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

Twinned structure of metal nanoparticles can strongly affect catalysis because of its unique atomic alignment and bond strain in metal nanoparticles. Here, the twin and single crystal structures of supported Ag nanoparticles are controlled reversibly by gas treatment. The single crystal Ag nanoparticles were formed in Ag/Al2O3 by H2 treatment, and subsequent CO gas treatment changed the Ag particle structure to twin. The change in the Ag particle structure from single to twin caused enhancement of CO oxidation activity. In addition, the catalytic activity was reversibly changed from low to high by applying H2 and CO gas treatment to Ag/Al2O3. The kinetic analysis for CO oxidation revealed that the twin Ag nanoparticles have stronger CO adsorption energy than the single crystal ones, which is responsible for the enhanced CO oxidation activity of twin Ag nanoparticles.

DOI： 10.1016/j.cattod.2022.06.029

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Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Catalysis Surveys from Asia  

A combination of two base-metal oxides in tandem configuration can realize three-way reaction without platinum group metals. For this purpose, catalysts for hydrocarbon preferential oxidation (HC-PROX) and for NO reduction by CO are required. For the design of HC-PROX catalysts, competitive oxidation of propene and CO on spinel-type MFe2O4 (M = Co, Cu, Mg, Mn, Ni, Zn) was investigated. MnFe2O4 preferentially oxidized propene in the co-presence of CO showing the best propene oxidation activity. Among the series of MFe2O4, the activity controlling factor was correlated to the M-O bond energy of the second metal oxides, and the preference for HC oxidation was dependent on the electronegativity of the second ion. A tandem catalyst using MnFe2O4 for HC-PROX and CuCo2O4 for NO-CO reaction showed TWC activity comparable to a Rh/CeO2.

DOI： 10.1007/s10563-022-09373-9

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Applied Surface Science  

We theoretically investigated surface modification of MCr2O4 (M = Mg and Zn) by Cu-doping and doping effects on catalytic activity for CO oxidation. DFT + U calculations elucidated that Cu-dopants in MCr2O4(1 1 1) exist on the surface layer, CO oxidation by Cu-doped MCr2O4(1 1 1) occurs through Mars van Krevelen mechanism, rate-determining step (RDS) is the first CO2 desorption with oxygen vacancy (OV) formation, and the catalytic activity is enhanced very much by Cu-doping. Also, we experimentally observed that CO conversion was dramatically improved to 70% by the Cu-doped ZnCr2O4 from 5.2% by non-doped ZnCr2O4 at 300 °C. Bader charge analysis and difference density map show that M atom on the MCr2O4 surface receives electron density from the dissociating O atom in the OV formation step and the Cu-dopant can receive more electron density than Mg and Zn atoms to facilitate the OV formation and accelerate the first CO2 desorption(RDS). This larger capability of Cu-dopant for receiving electron density results from the facts that the Cu atom has large electronegativity and + I oxidation state besides + II in metal oxide but Mg and Zn have small electronegativity and only + II oxidation state.

DOI： 10.1016/j.apsusc.2022.154681

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Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)   Publisher：Catalysis Science and Technology  

Direct catalytic conversion of methane to value-added chemicals with a high reaction rate and selectivity under mild conditions remains a great challenge. Rh-supported zeolite is one of the promising heterogeneous catalysts capable of selectively oxidizing methane to acetic acid using carbon monoxide and oxygen at low temperatures. However, the difficulty in the preparation of the catalytically active species, i.e., zeolite-confined RhI single-atom sites, has limited the mass activity. Here, we successfully prepared a highly-active Rh-containing zeolite using RhCl3 molten salt. By high-temperature treatment of the physically-mixed H+-MFI zeolite and bulk RhCl3, the RhCl3 molten salt was formed under in situ conditions and then diffused into the zeolite pores, resulting in being trapped within the zeolite cavity via host-guest interaction and ion-exchange with H+. The encapsulated RhCl3 species are efficiently dispersed with the formation of RhI single-atom species as the active sites in the catalytic reaction, boosting the direct conversion of methane to acetic acid with a record turnover frequency (592 mol molRh−1 h−1) and yield (14.6 mmol gcat−1 h−1) with high selectivity (76.9%).

