and electronic stimulator to confine Ru clusters for high-performance hydrogen evolution reaction.

DOI： 10.1039/d4ta02442g

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A structure-property relationship is disclosed between electrochemical surface area and active site utilization in ORR. The optimized NPC–Zn exhibits excellent zinc–air battery performance, serving as a power to drive capacitive deionization devices.

DOI： 10.1039/d4ta03422h

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Robust composites are designed to degrade chemical warfare agents by integrating UiO-66 catalysts and branched poly(ethyleneimine) into a ladder-like poly(silsesquioxane) matrix, making them ideal for protective coatings.

DOI： 10.1039/d4ta04668d

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The S/HBEA cell achieves an initial discharge capacity of 866.13 mA h g⁻¹ at 0.5C with a capacity decay of merely 0.13% per cycle during 300 cycles.

DOI： 10.1039/d4ta01037j

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A structural and electronic dual-modulation is achieved on 2D arrays of hollow carbon nanoboxes, exhibiting exceptional performance in rechargeable zinc–air batteries.

DOI： 10.1039/d4sc01257g

Scopus

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A carbon-based bifunctional heterogeneous enzyme was prepared. The carrier structure, immobilized enzyme structure, enzymatic properties, stability performance and DEHP removal were also investigated.

DOI： 10.1039/d4sc03752a

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Integrating mesoporous gold NP-based SERS nanotags with microfluidics offers a rapid, reliable, and sensitive approach for the multiplexed detection of SARS-CoV-2 and similar infectious diseases.

DOI： 10.1039/d4tc01638f

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

We propose a sequential liquid dispensing method in a centrifugal microfluidic device for the multiplexed genetic detection.

DOI： 10.1039/d4ra04055d

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c07375

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c07635

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/jacs.3c05544

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

Abstract

Hollow multi-shell mesoporous metal–organic framework (MOF) particles with accessible compartmentalization environments, plentiful heterogeneous interfaces, and abundant framework diversity are expected to hold great potential for catalysis, energy conversion, and biotechnology. However, their synthetic methodology has not yet been established. In this work, a facile dual-template-directed successive assembly approach has been developed for the preparation of monodisperse hollow multi-shell mesoporous MOF (UiO-66-NH₂) particles through one-step selective etching of successively grown multi-layer MOFs with alternating two types of mesostructured layers. This strategy enables the preparation of hollow multi-shell mesoporous UiO-66-NH₂ nanostructures with controllable shell numbers, accessible mesochannels, large pore volume, tunable shell thickness and chamber sizes. The methodology relies on creating multiple alternating layers of two different mesostructured MOFs via dual-template-directed successive assembly and their difference in framework stability upon chemical etching. Benefiting from the highly accessible Lewis acidic sites and the accumulation of reactants within the multi-compartment architecture, the resultant hollow multi-shell mesoporous UiO-66-NH₂ particles exhibit enhanced catalytic activity for CO₂ cycloaddition reaction. The dual-template-directed successive assembly strategy paves the way toward the rational construction of elaborate hierarchical MOF nanoarchitectures with specific physical and chemical features for different applications.

DOI： 10.1038/s41467-023-43259-2

Other Link： https://www.nature.com/articles/s41467-023-43259-2

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.est.2023.108780

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.146841

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.nanoen.2023.108914

Publishing type：Research paper (scientific journal)  

Correction to: Nature Communications, published online 13 July 2023 The original version of the Supplementary Information associated with this Article included incorrect Supplementary Datasets. Dataset 1 reported an editorial policy checklist; Dataset 3 reported a general description of Supplementary Figures and Tables contained in the Supplementary Information PDF file; Dataset 4 contained editorial instructions to the authors for the preparation of the final version of the article. Datasets 1, 3, and 4 have been removed in the corrected version of the Article. In addition, the Reporting Summary and the Source Data file were originally published with the wrong titles of Dataset 2 and Dataset 5. The HTML version of the article has been corrected.

DOI： 10.1038/s41467-023-40653-8

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PubMed

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.3c07270

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Electrocatalyst engineering from the atomic to macroscopic level of electrocatalysts is one of the most powerful routes to boost the performance of electrochemical devices. However, multi‐scale structure engineering mainly focuses on the range of atomic‐to‐particle scale such as hierarchical porosity engineering, while catalyst engineering at the macroscopic level, such as the arrangement configuration of nanoparticles, is often overlooked. Here, a 2D carbon polyhedron array with a multi‐scale engineered structure via facile chemical etching, ice‐templating induced self‐assembly, and high‐temperature pyrolysis processes is reported. Controlled phytic acid etching of the carbon precursor introduces homogeneous atomic phosphorous and nitrogen doping, as well as a well‐defined mesoporous structure. Subsequent ice‐templated self‐assembly triggers the formation of a 2D particle array superstructure. The atomic‐level doping gives rise to high intrinsic activity, while the well‐engineered porous structure and particle arrangement addresses the mass transport limitations at the microscopic particle level and macroscopic electrode level. As a result, the as‐prepared electrocatalyst delivers outstanding performance toward oxygen reduction reaction in both acidic and alkaline media, which is better than recently reported state‐of‐the‐art metal‐free electrocatalysts. Molecular dynamics simulation together with extensive characterizations indicate that the performance enhancement originates from multi‐scale structural synergy.

DOI： 10.1002/smll.202305459

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.apcatb.2023.122933

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.apcatb.2023.122945

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jallcom.2023.171438

Language：English   Publishing type：Research paper (scientific journal)   Publisher：IOP Publishing  

Abstract

Successful superconducting joints of reacted magnesium diboride (MgB₂) monofilament wires are reported in this paper. The absence of a reliable method to develop superconducting joints between reacted MgB₂ wires presents a major obstacle to the wider adoption of MgB₂ as a material for magnet winding. A hot uniaxial pressing (HUP) system was exploited for sintering purposes since it can facilitate the formation of condensed in situ bulk on the wire filament. The wires were manufactured with an extra thick barrier material to protect the filament from damage during HUP sintering. The sintering temperature and pressure of the HUP system were varied to comprehend the best-performing joint. The performance of joints could be improved by depreciating the pores within the intermediate bulk of the joint. To prove this point, joints were cut to study their morphology. However, due to sintering in pressurised conditions, the reaction of the in situ intermediate bulk was not completed. The x-ray diffraction result detected a significant unreacted magnesium phase in the intermediate bulk. This work obtained joints of reacted MgB₂ wires which can be considered for industrial MgB₂ magnetic resonance imaging magnets fabrication.

DOI： 10.1088/1361-6668/ad02c7

Other Link： https://iopscience.iop.org/article/10.1088/1361-6668/ad02c7/pdf

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Abstract

One of the difficulties limiting covalent organic frameworks (COFs) from becoming excellent adsorbents is their stacking/aggregation architectures owing to poor morphology/structure control during the synthesis process. Herein, an inorganic‐organic nanoarchitectonics strategy to synthesize the MXene/COF heterostructure (Ti₃C₂T_x/TAPT‐TFP) is developed by the assembly of β‐ketoenamine‐linked COF on the Ti₃C₂T_x MXene nanosheets. The as‐prepared Ti₃C₂T_x/TAPT‐TFP retains the 2D architecture and high adsorption capacity of MXenes as well as large specific surface area and hierarchical porous structure of COFs. As a proof of concept, the potential of Ti₃C₂T_x/TAPT‐TFP for solid‐phase microextraction (SPME) of trace organochlorine pesticides (OCPs) is investigated. The Ti₃C₂T_x/TAPT‐TFP based SPME method achieves low limits of detection (0.036–0.126 ng g⁻¹), wide linearity ranges (0.12–20.0 ng g⁻¹), and acceptable repeatabilities for preconcentrating trace OCPs from fruit and vegetable samples. This study offers insights into the potential of constructing COF or MXene‐based heterostructures for the microextraction of environmental pollutants.

DOI： 10.1002/smll.202305730

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DOI： 10.1021/jacs.3c08598

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DOI： 10.1021/jacs.3c05846

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Abstract

Solar‐powered vapor evaporation (SVG), based on the liquid‐gas phase conversion concept using solar energy, has been given close attention as a promising technology to address the global water shortage. At molecular level, water molecules escaping from liquid water should overcome the attraction of the molecules on the liquid surface layer to evaporate. For this reason, it is better to reduce the energy required for evaporation by breaking a smaller number of hydrogen bonds or forming weak hydrogen bonds to ensure efficient and convenient vapor production. Many novel evaporator materials and effective water activation strategies have been proposed to stimulate rapid steam production and surpass the theoretical thermal limit. However, an in‐depth understanding of the phase/enthalpy change process of water evaporation is unclear. In this review, a summary of theoretical analyses of vaporization enthalpy, general calculations, and characterization methods is provided. Various water activation mechanisms are also outlined to reduce evaporation enthalpy in evaporators. Moreover, unsolved issues associated with water activation are critically discussed to provide a direction for future research. Meanwhile, significant pioneering developments made in SVG are highlighted, hoping to provide a relatively entire chain for more scholars who are just stepping into this field.

DOI： 10.1002/adma.202212100

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Informa UK Limited  

DOI： 10.1080/29934168.2023.2268943

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DOI： 10.1016/j.cej.2023.145421

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1038/s41596-023-00872-1

Other Link： https://www.nature.com/articles/s41596-023-00872-1

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Abstract

Nanoarchitectonics, a concept encompassing nanoscale microstructures and atomic arrangements in materials, enables the precise modification of materials for desired applications by controlling their physical and chemical properties, as well as surface charge or energy. Particularly in metal materials, where surface reactions play a critical role, nanoarchitecture becomes the most influential factor affecting activity, selectivity, and stability. Focusing on platinum‐group metals (PGMs) due to their inherently high efficiency in energy and environmental applications, this article provides a comprehensive review of synthetic methods for the morphological control of metal nanomaterials. The morphological control is classified into atomic arrangements in 0D, 1D, and 2D nanocrystals, as well as nanoporous structures, and the mechanisms of major reactions are covered in detail. Each chapter is supplemented with a table featuring several examples, facilitating the reader's understanding of the structural controls of PGMs. Finally, the article outlines future challenges in achieving novel metal nanoarchitecture. The hope is that this review provides valuable insights into the synthesis of PGM‐based nanomaterials and serves as a guide for designing and synthesizing innovative metal nanostructures for diverse applications.

DOI： 10.1002/adfm.202301831

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.144703

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DOI： 10.1016/j.apcatb.2023.122771

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.144395

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DOI： 10.1016/j.cej.2023.144262

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.144600

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.143893

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DOI： 10.1016/j.cej.2023.144544

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Metal–organic frameworks (MOFs) can be customized through modular assembly to achieve a wide range of potential applications, based on their desired functionality. However, most of the initially reported MOFs are limited to microporous systems and are not sufficiently stable, which restricts their popularization. Heterogeneity is introduced into a simple MOF framework to create MOF‐based heterostructures with fascinating properties and interesting functions. Heterogeneity can be introduced into the MOFs via postsynthetic/ligand exchange. Although the ligand exchange has shown potential, it is difficult to precisely control the degree of exchange or position. Among the various synthesis strategies, hierarchical assembly is particularly attractive for constructing MOF‐based heterostructures, as it can achieve precise regulation of MOF‐based heterostructured nanostructures. The hierarchical assembly significantly expands the compositional diversity of MOF‐based heterostructures, which has high elasticity for lattice matching during the epitaxial growth of MOFs. This review focuses on the synthetic evolution mechanism of hierarchical assemblies of MOF‐based nanoarchitectures. Subsequently, the precise control of pore structure, pore size, and morphology of MOF‐based nanoarchitectures by hierarchical assembly is emphasized. Finally, possible solutions to address the challenges associated with heterogeneous interfaces are presented, and potential opportunities for innovative applications are proposed.