DOI： 10.1039/d2cy01471h

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Authorship：Last author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Catalysis Science and Technology  

A Pt-based CO oxidation catalyst that works even at low temperatures is desirable for industrial applications; however, its development is highly challenging because of Pt's high affinity toward CO. Here, we develop a PtIV single-atom/β-MnO2 composite metal-oxide surface (PtIV1/β-MnO2). Single PtIV sites were stably formed on the high surface β-MnO2 by strong interaction with MnIV defect sites. The resulting PtIV-O-MnIV local structures served the lattice oxygens as an oxidant to catalyze low-temperature oxidation of CO. PtIV1/β-MnO2 was highly resistant to CO poisoning because of the high-valence state of the PtIV single-atom sites. Aided by these geometric and electronic features, the CO oxidation was catalyzed with reaction rates of 0.676 and 0.206 molCO h−1 gPt−1 at 25 °C and 0 °C, respectively, under the O2-rich conditions (O2 : CO ratio of 66.7). These are record rates in the literature for Pt-based catalyst application for low-temperature CO oxidation under near atmospheric conditions.

DOI： 10.1039/d2cy00677d

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Authorship：Last author,　Corresponding author   Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Journal of Catalysis  

For the design of a high-performance platinum group metal-free three-way catalyst, we propose a new C3H6-preferential oxidation (C3H6-PROX) catalyst under stoichiometric automobile exhaust gas (NO–CO–C3H6–O2) using supported vanadia catalysts. Among various V2O5 supported catalysts, V2O5/TiO2 (anatase, coverage of around one monolayer) showed the best activity for C3H6-PROX with preferable formation of CO. The tandem catalyst combination using V2O5/TiO2 as the upstream C3H6-PROX catalyst and Cu/CeO2 as the downstream NO–CO reaction catalyst showed comparable activity for NO reduction as a Rh/ZrO2 catalyst. The reaction mechanism of C3H6 oxidation was analyzed using in situ Infrared spectroscopy. The C3H6 oxidation progressed with the formation of surface acetate as an intermediate, and acetate consumption was the key step of C3H6 oxidation. It is suggested that the Brønsted acid promoted the cleavage of the C–C bond of acetate, therefore, the number of Brønsted acid sites is one of the critical factors for the higher performance of C3H6-PROX catalysts.

DOI： 10.1016/j.jcat.2022.03.012

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

DOI： 10.1021/acsomega.1c06208

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

DOI： 10.1016/j.apcata.2021.118425

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

Iron-containing zeolites possess active sites capable of catalyzing the low-temperature partial oxidation of methane using hydrogen peroxide as an environmentally benign oxidant. However, only a trace number of active sites have been found in zeolites so far. The high turnover frequency was limited to low loading samples, resulting in an upper limit of similar to 50 mmol g(cat)(-1) h(-1) yield of C1 oxygenates. In this study, we synthesized a ZSM-5 catalyst containing a high concentration of single Fe sites with a high turnover frequency, and achieved a conversion of methane to C1 oxygenates of similar to 200 mmol g(cat)(-1) h(-1) yield. It was important to use ZSM-5 as a carrier, which can be synthesized by hydrothermal treatment of aluminosilicate gel containing only tetra-propyl ammonium cations as the structure-directing agent (SDA). This ZSM-5 carrier has a large fraction of local environments possessing the nearest framework AlO4 tetrahedra required for the fixation of Fe cations in the mononuclear state while suppressing the co-generation of oligomeric Fe sites, making it possible to design a reaction field for the highly efficient partial oxidation of methane. The findings in the present study clearly showed that the fraction of single Fe cations and the Al distribution in the zeolite matrix are powerful activity descriptors for this class of materials. Furthermore, Al-distribution modification based on previously-established protocols, i.e., rational choice of an SDA used in the zeolite synthesis, is a meaningful way to tune not only the fabrication efficiency of single Fe cations but also the catalytic performance of Fe/ZSM-5 catalysts.

DOI： 10.1039/d1cy01987b

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Journal of Physical Chemistry C  

Noble gas (Ng) elements are stable because of their octet electronic configuration, and thus Ng capture and purification are highly challenging. Here, we show a new concept for these applications: an orbital trap for Xe. This concept was found in Xe adsorption/separation processes at room temperature (RT) at the single Ag(I) site in MFI zeolite. Experiments and calculations showed the zeolite lattice-coordinated Ag(I) single ion has excellent electron-accepting nature and thereby induces the Xe 5p → Ag(I) 5s donation orbital interaction, forming a stable σ-bond with Xe even in the lower-pressure region and at RT. By contrast, the stable σ-bond for Kr adsorption is not established at RT because of the instability of the orbital interactions of the Kr 4p → Ag(I) 5s donation, as reflected from the relatively high energy of the Kr 4p orbital. Thus, the single Ag(I) site allows it to distinguish between Xe and Kr at RT; the Xe separation from the Xe/Kr gas mixture was achieved at RT using the Ag/MFI containing a high concentration of single Ag(I) sites. Our findings suggest that the orbital Xe trap using the local structure of porous materials shows promise as an efficient approach to selectively collect Xe (air concentration 0.087 ppm only). It will help to expand the range of applications of the costly Xe.