DOI： 10.1002/smll.202303884

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Abstract

Reactions occurring at surfaces and interfaces necessitate the creation of well‐designed surface and interfacial structures. To achieve a combination of bulk material (i.e., framework) and void spaces, a meticulous process of “nano‐architecting” of the available space is necessary. Conventional porous materials such as mesoporous silica, zeolites, and metal–organic frameworks lack advanced cooperative functionalities owing to their largely monotonous pore geometries and limited conductivities. To overcome these limitations and develop functional structures with surface‐specific functions, the novel materials space‐tectonics methodology has been proposed for future materials synthesis. This review summarizes recent examples of materials synthesis based on designing building blocks (i.e., tectons) and their hybridization, along with practical guidelines for implementing materials syntheses and state‐of‐the‐art examples of practical applications. Lastly, the potential integration of materials space‐tectonics with emerging technologies, such as materials informatics, is discussed.

DOI： 10.1002/anie.202307615

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Abstract

Although hollow carbon structures have been extensively studied in recent years, their interior surfaces are not fully utilized due to the lack of fluent porous channels in the closed shell walls. This study presents a tailored design of open‐mouthed particles hollow cobalt/nitrogen‐doped carbon with mesoporous shells (OMH‐Co/NC), which exhibits sufficient accessibility and electroactivity on both the inner and outer surfaces. By leveraging the self‐conglobation effect of metal sulfate in methanol, a raspberry‐structured Zn/Co‐ZIF (R‐Zn/Co‐ZIF) precursor is obtained, which is further carbonized to fabricate the OMH‐Co/NC. In‐depth electrochemical investigations demonstrate that the introduction of open pores can enhance mass transfer and improve the utilization of the inner active sites. Benefiting from its unique structure, the resulting OMH‐Co/NC exhibits exceptional electrocatalytic oxygen reduction performance, achieving a half‐wave potential of 0.865 V and demonstrating excellent durability.

DOI： 10.1002/smll.202304450

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/jacs.3c04612

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DOI： 10.1021/jacs.3c03029

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Oxford University Press (OUP)  

Abstract

Owing to their cost-effectiveness and renewability, wood-based solar steam generators (WSSG) have gained prominence in the field of desalination and water purification. However, conventional bi-layered WSSG is limited by the high energy consumption of fabrication and low strength of the bonding interface, which makes them unsuitable for long-term applications. Here, a unique bi-layered structural composite with polyaniline (PANI) nanorods uniformly incorporated into a 3D mesoporous matrix of natural wood was fabricated via a one-step in-situ polymerization strategy. The PANI decorated wood (PANI-wood) shows ultrahigh sunlight absorptance (∼98.9%) over a broad wavelength range (200–2500 nm) due to the conjugation of coralloid PANI nanorods and wood. Moreover, numerous aligned wood microchannels enable constant and rapid water transport at the air-water interface under the pressure of capillary forces. The highly stable PANI-wood composite shows high potential as an ideal solar steam generator with a high evaporation rate of 1.62 kg m2 h−1, which is significantly higher than those of other previously reported wood-based bi-layered composites. Moreover, PANI-wood exhibits long-term floating and is chemically stable, making it a potential candidate for low-energy photothermal interfacial sewage purification.

DOI： 10.1246/bcsj.20230145

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Abstract

Multimetallic alloys (MMAs) with various compositions enrich the materials library with increasing diversity and have received much attention in catalysis applications. However, precisely shaping MMAs in mesoporous nanostructures and mapping the distributions of multiple elements remain big challenge due to the different reduction kinetics of various metal precursors and the complexity of crystal growth. Here we design a one-pot wet-chemical reduction approach to synthesize core–shell motif PtPdRhRuCu mesoporous nanospheres (PtPdRhRuCu MMNs) using a diblock copolymer as the soft template. The PtPdRhRuCu MMNs feature adjustable compositions and exposed porous structures rich in highly entropic alloy sites. The formation processes of the mesoporous structures and the reduction and growth kinetics of different metal precursors of PtPdRhRuCu MMNs are revealed. The PtPdRhRuCu MMNs exhibit robust electrocatalytic hydrogen evolution reaction (HER) activities and low overpotentials of 10, 13, and 28 mV at a current density of 10 mA cm⁻² in alkaline (1.0 M KOH), acidic (0.5 M H₂SO₄), and neutral (1.0 M phosphate buffer solution (PBS)) electrolytes, respectively. The accelerated kinetics of the HER in PtPdRhRuCu MMNs are derived from multiple compositions with synergistic interactions among various metal sites and mesoporous structures with excellent mass/electron transportation characteristics.

DOI： 10.1038/s41467-023-39157-2

Other Link： https://www.nature.com/articles/s41467-023-39157-2

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Abstract

Ammonia borane (AB) is a promising material for chemical H₂ storage owing to its high H₂ density (up to 19.6 wt %). However, the development of an efficient catalyst for driving H₂ evolution through AB hydrolysis remains challenging. Therefore, a visible‐light‐driven strategy for generating H₂ through AB hydrolysis was implemented in this study using Ni−Pt nanoparticles supported on phosphorus‐doped TiO₂ (Ni‐Pt/P‐TiO₂) as photocatalysts. Through surface engineering, P‐TiO₂ was prepared by phytic‐acid‐assisted phosphorization and then employed as an ideal support for immobilizing Ni−Pt nanoparticles via a facile co‐reduction strategy. Under visible‐light irradiation at 283 K, Ni₄₀Pt₆₀/P‐TiO₂ exhibited improved recyclability and a high turnover frequency of 967.8 mol mol_Pt⁻¹ min⁻¹. Characterization experiments and density functional theory calculations indicated that the enhanced performance of Ni₄₀Pt₆₀/P‐TiO₂ originated from a combination of the Ni−Pt alloying effect, the Mott–Schottky junction at the metal‐semiconductor interface, and strong metal‐support interactions. These findings not only underscore the benefits of utilizing multipronged effects to construct highly active AB‐hydrolyzing catalysts, but also pave a path toward designing high‐performance catalysts by surface engineering to modulate the electronic metal‐support interactions for other visible‐light‐induced reactions.

DOI： 10.1002/anie.202305371

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.143733

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DOI： 10.1021/acsnano.3c01380

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The design and development of efficient catalysts for electrochemical nitrogen reduction reaction (ENRR) under ambient conditions are critical for the alternative ammonia (NH₃) synthesis from N₂ and H₂O, wherein iron‐based electrocatalysts exhibit outstanding NH₃ formation rate and Faradaic efficiency (FE). Here, the synthesis of porous and positively charged iron oxyhydroxide nanosheets by using layered ferrous hydroxide as a starting precursor, which undergoes topochemical oxidation, partial dehydrogenated reaction, and final delamination, is reported. As the electrocatalyst of ENRR, the obtained nanosheets with a monolayer thickness and 10‐nm mesopores display exceptional NH₃ yield rate (28.5 µg h⁻¹ mg_cat.⁻¹) and FE (13.2%) at a potential of −0.4 V versus RHE in a phosphate buffered saline (PBS) electrolyte. The values are much higher than those of the undelaminated bulk iron oxyhydroxide. The larger specific surface area and positive charge of the nanosheets are beneficial for providing more exposed reactive sites as well as retarding hydrogen evolution reaction. This study highlights the rational control on the electronic structure and morphology of porous iron oxyhydroxide nanosheets, expanding the scope of developing non‐precious iron‐based highly efficient ENRR electrocatalysts.

DOI： 10.1002/smll.202303221

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DOI： 10.1021/acs.nanolett.3c00183

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.143315

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.seppur.2023.123628

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DOI： 10.1016/j.cej.2023.142838

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Abstract

Covalent organic frameworks (COFs) with high specific surface area, tailored structure, easy functionalization, and excellent chemical stability have been extensively exploited as fantastic materials in various fields. However, in most cases, COFs prepared in powder form suffer from the disadvantages of tedious operation, strong tendency to agglomerate, and poor recyclability, greatly limiting their practical application in environmental remediation. To tackle these issues, the fabrication of magnetic COFs (MCOFs) has attracted tremendous attention. In this review, several reliable strategies for the fabrication of MCOFs are summarized. In addition, the recent application of MCOFs as outstanding adsorbents for the removal of contaminants including toxic metal ions, dyes, pharmaceuticals and personal care products, and other organic pollutants is discussed. Moreover, in‐depth discussions regarding the structural parameters affecting the practical potential of MCOFs are highlighted in detail. Finally, the current challenges and future prospects of MCOFs in this field are provided with the expectation to boost their practical application.

DOI： 10.1002/smll.202301044

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Wide bandgap (WBG) semiconductors have attracted significant research interest for the development of a broad range of flexible electronic applications, including wearable sensors, soft logical circuits, and long‐term implanted neuromodulators. Conventionally, these materials are grown on standard silicon substrates, and then transferred onto soft polymers using mechanical stamping processes. This technique can retain the excellent electrical properties of wide bandgap materials after transfer and enables flexibility; however, most devices are constrained by 2D configurations that exhibit limited mechanical stretchability and morphologies compared with 3D biological systems. Herein, a stamping‐free micromachining process is presented to realize, for the first time, 3D flexible and stretchable wide bandgap electronics. The approach applies photolithography on both sides of free‐standing nanomembranes, which enables the formation of flexible architectures directly on standard silicon wafers to tailor the optical transparency and mechanical properties of the material. Subsequent detachment of the flexible devices from the support substrate and controlled mechanical buckling transforms the 2D precursors of wide band gap semiconductors into complex 3D mesoscale structures. The ability to fabricate wide band gap materials with 3D architectures that offer device‐level stretchability combined with their multi‐modal sensing capability will greatly facilitate the establishment of advanced 3D bio‐electronics interfaces.

DOI： 10.1002/adfm.202211781

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DOI： 10.1021/acsnano.3c01758

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

The hybrid composed of anisotropic niobate layers modified with MoC nanoparticles is synthesized by multistep reactions. The stepwise interlayer reactions for layered hexaniobate induce selective surface modification at the alternate interlayers, and the following ultrasonication leads to the formation of double‐layered nanosheets. The further liquid phase MoC deposition with the double‐layered nanosheets leads to the decoration of MoC nanoparticles on the surfaces of the double‐layered nanosheets. The new hybrid can be regarded as a stacking of the two layers with anisotropically modified nanoparticles. The relatively high temperature in the MoC synthesis causes partial leaching of the grafted phosphonate groups. The exposed surface of the niobate nanosheets due to the partial leaching may interact with MoC to succeed in the hybridization. The hybrid after heating exhibits photocatalytic activity, indicating that this hybridization method can be useful for hybrid synthesis of semiconductor nanosheets and co‐catalyst nanoparticles toward photocatalytic application.

DOI： 10.1002/chem.202300218

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.jcis.2023.01.075

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Abstract

CsCl‐type intermetallic compounds TiM (M=Co, Fe) were obtained by deoxidizing trigonal ilmenite‐type MTiO₃ with a reducing agent CaH₂ in molten LiCl at 600 °C. X‐ray diffraction, nitrogen adsorption, scanning electron microscopy, and transmission electron microscopy with energy‐dispersive X‐ray, and X‐ray photoelectron spectroscopy analyses revealed the formation of nanoscale layered structures, which enhanced specific surface areas (approximately 20 m²/g) in the intermetallic compounds. In the initial deoxidation stage, Li₂TiO₃‐like compounds were observed as an intermediate, suggesting the substitution of M in MTiO₃ by Li from the molten LiCl. Compound MTiO₃ has a layered structure perpendicular to the c axis of the trigonal structure, suggesting that the layered structures may originate from the crystal structure of the precursors. Formation of the Li₂TiO₃‐like intermediate may help maintain the original layered structure during deoxidation and the subsequent alloying at temperatures as low as 600 °C.

DOI： 10.1002/chem.202300194

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Abstract

In this study, a specific organosilane molecule (octadecyldimethyl(3-trimethoxysilylpropyl)ammonium) is used to form soft-templates that store organic corrosion inhibitors (tolytriazole), and chemically anchor to silica surface during a sol-gel process. As the anchored soft-templates in the resulting mesostructured silica are not removed, it successfully achieves an environmental-friendly synthetic method and a prolonged storage of tolyriazole. Coating of a copper substrate with the mesostructured silica embedding tolytriazole, therefore, endows a prolonged anticorrosion effect.

DOI： 10.1246/bcsj.20230004

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DOI： 10.1021/jacs.3c01755

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Materials derived from metal–organic frameworks (MOFs) have demonstrated exceptional structural variety and complexity and can be synthesized using low‐cost scalable methods. Although the inherent instability and low electrical conductivity of MOFs are largely responsible for their low uptake for catalysis and energy storage, a superior alternative is MOF‐derived metal‐based derivatives (MDs) as these can retain the complex nanostructures of MOFs while exhibiting stability and electrical conductivities of several orders of magnitude higher. The present work comprehensively reviews MDs in terms of synthesis and their nanostructural design, including oxides, sulfides, phosphides, nitrides, carbides, transition metals, and other minor species. The focal point of the approach is the identification and rationalization of the design parameters that lead to the generation of optimal compositions, structures, nanostructures, and resultant performance parameters. The aim of this approach is to provide an inclusive platform for the strategies to design and process these materials for specific applications. This work is complemented by detailed figures that both summarize the design and processing approaches that have been reported and indicate potential trajectories for development. The work is also supported by comprehensive and up‐to‐date tabular coverage of the reported studies.

DOI： 10.1002/adma.202210166

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsomega.3c00512

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acssensors.2c02720

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsmaterialslett.2c01169

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.142221

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.chemmater.2c03282

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Abstract

Organic–inorganic hybrid perovskite solar cells (PSCs) are among the most promising candidates for the next generation of photovoltaic devices because of the significant increase in their power conversion efficiency (PCE) from less than 10% to 25.7% in past decade. The metal‐organic framework (MOF) materials owing to their unique properties, such as large specific surface area, abundant binding sites, adjustable nanostructures, and synergistic effects, are used as additives or functional layers to enhance the device performance and long‐term stability of PSCs. This review focuses on the recent advancements in the applications of MOFs as/in different functional layers of PSCs. The photovoltaic performance, impact, and advantages of MOF materials integrated into the perovskite absorber, electron transport layer, hole transport layer, and interfacial layer are reviewed. In addition, the applicability of MOFs to mitigate leakage of Pb²⁺ from halide perovskites and corresponding devices is discussed. This review concludes with the perspectives on further research directions for employing MOFs in PSCs.

DOI： 10.1002/smll.202208119

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/smll.202208119

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DOI： 10.1021/jacs.2c10637

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2023.141504

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

Abstract

Layered potassium manganese oxides are promising candidates for use in aqueous supercapacitors owing to their wide potential windows, layered feature, and Faradaic redox reactions that occur on surfaces and in bulk regions. However, the practical application is hindered by rapid performance degradation due to their inherently low electrical conductivities and inferior structural stabilities. Here, we develop ultralong nanobelts comprising hydrated Na-intercalated oxygen-deficient potassium manganese oxide (H-Na-D-KMO), in which the Na⁺ ions are preintercalated and synchronously induce the generation of oxygen vacancies, as high-energy-density and durable electrodes for Mg-ion supercapacitors. The experimental results indicated that preintercalation of Na⁺ ions and formation of oxygen vacancies improved the electrical properties and ion diffusion, which accounted for the fast reaction kinetics and good cycling performance of H-Na-D-KMO. The optimized H-Na-D-KMO delivered a significantly enhanced specific capacitance and cycling performance compared to those of pure H-KMO. Asymmetric supercapacitors with H-Na-D-KMO as the cathode and as-prepared MoO₂@carbon as the anode exhibited an ultrahigh energy density of 108.4 Wh kg^–1 at 11,000 Wh kg⁻¹, which is superior to most supercapacitors reported in the literature. Moreover, the assembled device exhibited good cycling stability for over 5000 cycles with a fading rate of 0.002% per cycle and good mechanical flexibility, which opens an avenue for further advancements in high-energy supercapacitors.

DOI： 10.1038/s41427-022-00450-z

Other Link： https://www.nature.com/articles/s41427-022-00450-z

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acs.chemmater.2c03639

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acscatal.2c04685

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.2c07694

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.140464

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.139544

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.matre.2023.100176

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.139875

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Oxford University Press (OUP)  

Abstract

Electrochemical faradic deionization (EDI), one of the most promising research branches of capacitive deionization (CDI), has demonstrated considerable potential for water desalination and ion removal (particularly at medium to low salinity). However, the associated relatively slow anion-capturing kinetics have limited the practical applications of EDI. Based on several studies, researchers have attributed this slow anion-capturing rate to the sluggish conversion-reaction-induced anion-capturing process (as most anion-capturing electrodes belong to the conversion type). Herein, we report a strategy for accelerating the anion-capturing process to enhance the desalination rate of EDI by utilizing an intercalation-type FeOOH electrode. The chloride-driven EDI system equipped with hollandite-type FeOOH nanospindles is found to present a high desalination rate (up to 4.44 mg g−1 min−1) and desalination capacity (51.77 mg g−1). The current study can inspire the future design of ultrafast EDI systems and bring the EDI technique closer to its practical application.

DOI： 10.1246/bcsj.20220274

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

To increase chemical reaction rates, general solutions include increasing the concentration/temperature and introducing catalysts. In this study, the rate constant of an electrophilic metal coordination reaction is accelerated 23‐fold on the surface of layered aluminosilicate (LAS), where the reaction substrate (ligand molecule) induces dielectric polarization owing to the polar and anionic surface. According to the Arrhenius plot, the frequency factor (A) is increased by almost three orders of magnitude on the surface. This leads to the conclusion that the collision efficiency between the ligands and metal ions is enhanced on the surface due to the dielectric polarization. This is surprising because one side of the ligand is obscured by the surface, so the collision efficiency is expected to be decreased. This unique method to accelerate the chemical reaction is expected to expand the range of utilization of LASs, which are chemically inert, abundant, and environmentally friendly. The concept is also applicable to other metal oxides which have polar surfaces, which will be useful for various chemical reactions in the future.

DOI： 10.1002/smll.202205857

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/smll.202205857

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

It is of great significance to design a bifunctional electrocatalyst for promoting hydrogen (HER) and oxygen (OER) evolution reactions simultaneously. Herein, inspired by the appropriate H atom binding energy on cobalt phosphides and excellent oxygen evolution kinetics on cobalt oxides, the regulative synthesis of a Co₂P–Co_xO_y (Co_xO_y = CoO or Co₃O₄) heterogeneous nanoparticle‐anchored porous carbon network electrocatalyst via one‐pot heat treatment is reported. The as‐synthesized Co₂P–Co₃O₄/C exhibits superior electrochemical activity with low overpotentials of 86 mV for HER and 246 mV for OER at 10 mA cm⁻² in an alkaline electrolyte. Moreover, compared to the commercial Pt/C || RuO₂/C system, the Co₂P–Co₃O₄/C || Co₂P–Co₃O₄/C system presents outstanding activity toward overall water splitting (1.55 V@10 mA cm⁻²), which is well maintained over long‐term (120 h) electrocatalysis. Density functional theory calculations show that the rich interfaces between Co₂P and Co₃O₄ offer a synergistic effect, which enables Co₂P–Co₃O₄/C as an excellent electrocatalyst toward both HER and OER.

DOI： 10.1002/sstr.202200235

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/sstr.202200235

Authorship：Last author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.139104

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.chemosphere.2022.137031

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.140933

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.139193

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Enlargement of micropores in zeolitic imidazolate framework particles into mesopores is achieved via an ethylene glycol-assisted aqueous etching method. The etched carbon shows a higher specific capacitance than unetched one at high scan rates.

DOI： 10.1039/d2ta06307g

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The trifunctional catalysts, Mg–Pt/meso-ZSM and Mg–Ni/meso-ZSM exhibit a higher increase in oil yield and enhanced selectivity toward alkenes and alkanes in oil than commercial ZSM-5 catalyst.

DOI： 10.1039/d3ta01368e

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

N, P-doped graphitic carbon/MXene heterostructures were constructed for advanced capacitive deionization electrodes, yielding superior salt adsorption capacity, rapid removal rate, and excellent cycling stability.

DOI： 10.1039/d3ta00696d

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A composite polymer electrolyte with ionic liquid grafted-LAP exhibits high conductivity and mechanical strength, contributing to dendrite-free all-solid-state lithium metal batteries.

DOI： 10.1039/d3sc01647a

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Conjugated microporous polymers (CMPs) are a prospective class of porous materials that are promising in a wide variety of applications due to their outstanding physical and chemical properties.

DOI： 10.1039/d2ta07966f

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The stereo-assembly of ultrathin Pd nanosheets in situ grown on the MXene surface was achieved via a convenient wet-chemical approach, which possess superior electrocatalytic performance for the methanol oxidation reaction.

DOI： 10.1039/d3sc03735e

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The activity of Ni–Mo catalysts for the hydrogen evolution reaction originates from the interfaces of alloy–oxide or alloy–hydroxide, in which the oxide or hydroxide promotes water dissociation and the alloy accelerates hydrogen combination.

DOI： 10.1039/d2sc06298d

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

We fabricated a range of N_y-MnO_x using compartmentalized microemulsion crystallization followed by post-calcination. These materials have the unique ability to generate sufficient ¹O₂ at room temperature without requiring an external field.

DOI： 10.1039/d3sc04418a

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Soft-hard interface has been developed by introducing conducting polymer hydrogels to improve the cycling electrochemical deionization performance of Prussian blue analogues.

DOI： 10.1039/d2mh01149b

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

This review covers the use of Prussian blue and its analogues as sacrificial templates and the adopted strategies to produce new materials with diverse compositions, structures and morphologies.

DOI： 10.1039/d2ta09501g

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A novel fused porphyrinoid undergoes supramolecular assembly to form a persistently porous solution processable material for sensing of acetone vapour under high humidity using a membrane-type surface stress sensor.

DOI： 10.1039/d2qm01039a

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The effect of metal–organic framework particle size on capacitive performance in oxygenated saline water was studied, suggesting that as particle size increases, the performance decreases.

DOI： 10.1039/d2cc06460j

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Hydrotalcites and their related materials hold great potential to unlock seawater splitting effectively.

DOI： 10.1039/d3ta02524a

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Nanosheet-like sorghum biomass obtained by mild alkaline treatment and high-energy ball milling is heteroatom-doped with N and S during pyrolysis. The resulting N, S co-doped carbon shows a significantly improved K-ion storage as an anode material in potassium ion batteries.

DOI： 10.1039/d3ta03215a

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Metal–organic framework (MOF) derivatives, such as pyrolytic carbons, pyrolytic metal-containing carbons, and MOF-based hybrids, have been designed to replace conventionally used carbon materials for promoting capacitive deionization performance.

DOI： 10.1039/d2ee03530h

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

We present a rational design of thiophene-based conjugated microporous polymers (CMPs) demonstrating their tunable adsorption reduction of toxic Cr(vi) ions with comparable performances.

DOI： 10.1039/d3ta00175j

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

Functional upcycling is post-polymerisation modification or surface functionalisation of plastic waste without considerable polymer chain destruction to produce a new upcycled material with added value.

DOI： 10.1039/d2cs00689h

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

The upcycling of waste polymers into novel materials with high added value is a vital task for modern chemical engineering.

DOI： 10.1039/d2ta08127j

Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Springer Science and Business Media LLC  

DOI： 10.1007/s12274-022-5250-1

Other Link： https://link.springer.com/article/10.1007/s12274-022-5250-1/fulltext.html

Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Flexible and implantable electronics hold tremendous promises for advanced healthcare applications, especially for physiological neural recording and modulations. Key requirements in neural interfaces include miniature dimensions for spatial physiological mapping and low impedance for recognizing small biopotential signals. Herein, a bottom‐up mesoporous formation technique and a top‐down microlithography process are integrated to create flexible and low‐impedance mesoporous gold (Au) electrodes for biosensing and bioimplant applications. The mesoporous architectures developed on a thin and soft polymeric substrate provide excellent mechanical flexibility and stable electrical characteristics capable of sustaining multiple bending cycles. The large surface areas formed within the mesoporous network allow for high current density transfer in standard electrolytes, highly suitable for biological sensing applications as demonstrated in glucose sensors with an excellent detection limit of 1.95 µm and high sensitivity of 6.1 mA cm⁻² µM⁻¹, which is approximately six times higher than that of benchmarking flat/non‐porous films. The low impedance of less than 1 kΩ at 1 kHz in the as‐synthesized mesoporous electrodes, along with their mechanical flexibility and durability, offer peripheral nerve recording functionalities that are successfully demonstrated in vivo. These features highlight the new possibilities of our novel flexible nanoarchitectonics for neuronal recording and modulation applications.

DOI： 10.1002/smll.202204946

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/smll.202204946

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Direct conversion of cyclohexane to adipic acid (AA) under mild conditions is an attractive technology in response to the increasing industrial demand of chemical intermediate AA. Exploring advanced free radical oxidation systems is the key to converting cyclohexane in a direct and mild manner. This study demonstrates that electrocatalytic water oxidation can quantitatively generate hydroxyl radicals (⋅OH) to selectively oxidize cyclohexane to AA by a vanadium oxide (VO_x)‐platinum (Pt) composite catalyst coupled with persulfate (PS) redox mediator at the electrode/electrolyte interface under ambient temperature and pressure. The three active components of VO_x, Pt, and PS can produce different concentrations of ⋅OH radicals alone or in combination, resulting in different AA selectivity and cyclohexane conversion, and the activity increased with the increase of free radical concentration before AA peroxidation. The optimized ternary oxidation system of VO_x‐Pt‐PS achieved a cyclohexane conversion of 85 % with 95 % AA selectivity and the corresponding yield was 81 %, better than most traditional oxidation systems. Electrochemical interfaces‐driven radical oxidation provides opportunities to oxidatively convert many other inexpensive hydrocarbons to value‐added chemicals.

DOI： 10.1002/cctc.202201220

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/cctc.202201220

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

Abstract

Artificial assembly of organic–inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer‐confined organic (polyaniline [PANI])–inorganic (MoS₂) hybrid with a dual charge‐storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS₂, expands the interlayer spacing of MoS₂, and increases the hydrophilicity. More in‐depth insights from the synchrotron radiation‐based X‐ray technique illustrate that the covalent grafting of PANI to MoS₂ induces the formation of MoN bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross‐layer electron transfer and decreases the diffusion barrier of K⁺ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic–inorganic heterostructures for superior K‐ion storage. The K‐ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X‐ray photoelectron spectroscopy.

DOI： 10.1002/smll.202204275

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/smll.202204275

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

A uniform nanoframe structure derived from a Prussian blue analogue (PBA) with an internal cavity is successfully synthesized by sonochemical etching. The uniquely structured PBA nanoframes possess a three-dimensional open structure and high surface area, resulting in enhanced electrochemical properties for the oxygen evolution reaction as a model reaction.

DOI： 10.1039/d2cc03253h

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier BV  

DOI： 10.1016/j.cej.2022.136344

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

Here, we report the synthesis of two-dimensional (2D) layered metal-organic framework (MOF) nanoparticle (NP) superstructures via an ice-templating strategy. MOF NP monolayers and bilayers can be obtained by regulating the concentration of colloidal MOF NPs without any external fields during self-assembly. Adjacent polyhedral MOF NPs are packed and aligned through crystalline facets, resulting in the formation of a quasi-ordered array superstructure. The morphology of the MOF layers is well preserved when subjected to pyrolysis, and the obtained carbon NPs have hollow interiors driven by the outward contraction of MOF precursors during pyrolysis. With the advantages of large surface areas, hierarchical porosity, high exposure of active sites, and fast electron transport of the 2D layered structure, the mono- and bilayered carbon NP superstructures show better oxygen reduction activity than isolated carbon particles in alkaline media. Our work demonstrates that ice-templating is a powerful strategy to fabricate superstructures of various MOFs and their derivatives.

DOI： 10.1021/jacs.2c06109

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

In this study, we present microporous carbon (MPC), hollow microporous carbon (HMC) and hierarchically porous carbon (HPC) to demonstrate the importance of strategical designing of nanoarchitectures in achieving advanced catalyst (or electrode) materials, especially in the context of oxygen reduction reaction (ORR). Based on the electrochemical impedance spectroscopy and ORR studies, we identify a marked structural effect depending on the porosity. Specifically, mesopores are found to have the most profound influence by significantly improving electrochemical wettability and accessibility. We also identify that macropore contributes to the rate capability of the porous carbons. The results of the rotating ring disk electrode (RRDE) method also demonstrate the advantages of strategically designed double-shelled nanoarchitecture of HPC to increase the overall electron transfer number (n) closer to four by offering a higher chance of the double two-electron pathways. Next, selective doping of highly active Fe-N-x sites on HPC is obtained by increasing the nitrogen content in HPC. As a result, the optimized Fe and N co-doped HPC demonstrate high ORR catalytic activity comparable to the commercial 20 wt% Pt/C in alkaline electrolyte. Our findings, therefore, strongly advocate the importance of a strategic design of advanced catalyst (or electrode) materials, especially in light of both structural and doping effects, from the perspective of nanoarchitectonics.

DOI： 10.1039/d2sc02726g

Web of Science

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Controlling the morphology, composition, and crystalline phase of mesoporous nonnoble metal catalysts is essential for improving their performance. Herein, well-defined P- and B-codoped NiFe alloy mesoporous nanospheres (NiFeB-P MNs) with an adjustable Ni/Fe ratio and large mesopores (11 nm) are synthesized via soft-template-based chemical reduction and a subsequent phosphine-vapor-based phosphidation process. Earth-abundant NiFe-based materials are considered promising electrocatalysts for the oxygen evolution reaction (OER) because of their low cost and high intrinsic catalytic activity. The resulting NiFeB-P MNs exhibit a low OER overpotential of 252 mV at 10 mA cm(-2), which is significantly smaller than that of B-doped NiFe MNs (274 mV) and commercial RuO2 (269 mV) in alkaline electrolytes. Thus, this work highlights the practicality of designing mesoporous nonnoble metal structures and the importance of incorporating P in metallic-B-based alloys to modify their electronic structure for enhancing their intrinsic activity.

DOI： 10.1002/smll.202203411

Web of Science

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry (RSC)  

A CNTs supported amorphous Ni–P alloy NPs catalyst is synthesized by a simple one-pot microwave heating method. The resulting outstanding hydrogenation performance is due to the high-dispersion of Ni–P NPs and the enhanced metal–support interaction.

DOI： 10.1039/d1ta10742a

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley  

DOI： 10.1002/smll.202104507

Other Link： https://onlinelibrary.wiley.com/doi/full-xml/10.1002/smll.202104507

Language：English  

DOI： 10.1002/sstr.202200015

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/adma.202201954

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/adma.202107212

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/adfm.202204714

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsami.2c15764

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acscatal.2c03480

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsnano.1c09615

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsnano.2c03188

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsnano.2c08245

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acssuschemeng.2c03315

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/jacs.2c00719

Language：English   Publisher：Springer Nature  

DOI： 10.1038/s41596-022-00718-2

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1cc04880e

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry ({RSC})  

A heterostructured porous carbon framework (PCF) composed of reduced graphene oxide (rGO) nanosheets and metal organic framework (MOF)-derived microporous carbon is prepared to investigate its potential use in a lithium-ion battery. As an anode material, the PCF exhibits efficient lithium-ion storage performance with a high reversible specific capacity (771 mA h g(-1) at 50 mA g(-1)), an excellent rate capability (448 mA h g(-1) at 1000 mA g(-1)), and a long lifespan (75% retention after 400 cycles). The in situ transmission electron microscopy (TEM) study demonstrates that its unique three-dimensional (3D) heterostructure can largely tolerate the volume expansion. We envisage that this work may offer a deeper understanding of the importance of tailored design of anode materials for future lithium-ion batteries.

DOI： 10.1039/D1CC05298E

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Scopus

PubMed

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1mh01882e

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1qi01613j

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1sc06314f

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1ta08741j

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1ta08837h

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1ta09019d

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d1ta09562e

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2dt01557a

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2mh00075j

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2sc00892k

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2sc02619h

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2sc04012c

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2sc05679h

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2ta00392a

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2ta01869a

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/d2ta06950d

Language：English   Publisher：Taylor and Francis Ltd.  

DOI： 10.1080/10643389.2021.1886891

Language：English   Publisher：Korea Nano Technology Research Society  

DOI： 10.1186/s40580-022-00300-2

Language：English   Publisher：Chemical Society of Japan  

DOI： 10.1246/bcsj.20210249

Language：English   Publisher：Chemical Society of Japan  

DOI： 10.1246/bcsj.20210286

Language：English   Publisher：Chemical Society of Japan  

DOI： 10.1246/bcsj.20220010

Language：English   Publisher：Tsinghua University Press  

DOI： 10.26599/NRE.2022.9120007

Language：English   Publisher：Tsinghua University Press  

DOI： 10.26599/NRE.2022.9120009

Language：English   Publisher：Chinese Chemical Society  

DOI： 10.31635/ccschem.022.202201892

Language：English   Publisher：MDPI  

DOI： 10.3390/magnetochemistry8070071

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acs.chemmater.2c00160

Language：English   Publisher：Royal Society of Chemistry  

DOI： 10.1039/D2TA00392A

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/admi.202102241

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsami.2c12804

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsami.1c20199

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acsami.1c19581

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acs.langmuir.2c00956

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acs.chemrev.1c00233

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acs.chemmater.2c01125

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/acs.chemmater.2c00999

Language：English   Publisher：American Chemical Society  

DOI： 10.1021/accountsmr.1c00258

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.snb.2022.131980

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.nantod.2022.101526

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.nanoen.2022.107652

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.nanoen.2022.107253

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.nanoen.2022.107146

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.nanoen.2021.106868

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.micromeso.2021.111579

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.jpowsour.2022.231776

Language：English   Publisher：National Engg. Reaserch Center for Magnesium Alloys  

DOI： 10.1016/j.jma.2022.01.010

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.jcou.2022.101883

Language：English   Publisher：Academic Press Inc.  

DOI： 10.1016/j.jcis.2022.04.114

Language：English   Publisher：Academic Press Inc.  

DOI： 10.1016/j.jcis.2022.02.039

Language：English   Publisher：Academic Press Inc.  

DOI： 10.1016/j.jcis.2021.09.125

Language：English   Publisher：Academic Press Inc.  

DOI： 10.1016/j.envres.2022.113331

Language：English   Publisher：Academic Press Inc.  

DOI： 10.1016/j.envres.2022.112909

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.ensm.2022.08.035

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2022.138065

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2022.137932

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2022.136939

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2022.136861

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.133851

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.133213

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.133161

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.133115

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.132965

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.132700

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.cej.2021.130946

Language：English   Publisher：Elsevier B.V.  

DOI： 10.1016/j.ccr.2022.214440

Language：English   Publisher：Elsevier Ltd  

DOI： 10.1016/j.cartre.2022.100168

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202203545

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202203147

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202107571

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202107450

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202107182

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202106629

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202105748

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202104847

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202104387

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202103617

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202102477

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/smll.202102397

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/cey2.213

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/anie.202203646

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/anie.202116179

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/anie.202114729

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/aenm.202200434

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/aenm.202103867

Language：English   Publisher：John Wiley and Sons Inc  

DOI： 10.1002/admi.202102560

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE SA  

The rational design and fabrication of ordered mesoporous materials with highly exposed surface area are of great significance to address the fundamental challenges in electrochemistry-related applications by providing more active sites and fast ion/gas diffusion channel. In this work, a self-template method is reported to prepare hollow-structured mesoporous carbon (HOMC) nanoplates by depositing resol-F127 micelles onto the surface of metal-organic-framework (MOF) nanoplates, followed by hydrothermal reaction and carbonization. The parameters influencing the morphology and microstructure of the HOMC materials, i.e., the MOF-to-resol-F127 ratio and the concentration of resol-F127 micelles, are systematically investigated. Fe-doped HOMC (Fe/ HOMC) is obtained after carbonization, as a result from adding FeCl3 during the hydrothermal reaction. Benefiting from morphological aspects, such as the nanoplate shape, the hollow structure, and mesoporous walls, the Fe/HOMC exhibits higher electrocatalytic activity and efficiency than the commercial Pt/C during oxygen reduction reaction (ORR). In addition, when compared to traditional Pt/C benchmark, the Fe/HOMC shows a superior durability and tolerance to methanol poisoning while operating for ORR. The assembled Zn-air battery possesses high power densities with excellent cycling stability. The strategy proposed here can provide a new avenue for the design of ordered mesoporous materials with hollow structure for a wide variety of applications.

DOI： 10.1016/j.cej.2020.127635

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier Ltd  

Here, we present a new family of hierarchical porous hybrid materials as an innovative tool for ultrasensitive and selective sensing of enantiomeric drugs in complex biosamples via chiral surface-enhanced Raman spectroscopy (SERS). Hierarchical porous hybrid films were prepared by the combination of mesoporous plasmonic Au films and microporous homochiral metal-organic frameworks (HMOFs). The proposed hierarchical porous substrates enable extremely low limit of detection values (10−12 M) for pseudoephedrine in undiluted blood plasma due to dual enhancement mechanisms (physical enhancement by the mesoporous Au nanostructures and chemical enhancement by HMOF), chemical recognition by HMOF, and a discriminant function for bio-samples containing large biomolecules, such as blood components. We demonstrate the effect of each component (mesoporous Au and microporous AlaZnCl (HMOF)) on the analytical performance for sensing. The growth of AlaZnCl leads to an increase in the SERS signal (by around 17 times), while the use of mesoporous Au leads to an increase in the signal (by up to 40%). In the presence of a complex biomatrix (blood serum or plasma), the hybrid hierarchical porous substrate provides control over the transport of the molecules inside the pores and prevents blood protein infiltration, provoking competition with existing plasmonic materials at the limit of detection and enantioselectivity in the presence of a multicomponent biomatrix.

DOI： 10.1016/j.bios.2021.113109

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

We have developed a simple soft template-mediated coupling construction approach to achieve an unexplored sandwiched mesoporous polypyrrole nanocoating/single-crystal Ag nanoplate hybrid by a one-step inorganic/organic redox reaction at the liquid interface, and the hybrid possesses an adjustable meso-structure and architecture, strong near-infrared absorption and Raman enhancement effect, and outstanding chemical sensing performance.

DOI： 10.1039/d1ta01110c

Scopus

Language：English   Publisher：WILEY  

Lithium-sulfur (Li-S) batteries have attracted particular interest as promising next-generation energy storage devices because of their high theoretical energy density and low cost. The real performance of Li-S batteries is, however, far from achieving the expected values, even when using a porous, highly conductive host of sulfurs to improve their electric conductivity and accommodate their volume changes. The performance restrictions are mainly attributable to the slow reaction kinetics of converting lithium polysulfides species to lithium sulfide and elemental sulfur during the charging and discharging processes, respectively. Recent studies show that single-atom catalysts (SACs) with superior catalytic activity offer an effective strategy for solving this tough issue. The recent advances in utilizing SACs for Li-S batteries, which involve catalyst preparation, battery performance, and mechanistic insights, are summarized here. Modification of the cathodes and separators with SACs helps to absorb polysulfide and promote their conversion kinetics, thus suppressing the notorious "shuttle effect." In addition, the introduction of SACs into Li-S batteries promotes the efficiency of Li stripping/plating and prevents the growth of Li dendrites. Overall, the boost effects of SAC on Li-S batteries performance are noticeable and deserving of more research attention to develop better Li-S batteries.

DOI： 10.1002/admi.202002159

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Metal-organic frameworks (MOFs) and covalent-organic frameworks (COFs) are promising precursors for preparing high-performance carbonaceous materials for capacitive deionization (CDI). However, the simple pyrolysis of single MOFs or COFs usually leads to carbonaceous materials with disadvantages in salt adsorption capacity (SAC) and cycling stability, which are unfavorable to the further development of CDI. To address this issue, herein, we report the directed core-shell motif hybridization of COFs on MOFs to obtain selectively functionalized carbonaceous precursors, NH2-MIL-125(Ti)@TP-DQ COF, which then produce titanium dioxide nanoparticle-embedded nitrogen-rich carbon architectures, called TiO2@COF, via pyrolysis. It is evidently expected that the resulting TiO2@COF possesses several advantageous features: (1) the inner core, which contains titanium dioxide nanoparticles, provides abundant faradic active sites for ion accommodation contributing additionally to the high SAC
(2) the outer capacitive shell, which is fibrous nitrogen-rich carbon, not only protects the inner core from the harsh environment of the solution and stabilizes the cycling performance but also affords plentiful nitrogen dopants for enhanced pseudocapacitive capacity and abundant pores for ion adsorption and electrolyte permeation
and (3) the outer COF-derived fibers interconnect with each other, giving rise to increasing electrical conductivity. As a result, TiO2@COF delivers a high SAC of 33.66 mg g-1 and favorable cycling stability over 40 cycles, significantly exceeding those of CDI electrodes derived from single MOFs or COFs. This work is expected to enrich the construction of selectively functionalized carbonaceous particles from MOFs and COFs and may also endow multiple promising applications of core-shell motif hybrids.

DOI： 10.1021/acs.chemmater.0c04129

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier Ltd  

Porous metallic aerogels are a new class of cutting-edge materials useful in catalysis because they combine high conductivity with low density and high surface area. However, the exploration of transition metal-based aerogels with core-shell architectures remains a fundamental challenge. Here, we report a one-step auto-programmed synthesis method to generate a core-shell Cu@Fe@Ni metallic aerogel. Electroactivating (EA) the core-shell Cu@Fe@Ni causes the Fe inner shell to migrate into the Ni outer shell and forms a highly-active catalytic hydroxide on the surface of the aerogel. The resulting EA-Cu@Fe@Ni catalysts exhibited a low OER overpotential of 240 mV at 10 mA cm-2, which is much smaller than bimetallic CuNi (320 mV), CuFe (390 mV), and RuO2 (271 mV). In-situ Raman measurements confirm that the catalyst's outer layer is composed of NiOOH doped with Fe during the electrochemical activation process, resulting in the high OER performance. This work describes the first example of a trimetallic core-shell aerogel synthesized in one step and enables another strategy for designing highly active metals/metal oxide electrocatalysts via surface reconstruction.

DOI： 10.1016/j.nanoen.2020.105644

Scopus

Language：English   Publisher：WILEY-V C H VERLAG GMBH  

In recent years, due to their structural diversity, adjustability, versatility, and excellent electrochemical properties, organic compounds with nitrogen-containing groups (OCNs) have become some of the most promising organic electrode materials. The nitrogen-containing groups acting as electrochemical active sites include carbon-nitrogen groups, nitrogen-nitrogen groups, nitrogen-oxygen groups in OCNs, and nitrogen-containing groups in covalent organic frameworks. The molecular structure regulation of OCNs with nitrogen-containing groups acting as electrochemical active centers can suppress dissolution in electrolytes, increase electronic conductivity, and improve the kinetics of redox reactions. The kinetics behavior and electrochemical characteristics of OCN electrode materials in alkali metal rechargeable batteries with organic electrolytes are reviewed, and the related relationships between the structure and electrochemical properties of OCNs are the core of this review. Herein, the electrochemical reaction mechanisms and the strategies to improve the electrochemical activity of nitrogen-containing groups in OCNs are clarified, and the conjugate molecular structure of OCNs is shown to be an important direction for improvement. These results will have implications for research on electrode materials and provide more choices for rechargeable batteries. Moreover, this work will guide the study of more efficient OCNs that can be used as electrode materials.

DOI： 10.1002/aenm.202002523

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Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier B.V.  

Mesoporous oxides are outstanding metal nanoparticle catalyst supports owing to their well-defined porous structures. Such mesoporous architectures not only prevent the aggregation of metal nanoparticles but also enhance their catalytic performance. Metal/metal oxide heterojunctions exhibit unique chemical and physical properties because of the surface reconstruction around the junction and electron transfer/interaction across the interface. This article reviews the methods used for synthesizing metal-supported hybrid nanostructures and their applications as catalysts for environmental remediation and sensors for detecting hazardous materials.

DOI： 10.1016/j.jhazmat.2020.123348

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Hosokawa Powder Technology Foundation  

This work demonstrates the fabrication of a nanoporous iron carbide-iron oxide/reduced graphene oxide (IC-IO/ rGO) hybrid via a controlled one-step thermal treatment of Prussian blue (PB)/GO hybrid at 450 °C under N2 flow. The PB/GO hybrid is initially prepared through the in-situ deposition of PB nanoparticles on the GO sheets through electrostatic interactions. The morphological analysis of the hybrid reveals the uniform coverage of the rGO sheets by IC-IO nanoparticles and the even distribution of carbon (C), oxygen (O), and iron (Fe) on the rGO nanosheets. As a result of the hybrid composition and controlled morphology, the surface area of the obtained IC-IO/rGO hybrid (~40 m2 /g) is significantly enhanced compared to those of the calcined GO sheets and PB nanoparticles (without GO).

DOI： 10.14356/kona.2021015

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

Concave metallic nanocrystals with a high density of low-coordinated atoms on the surface are essential for the realization of unique catalytic properties. Herein, mesoporous palladium nanocrystals (MPNs) that possess various degrees of curvature are successfully synthesized following an approach that relies on a facile polymeric micelle assembly approach. The asprepared MPNs exhibit larger surface areas compared to conventional Pd nanocrystals and their nonporous counterparts. The MPNs display enhanced electrocatalytic activity for ethanol oxidation when compared to state-of-the-art commercial palladium black and conventional palladium nanocubes used as catalysts. Interestingly, as the degree of curvature increases, the surface-area-normalized activity also increases, demonstrating that the curvature of MPNs and the presence of high-index facets are crucial considerations for the design of electrocatalysts.

DOI： 10.1021/acsami.0c13136

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier B.V.  

The design and construction of superior electrocatalysts based on covalent organic frameworks (COFs) for oxygen reduction reaction (ORR) have attracted increasing interest. However, COFs typically exhibit low electrocatalytic activity as a result of their poor electrical conductivity. In this study, a highly graphitic nitrogen-doped porous carbon electrocatalyst (GC@COF-NC) is fabricated by utilizing metal-organic framework (MOF)-derived GC@COF core-shell heterostructure as a sacrificial template. Featured with high conductivity, hierarchical porosity (micropores and mesopores), and abundant N doping, the resulting GC@COF-NC heterostructure manifests a high activity for ORR in an alkaline solution with exceptional onset and half-wave potentials, direct four-electron pathway, and good long-term stability. This synthetic strategy is expected to open a new avenue toward the construction of other COF-derived heteroatom-doped graphitic carbon heterostructures with promising potential for electrocatalytic applications.

DOI： 10.1016/j.cej.2020.125154

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier Ltd  

Hollow iron-doped Co–Mo sulfide (H–Fe–CoMoS) heterostructures with a highly efficient water-splitting catalytic ability were achieved by applying a multiscale optimization strategy. Morphological and compositional optimization on a macroscale achieved by assembling a bimetallic Co–Mo sulfide (CoMoS) heterostructure in a hollow-structured composite (H–CoMoS) gave the electrocatalyst an ability to conduct enhanced bifunctional activities for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Intrinsic electronic structure optimization on a microscale achieved by introducing a small amount of iron (Fe) into H–CoMoS (H–Fe–CoMoS) further improved its catalytic activity and stability. Electrochemical measurements revealed that this multiscale structural optimization promoted enhanced electrical conductivity and increased the number of electrochemical active sites on the H–Fe–CoMoS, leading to its remarkable electrocatalytic performance as a bifunctional catalyst for both HER and OER in alkaline media. The H–Fe–CoMoS showed overpotentials of 282 mV and 137 mV to achieve a current density of 10 mA cm−2 for OER and HER, respectively, which are comparable to the performance of the benchmark OER catalyst RuO2 and HER catalyst Pt/C.

DOI： 10.1016/j.nanoen.2020.104913

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Chemical Society of Japan  

The synthesis of high-performance porous carbon materials via carbonization of environment-friendly biomass fits perfectly with the concepts of sustainability and green chemistry. Herein, we report lignocellulose-derived porous carbon materials and their high capacitive deionization (CDI) performance, achieving a high salt adsorption capacity of 12.5 mg g11 and good cycling stability. The preparation of porous carbon materials via direct carbonization of lignocellulose provides a number of advantages, including cost-effectiveness, high production yields, and environment-friendliness, which are ideal for industrial application of CDI. This work not only suggests novel insights to design and prepare high-performance carbon materials but also highlights the significance of green chemistry using nature-provided biomass materials to synthesize porous carbon materials.

DOI： 10.1246/bcsj.20200055

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Mesostructured polydopamine (PDA) coating has been successfully achieved on the surface of zeolitic imidazolate framework-8 (ZIF-8) particles by incorporating Pluronic F127 (with a pore-expanding agent, 1,3,5-trimethylbenzene) as a pore-directing agent during dopamine polymerization. Upon pyrolysis at high temperatures, mesostructured PDA-coated ZIF-8 particles become hierarchically porous double-shell carbons (HPDCs) with a wide pore size distribution ranging from micro- A nd meso-to macropores. The formation of a hollow inner shell progresses initially with the shrinkage of ZIF-8 at the periphery where the interface interactions with mesostructured PDA exist, and then the subsequent disintegration of the ZIF-8 core at higher temperatures occurs. Our HPDCs prepared in this study feature physical and electrochemical advantages of hierarchically porous carbons such as high electrochemically accessible surface area, short diffusion distance, and high mass-transfer rate, thus demonstrating significantly improved ion diffusion and surface-enhanced high specific capacitance at high charge-discharge rates. HPDC5.0 therefore exhibits the capacitance retention of up to 76.7% from 1 to 10 A g-1 and maximum specific capacitance of 344.7 F g-1 at 1 mV s-1. It also possesses superior electrochemical stability with about 108% capacitance retention even after 10,000 consecutive cycles of galvanostatic charge-discharge at 10 A g-1.

DOI： 10.1021/acsami.0c07467

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

There is growing interest in developing mesoporous metallic alloys for electrochemical applications such as catalysts in fuel cells and batteries. As is well known, the chemical compositions of alloys can significantly affect their electrochemical properties. Although tuning the chemical compositions of mesoporous metallic alloys for enhancing the electrochemical activity has been reported, they have mostly been limited to binary components partly because experimental exploration over possible multi-compositional spaces is a time-consuming process. Here, we describe, for the first time, the application of the active learning scheme using Bayesian optimization for the exploratory search of the chemical compositions of mesoporous trimetallic PtPdAu alloys with optimum catalytic activity in the electrocatalytic oxidation of methanol. Unexpectedly, it was found that the PtPdAu alloys yielding the highest catalytic activity contain only a small percentage of Au. These compositions were discovered by performing only 47 experiments, less than 1% of all possible compositions in our experimental design. Our current approach is highly efficient and would be applicable to any system to accelerate the discovery of novel materials.

DOI： 10.1039/d0ta04096g

Scopus

Publishing type：Research paper (scientific journal)  

A new heterostructured material is synthesized with lamellar arrangements in nanoscale precision through an innovative synthetic approach. The self-assembled Ni-based cyano-bridged coordination polymer flakes (Ni-CP) and graphene oxide (GO) nanosheets with a layered morphology (Ni-CP/GO) are used as precursors for the synthesis of multicomponent hybrid materials. Annealing of Ni-CP/GO in nitrogen at 450 °C allows the formation of Ni3C/rGO nanocomposites. Grinding Ni-CP/GO and thiourea and annealing under the same conditions produces N,S-codoped reduced GO-wrapped NiS2 flakes (NiS2/NS-rGO). Interestingly, further heating up to 550 °C allows the phase transformation of NiS2 into NiS accompanied by the formation of a face-centered cubic (FCC-Ni) metal phase between NS-rGO layers (FCC-Ni-NiS/NS-rGO). Among all the materials, the resulting FCC-Ni-NiS/NS-rGO exhibits good electrocatalytic activity and stability toward the oxygen evolution reaction (OER) owing to the synergistic effect of multiphases, the well-designed alternating layered structures on the nanoscale with abundant active sites.

DOI： 10.1002/cssc.202000159

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Chemical Society of Japan  

To date, a wide variety of mesoporous metals has been synthesized using self-assembly of polymeric micelles for catalytic and sensing applications. However, systematic study of trimetallic mesoporous alloys has rarely been performed due to their complex nature. Herein, we demonstrate the synthesis of mesoporous PdPtRh particles by a chemical reduction process with the assistance of a block copolymer, Pluronicμ F127. Furthermore, we have also systematically characterized these alloys and evaluated their catalytic performance for methanol oxidation reaction (MOR), in comparison to mesoporous Pt and PdPt particles. Among all the prepared catalysts, the mesoporous PdPtRh sample shows the highest electrocatalytic performance for MOR with high conversion efficiency and tolerance for intermediate generation as well as excellent stability.

DOI： 10.1246/bcsj.20200128

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

The exploration of new carbon materials to overcome the rapid performance decay of common carbon materials in oxygenated saline water (i.e., natural saline water) is the biggest challenge for the industrial application of the capacitive deionization (CDI) technology. In this work, we first report the layer-by-layer motif synthesis of 3D interconnected metal-organic framework (MOF) tubes and the derived nitrogen-iron-doped carbon tubes (3D-FeNC tubes) by using continuous polymeric fibers as templates. The elaborately designed 3D-FeNC tubes exhibit multiple advantages, including fast ionic diffusion (originating from the 1D hollow structure of the tubes), efficient electronic pathways and abundant active sites (arising from the 3D interconnected carbon frameworks), which are beneficial for enhancing the oxygen reduction ability. As a consequence, the as-prepared 3D-FeNC tubes exhibit an unprecedented CDI performance in oxygenated saline water with an exceptional salt adsorption capacity of 40.70 mg g-1 and ultrahigh capacity retention of 93.82% even after 200 cycles, highlighting the significance of morphological control and the benefits of hollow structured materials.

DOI： 10.1039/c9mh01829h

Scopus

Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society (ACS)  

DOI： 10.1021/acsnano.9b08904

Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society ({ACS})  

DOI： 10.1021/acs.langmuir.9b02474

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley-VCH Verlag  

Although graphene nanomesh is an attractive 2D carbon material, general synthetic routes to produce functional graphene nanomesh in large-scale are complex and tedious. Herein, we elaborately design a simple two-step dimensional reduction strategy for exploring nitrogen-doped graphene nanomesh by thermal exfoliation of crystal- and shape-modified metal-organic frameworks (MOFs). MOF nanoleaves with 2D rather than 3D crystal structure are used as the precursor, which are further thermally unraveled into nitrogen-doped graphene nanomesh by using metal chlorides as the exfoliators and etching agent. The nitrogen-doped graphene nanomesh has a unique ultrathin two-dimensional morphology, high porosity, rich and accessible nitrogen-doped active sites, and defective graphene edges, contributing to an unprecedented catalytic activity for the oxygen reduction reaction (ORR) in acid electrolytes. This approach is suitable for scalable production.

DOI： 10.1002/anie.201906870

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PubMed

Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry ({RSC})  

DOI： 10.1039/C9TA09822D

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley-VCH Verlag  

Highly efficient earth-abundant electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are of great importance for renewable energy conversion systems. Herein, hollow porous heterometallic phosphide nanocubes are developed as a highly active and robust catalyst for electrochemical water splitting via one-step phosphidation of a NiCoFe Prussian blue analogue. Through modulation of the composition of metals in the precursors, the optimal NiCoFeP exhibiting increased electrical conductivity and abundant electrochemically active sites, leading to high electrocatalytic activities and outstanding kinetics for both HER and OER, is successfully obtained. NiCoFeP shows low overpotentials of 273 mV for OER and 131 mV for HER at a current density of 10 mA cm−2 and quite low Tafel slopes of 35 mV dec−1 for OER and 56 mV dec−1 for HER.

DOI： 10.1002/smll.201802442

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PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Two-dimensional (2D) metals are an emerging class of nanostructures that have attracted enormous research interest due to their unusual electronic and thermal transport properties. Adding mesopores in the plane of ultrathin 2D metals is the next big step in manipulating these structures because increasing their surface area improves the utilization of the material and the availability of active sites. Here, we report a novel synthetic strategy to prepare an unprecedented type of 2D mesoporous metallic iridium (Ir) nanosheet. Mesoporous Ir nanosheets can be synthesized with close-packed assemblies of diblock copolymer (poly-(ethylene oxide)-b-polystyrene, PEO-b-PS) micelles aligned in the 2D plane of the nanosheets. This novel synthetic route opens a new dimension of control in the synthesis of 2D metals, enabling new kinds of mesoporous architectures with abundant catalytically active sites. Because of their unique structural features, the mesoporous metallic Ir nanosheets exhibit a high electrocatalytic activity toward the oxygen evolution reaction (OER) in acidic solution as compared to commercially available catalysts.

DOI： 10.1021/jacs.8b05206

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PubMed

Publishing type：Research paper (scientific journal)  

A novel approach for hybridizing nanoporous NiCo oxide flakes with graphene sheets is reported. Positively charged cyano-bridged CoNi coordination polymer flakes (CoNi-CP) are mixed with graphene (G) suspension with negatively charged surface. Due to effective electrostatic interaction, both the materials are hybridized to form CoNi-CP/G composite. The as-prepared CoNi-CP/G composite is thermally treated in air, to remove the organic components without affecting the integrity of the parent G sheets. Through the thermal treatment, the CoNi-CP flakes wrapped into G sheets are converted to NiCo oxide, resulting in a new composite consisting of NiCo oxide flakes and G sheets. The NiCo-oxide/G composite shows the high specific capacitance (∼ 199 F g-1) at 5 mV/s, and features the good capacitance retention of ∼68% at 100 mV(∼ 135 F g−1).

DOI： 10.1002/slct.201801174

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Publishing type：Research paper (scientific journal)  

Herein, we report a novel method for the formation of hollow Prussian blue analogue (CoFe–PBA) nanocubes, using spherical silica particles as sacrificial templates. In the first step, silica cores are coated by a CoFe–PBA shell and then removed by etching with hydrofluoric acid (HF). The cubic shape of CoFe–PBA is well-retained even after the removal of the silica cores, resulting in the formation of hollow CoFe–PBA cubes. The specific capacity of the hollow CoFe–PBA nanocubes electrodes is about two times higher than that of solid CoFe–PBA nanocubes as storage materials for sodium ions. Such an improvement in the electrochemical properties can be attributed to their hollow internal nanostructure. The hollow architecture can offer a larger interfacial area between the electrolyte and the electrode, leading to an improvement in the electrochemical activity. This strategy can be applied to develop PBAs with hollow interiors for a wide range of applications.

DOI： 10.1002/open.201800120

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Triblock copolymer micelles coated with melamine-formaldehyde resin were self-assembled into closely packed two-dimensional (2D) arrangements on the surface of graphene oxide sheets. Carbonizing these structures created a 2D architecture composed of reduced graphene oxide (rGO) sandwiched between two monolayers of sub-40 nm diameter hollow nitrogen-doped carbon nanospheres (N-HCNS). Electrochemical tests showed that these hybrid structures had better performance for oxygen reduction compared to physically mixed rGO and N-HCNS that were not chemically bonded together. Further impregnation of the sandwich structures with iron (Fe) species followed by carbonization yielded Fe1.6-N-HCNS/rGO-900 with a high specific surface area (968.3 m2 g-1), a high nitrogen doping (6.5 at%), and uniformly distributed Fe dopant (1.6 wt %). X-ray absorption fine structure analyses showed that most of the Fe in the nitrogen-doped carbon framework is composed of single Fe atoms each coordinated to four N atoms. The best Fe1.6-N-HCNS/rGO-900 catalyst performed better in electrocatalytic oxygen reduction than 20 wt % Pt/C catalyst in alkaline medium, with a more positive half-wave potential of 0.872 V and the same limiting current density. Bottom-up soft-patterning of regular carbon arrays on free-standing 2D surfaces should enable conductive carbon supports that boost the performance of electrocatalytic active sites.

DOI： 10.1021/acsnano.8b01502

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Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier Ltd  

Low efficiency, short lifetimes, and limited kinds of catalysts are still three fundamental shortcomings that have plagued electrochemical water splitting. Herein, we rationally synthesized a cost-effective Co3S4@MoS2 hetero-structured catalyst that has proven to be a highly active and stable bifunctional catalyst for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline environment. The heterostructure was obtained via a first hydrothermal approach to obtain hollow Co3S4 nanoboxes based on the ionic exchange reaction between Fe(CN)6 3− of Co-Fe Prussian blue analogue (PBA) and S2− at 120 °C, and the subsequent in situ growth of MoS2 nanosheets on the surface of Co3S4 nanoboxes at an elevated temperature of 200 °C. The synergistic effects between the active and stable HER catalyst of MoS2 and the efficient OER catalyst of Co3S4, as well as the morphological superiority of hollow and core-shell structures, endow Co3S4@MoS2 with remarkable electrocatalytic performance and robust durability toward overall water splitting. As a result, the designed non-noble electrocatalyst of Co3S4@MoS2 exhibits a low overpotential of 280 mV for OER and 136 mV for HER at a current density of 10 mA cm−2 in an alkaline solution. Meanwhile, a low cell voltage of 1.58 V is achieved by using the heterostructure as both anode and cathode catalysts. This work paves the way to the design and construction of other prominent electrocatalysts for overall water splitting.

DOI： 10.1016/j.nanoen.2018.03.012

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

Herein, we report the synthesis of gold (Au)-loaded mesoporous iron oxide (Fe2O3) as a catalyst for both CO and NH3 oxidation. The mesoporous Fe2O3 is firstly prepared using polymeric micelles made of an asymmetric triblock copolymer poly(styrene-b-acrylic acid-b-ethylene glycol) (PS-b-PAA-b-PEG). Owing to its unique porous structure and large surface area (87.0 m2 g-1), the as-prepared mesoporous Fe2O3 can be loaded with a considerably higher amount of Au nanoparticles (Au NPs) (7.9 wt%) compared to the commercial Fe2O3 powder (0.8 wt%). Following the Au loading, the mesoporous Fe2O3 structure is still well-retained and Au NPs with varying sizes of 3-10 nm are dispersed throughout the mesoporous support. When evaluated for CO oxidation, the Au-loaded mesoporous Fe2O3 catalyst shows up to 20% higher CO conversion efficiency compared to the commercial Au/Fe2O3 catalyst, especially at lower temperatures (25-150 °C), suggesting the promising potential of this catalyst for lowerature CO oxidation. Furthermore, the Au-loaded mesoporous Fe2O3 catalyst also displays a higher catalytic activity for NH3 oxidation with a respectable conversion efficiency of 37.4% compared to the commercial Au/Fe2O3 catalyst (15.6%) at 200 °C. The significant enhancement in the catalytic performance of the Au-loaded mesoporous Fe2O3 catalyst for both CO and NH3 oxidation may be attributed to the improved dispersion of the Au NPs and enhanced diffusivity of the reactant molecules due to the presence of mesopores and a higher oxygen activation rate contributed by the increased number of active sites, respectively.

DOI： 10.1039/c7nr08895g

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PubMed

Publishing type：Research paper (scientific journal)  

We report a simple sol-gel method for the preparation of multilayered hybrid thin films composed of nanostructured SrTiO3 (STO) and BaTiO3 (BTO) layers. A nanoporous thin film of STO is prepared by the spin-coating method on Si/SiO2/Ti/Pt substrate. When the BTO is processed, the BTO is crystallized between STO crystal pores. A significant strain field is induced on the interface between the STO and BTO surfaces. The concave shape of the nanopores could enable the realization of a highly strained interfacial heterostructure composed of STO/BTO. Compared to nanostructured STO, BTO, and bilayer STO/BTO films, multilayered STO/BTO films show the highest dielectric constant and a high Curie temperature (Tc) at around 280 °C, which is suitable for electric capacitor applications.

DOI： 10.1021/acsanm.7b00310

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Mesoporous metals are useful for heterogeneous catalysis because their ultrapermeable architecture promotes mass transport to abundant active sites. Our group recently developed a method to manipulate the interior space of nanocrystals by synthesizing mesoporous Rh nanospheres that serve as high performance catalysts for methanol oxidation and nitric oxide (NO) remediation (Jiang, B.
et al. Nat. Commun. 2017, 8, 15581). Here, we extend this concept and propose a sophisticated soft-templating strategy to synthesize three-dimensional mesoporous bimetallic RhCu nanospheres. The nanospheres are alloys of Rh and Cu, and their compositions can be continuously tuned by varying the amount of metal precursors. The mesoporous RhCu nanospheres were examined for catalytic remediation of NO and show good catalytic performance considering the reduced economic cost of the alloyed material. This method offers a general approach for the precise design of high surface area Rh-based metal catalysts.

DOI： 10.1021/acs.chemmater.7b04307

Scopus

Publishing type：Research paper (scientific journal)  

DOI： 10.1166/jnn.2018.14553

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

Mesoporous hollow carbon spheres with Pt nanoparticles (NPs) loaded on their inner walls (Pt@HC-meso) have been designed and prepared through a dual-templating method. The core-shell structured Pt/SiO2@micelle-polydopamine (PDA) precursor is obtained by first depositing Pt NPs on silica spheres and then coating them with the carbon precursor of PDA and diblock copolymer micelles as soft templates. The subsequent carbonization and KOH etching convert the micelle-PDA shells into mesoporous carbon and remove the silica cores, respectively. Thus, the Pt NPs are subjected to calcination and left on the inner walls. The fabricated Pt@HC-meso achieved high electrocatalytic performance and outstanding stability in catalyzing methanol oxidation. We infer that the mesoporous carbon shells not only provide accessible diffusion pathways for the reactants, but also protect the inner Pt NPs from collision with Pt NPs in other hollow carbon spheres. Each hollow carbon sphere with Pt NPs inside can be regarded as an independent nanoreactor. Moreover, observations of the morphology have proved that the calcined Pt NPs avoid a second aggregation during the electrocatalytic process and maintain long-term stability.

DOI： 10.1039/c7nr07267h

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

A simple method is developed to assemble Mo2C nanocrystals on the surfaces of hollow, highly conductive mesoporous nanoparticles. Diblock copolymer (PS-b-PEO) micelles are used as templates to assist in the fast complexation of molybdate (MoO42-) and poly-dopamine (PDA) precursors to make hollow precursor MoO42-/PDA/PS-b-PEO particles. Then these particles are carbonized to generate mesoporous N-doped carbon nanosheets riddled with ultrafine molybdenum carbide (Mo2C) nanoparticles (MMo2C/NCS). An N-doped carbon matrix serves as an electron conductor and helps to prevent the aggregation of the Mo2C nanoparticles. The Mo2C nanoparticles in turn enhance the catalytic performance for the oxygen reduction reaction (ORR). The unique mesoporous 2D nanosheet and its derived 3D hollow structure expose numerous active catalytic sites while enabling free diffusion of the electrolyte and mass transfer. Based on these properties, MMo2C/NCS show enhanced catalytic activity for the ORR.

DOI： 10.1039/c7mh00586e

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：American Chemical Society  

Herein, we present a facile metal-organic framework-engaged strategy to synthesize hollow Co3S4@MoS2 heterostructures as efficient bifunctional catalysts for both H2 and O2 generation. The well-known cobalt-based metal-organic zeolitic imidazolate frameworks (ZIF-67) are used not only as the morphological template but also as the cobalt precursor. During the two-step temperature-raising hydrothermal process, ZIF-67 polyhedrons are first transformed to hollow cobalt sulfide polyhedrons by sulfidation, and then molybdenum disulfide nanosheets further grow and deposit on the surface of hollow cobalt sulfide polyhedrons at the increased temperature. The crystalline hollow Co3S4@MoS2 heterostructures are finally obtained after subsequent thermal annealing under a N2 atmosphere. Due to the synergistic effects between the hydrogen evolution reaction active catalyst of MoS2 and the oxygen evolution reaction active catalyst of Co3S4, the obtained hollow Co3S4@MoS2 heterostructures exhibit outstanding bifunctional catalytic performances toward both hydrogen and oxygen evolution reactions in acidic and alkaline media.

DOI： 10.1021/acs.chemmater.7b00867

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

We report a new approach for the fabrication of hybrid titanium dioxide/carbon materials derived from a porous titanium coordination polymer composed of a catechol-substituted porphyrin And Ti4+. Titanium dioxide nanocrystals were formed distributed in a nitrogen-doped carboniferous matrix after the thermolysis of the coordination polymer. The identity of the titanium dioxide phase, i.e., anatase or rutile, could be controlled by varying the thermolysis temperature. Electrochemical performances of the composites were explored with results demonstrating that the hybrid materials ate promising cathodic materials for the oxygen reduction reaction.

DOI： 10.1021/acsami.7b03305

Web of Science

Publishing type：Research paper (scientific journal)  

DOI： 10.1039/c7ra07810b

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

Here, ultrathin nitrogen-doped carbon/graphene nano-sandwiches were synthesized by carbonization of graphene oxide-based nanosheets, which were fully covered with ultrasmall ZIF-8 nanocrystals. The novel sandwich structure possesses large accessible surface area, excellent electrical conductivity, and high nitrogen content, thus showing superior desalination performance.

DOI： 10.1039/c7cc05673g

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

We report a one-pot synthetic strategy for the production of an efficient oxygen reduction reaction (ORR) electrocatalyst by the hybridization of hexagonally ordered mesoporous/crystalline tin phosphate (mesoSnPi) nanoflakes with thin layers of graphene oxide (GO). In the electrocatalytic measurements, the obtained nanocomposite (SnPi@GO) exhibited a superior electrocatalytic performance for ORR over mesoporous tin phosphate (mesoSnPi), bulk tin phosphate (bulkSnPi), bulk tin oxide (bulkSnO), various transition metal phosphate nanomaterials and most state-of-the-art manganese oxides.

DOI： 10.1039/c7cc01311f

Scopus

PubMed

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Wiley-VCH Verlag  

Cobalt sulfide/sulfur doped carbon composites (Co9S8/S-C) were synthesized by calcining a rationally designed sulfur-containing cobalt coordination complex in an inert atmosphere. From the detailed transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS) analyses, the electrocatalytically active Co9S8 nanoparticles were clearly obtained and combined with the thin sulfur doped carbon layers. Electrochemical data showed that Co9S8/S-C had a good activity and long-term stability in catalyzing oxygen evolution reaction in alkaline electrolyte, even better than the traditional RuO2 electrocatalyst. The excellent electrocatalytic activity of Co9S8/S-C was mainly attributed to the synergistic effect between the Co9S8 catalyst which contributed to the oxygen evolution reaction and the sulfur doped carbon layer which facilitated the adsorption of reactants, prevented the Co9S8 particles from aggregating and served as the electrically conductive binder between each component.

DOI： 10.1002/chem.201604162

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC  

Hybrid organic-inorganic metal halide perovskites have fascinating electronic properties and have already been implemented in various devices. Although the behavior of bulk metal halide perovskites has been widely studied, the properties of perovskite nanocrystals are less well-understood because synthesizing them is still very challenging, in part because of stability. Here we demonstrate a simple and versatile method to grow monodisperse CH3NH3PbBrxIx-3 perovskite nanocrystals inside mesoporous silica templates. The size of the nanocrystal is governed by the pore size of the templates (3.3, 3.7, 4.2, 6.2, and 7.1 nm). In-depth structural analysis shows that the nanocrystals maintain the perovskite crystal structure, but it is slightly distorted. Quantum confinement was observed by tuning the size of the particles via the template. This approach provides an additional route to tune the optical bandgap of the nanocrystal. The level of quantum confinement was modeled taking into account the dimensions of the rod-shaped nanocrystals and their close packing inside the channels of the template. Photoluminescence measurements on CH3NH3PbBr clearly show a shift from green to blue as the pore size is decreased. Synthesizing perovskite nanostructures in templates improves their stability and enables tunable electronic properties via quantum confinement. These structures may be useful as reference materials for comparison with other perovskites, or as functional materials in all solid-state light-emitting diodes.

DOI： 10.1021/jacs.6b05608

Web of Science

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Mesoporous Trimetallic PtPdRu Spheres with well-defined spherical morphology and uniformly sized pores were synthesized in an aqueous solution using ascorbic acid as the reducing agent and triblock copolymer F127 as the pore directing agent. These mesoporous PtPdRu spheres exhibited enhanced electrocatalytic activity compared to commercial Pt black, resulting in a similar to 4.9 times improvement in mass activity for the methanol oxidation reaction. The excellent electrocatalytic activity and stability are due to the unique mesoporous architecture and electronic landscape between different elements.

DOI： 10.1002/chem.201600774

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ELSEVIER SCIENCE BV  

Here we prepare thermo-responsive hydrogel containing mesoporous silica (KIT -6) with high surface area. Our hybrid hydrogel is prepared by gelation of NIPAM monomer with mesoporous silica particles in presence of cross linker. Owing to the doped mesoporous silica, a large amount of guest molecules are adsorbed easily. With increase of temperature, the hybrid hydrogel shrinks to retard the release of guest molecules. (C) 2015 Elsevier B.V. All rights reserved.

DOI： 10.1016/j.matlet.2015.12.132

Web of Science

Publishing type：Research paper (scientific journal)  

DOI： 10.1166/nnl.2016.2140

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Nanoporous pseudo Pd@Pt bimetallic particles were prepared using a facile one-step synthetic approach. The morphologies of the resultant particles are changed from spheres to cubes by increasing the molar ratio of the Pd/Pt precursor solution. Compared to commercially available Pt black and Pt/C-20%, the nanoporous pseudo Pd@Pt bimetallic particles were up to 7 times and 2.1 times more active for the methanol oxidation reaction on the basis of equivalent Pt, respectively. This excellent electrocatalytic activity is caused by a combination of the high surface area of the nanoporous architecture in addition to the bimetallic synergetic effect. Through this work, we demonstrate a general approach for the creation of nanoporous bimetallic Pt-based particles with controlled shape, composition and size for enhanced catalytic activity.

DOI： 10.1039/c6ta00037a

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

In this study, three-dimensional (3D) PdCu alloyed nanostructures, consisting of one-dimensional (1D) branches, were successfully synthesized through a facile wet-chemical method without using any seeds or organic solvent. The success of this approach relies on the use of hydrochloric acid (HCl) to control the reduction rate, and on the presence of bromide ions (Br-) to selectively adsorb on certain facets of the PdCu nucleus. The as-prepared 3D PdCu nanostructures exhibit a greatly enhanced catalytic activity toward formic acid oxidation, owing to a suitable electronic landscape resulting from the alloy structure and the unique morphology.

DOI： 10.1039/c5cc08581k

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

Core-shell-corona type triblock copolymer poly(styrene-b-2-vinylpyridine-b-ethylene oxide) (PS-b-P2VP-b-PEO) micelles have been selected here to direct the synthesis of mesoporous Pt-on-Pd spheres, consisting of a Pd concentrated core and a Pt shell, as established by elemental mapping. It is important to note that the size of the PS core determines the resultant size of the mesopores. A self-evaporation method has been developed to prepare swollen micelles, so as to further enlarge the pore size (∼40 nm). Compared with commercially available catalysts (e.g., Pt black or Pt, 20 wt% on carbon black), good oxygen reduction reaction performance on the mesoporous Pt-on-Pd spheres is observed, due to the exposure of the most active Pt (111) planes and the synergistic effects from Pt and Pd in the pseudo core-shell structure.

DOI： 10.1039/c6ta02526a

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Elsevier Ltd  

Palladium-introduced ordered mesoporous carbon (Pd-C) composite materials were prepared through a facile co-assembly process by employing nonionic block copolymers (Pluronic F127) as a structure-directing agent, low-molecular weight phenolic resin (resol) as a carbon precursor and tetraethyl orthosilicate and palladium chloride as additives. The addition of Pd nanoparticles (less than 9 wt.%) were well-dispersed throughout the Pd-C frameworks without destroying the ordered tubular mesochannels. Layered graphitic sheets were readily formed due to the catalytic graphitization of amorphous carbon by Pd nanoparticles, leading to an increased crystallinity and electronic conductivity of carbon support (Pd-C). The Pt/Pd-C catalysts were prepared by loading Pt nanoparticles onto the Pd-C supports. Abundant Pt nanoparticles with an average size of 3 nm were well-deposited onto the Pd-C framework by the means of the distributed anchor sites of Pd nanoparticles, finally increasing the utilization of Pt catalyst. Herein, the Pt catalyst supported on Pd-C composite materials exhibited much higher electrochemical active surface areas compared to Pt catalysts supported on pure ordered mesoporous carbon because of its increased electronic conductivity, active anchor sites and electrocatalytic active Pd nanoparticles.

DOI： 10.1016/j.electacta.2015.04.154

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：Royal Society of Chemistry  

We report a simple method for the preparation of ternary PtPdCu spheres with a three-dimensional (3D) nanoporous structure in a solution phase. The structure, composition, and electronic states of the obtained material are characterized and studied by various physical techniques. By varying the amount of Cu precursor involved in the reaction, the composition of the spheres can be adjusted without affecting the morphology. Due to the nanoporous structure and the multimetallic synergetic effect, our ternary nanoporous PtPdCu spheres exhibited 1.7, 2.8, and 4.9 times higher activity than that of binary nanoporous PtPd spheres, dendritic Pt, and commercial Pt black catalysts, respectively.

DOI： 10.1039/c5ta02951a

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Here we propose a novel way to construct mesoporous architectures through evaporation-induced assembly of polymeric micelles with crystalline nanosheets. As a model study, we used niobate nanosheets exfoliated by the direct reaction of K4Nb6O17 center dot 3H(2)O crystals with an aqueous solution of propylamine. The electrostatic interaction between negatively charged nanosheets and positively charged polymeric micelles enable us to form composite micelles with the nanosheets. Removal of the micelles by calcination results in robust mesoporous oxides with the original crystalline structure.

DOI： 10.1002/anie.201410942

Web of Science

Scopus

Publishing type：Research paper (scientific journal)  

DOI： 10.1021/jacs.5b06278

Scopus

Language：English   Publishing type：Research paper (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Pt-decorated mesoporous silica is directly prepared using a polymeric micelles assembly approach using an asymmetric triblock copolymer, poly(styrene-b-2-vinylpyridine-b-ethylene oxide) as the structure directing agent. Strongly immobilized, fully accessible, and uniformly dispersed Pt nanoparticles on mesoporous silica wall exhibit superior catalytic activity toward CO oxidation.

DOI： 10.1039/c4cc02556c

Web of Science

Language：English   Publishing type：Research paper (scientific journal)   Publisher：AMER CHEMICAL SOC