DOI： 10.1021/acs.jpcc.2c01515

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

DOI： 10.1021/acs.jpcc.1c06760

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

DOI： 10.1021/acsanm.1c00128

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

Pd/Al2O3 catalysts were prepared using various Al2O3 supports with different structural features such as crystalline phase and crystallinity related to Al3+ coordination, revealing a significant insight into the methane (CH4) combustion activity of Pd nanoparticles with the fraction of penta-coordinated Al3+ sites in the Al2O3 supports.

DOI： 10.1039/d1cy00098e

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

DOI： 10.1021/acs.jpcc.1c01042

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

DOI： 10.1627/jpi.64.166

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

DOI： 10.1039/d0cy01989e

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

DOI： 10.1016/j.jcat.2020.11.006

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

DOI： 10.1039/d0cy01294g

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Journal of Physical Chemistry Letters  

Isolation of the atomic O radical anion bound to a metal ion (metal-oxyl) on solid surfaces is highly desirable for an understanding of how we should design the surface structure for using oxyl as the reactive site. Owing to the analytical difficulty of oxyl, however, even identification of oxyl remains scarce. Herein, we report isovalent ZnII-oxyl and GaIII-oxyl bonds isolated in the zeolite matrix. Close similarities in reactivity, spectroscopic property, and bonding nature were observed between them, but their site requirements were entirely different; the former is generated at the monovalent ion-exchangeable site, whereas the latter at the divalent ion-exchangeable site. This study strongly suggests that tuning the polarization of the metal-oxygen bond using the charge-controlled lattice oxygens is a useful way to constrain surface metal-oxyl bonds.

DOI： 10.1021/acs.jpclett.0c02980

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

DOI： 10.1021/acscatal.0c03425

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

DOI： 10.1246/CL.200856

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

DOI： 10.1021/acscatal.0c02050

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

DOI： 10.1016/j.cattod.2019.12.002

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1039/d0cy00017e

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

DOI： 10.1021/acsami.0c05938

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

The selective catalytic reduction of NO with ammonia (NH3-SCR) catalyzed by Cu-CHA zeolites is thoroughly investigated using in situ spectroscopic experiments combined with on-line mass spectroscopy (MS) under steady-state NH3-SCR conditions and transient conditions for Cu(II)/Cu(I) redox cycles. Quantitative analysis of the in situ XANES spectra of Cu-CHA under steady-state conditions of NH3-SCR show that NH3-coordinated Cu(II) species is the dominant Cu species at low temperatures (100-150 degrees C). At higher temperatures, Cu(II) species and [Cu(NH3)(2)](+) complex coexist, possibly because the rate of the Cu(II) -> Cu(I) reduction step is comparable to that of the Cu(I)-> Cu(II) oxidation step. In situ XANES, IR/MS, and UV-vis/MS experiments on the reduction half cycle demonstrate that the reduction of Cu(II) species occurs via the reaction of NH3-liganded Cu(II) with NO to yield N-2 and H2O. For the oxidation half cycle, in situ XANES experiments of Cu(I) oxidation in 10 % O-2 at 200 degrees C indicate that an increased density in CHA zeolite exhibits a higher oxidation rate. In situ UV-vis experiments of Cu(I) reoxidation using different mixtures of oxidant feed gas demonstrate the key role of O-2 in the oxidation cycle. It is suggested that the reoxidation of Cu(I) to Cu(II) species occurs with only O-2 as the oxidant, and a high Cu density in CHA zeolite promotes SCR activity by enhancing the oxidative activation of Cu(I) to Cu(II) during the catalytic cycle.

DOI： 10.1002/cctc.202000024

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

DOI： 10.1021/acsami.0c00506

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

Anion exchange membrane fuel cells (AEMFCs) have been developed to the extent that the cell performance is nearing that of conventional proton exchange membrane fuel cells. For further improvement of AEMFC cell performance, it is necessary to develop the catalysis of hydrogen oxidation reactions (HORs) under basic conditions at the anode. Here, significant poisoning of Pt/C under basic conditions is demonstrated by electrochemical active surface area (ECSA) analysis using not only electrochemical measurement but also in situ Pt L-3-edge X-ray adsorption spectroscopy (XAS). Furthermore, the in situ XAS analysis reveals that the surface modification of Pt/C with another metal species improves the ECSA of the Pt nanoparticles by removal of the surface poisoning, which contributes to the enhanced HOR performance of the modified Pt/C catalysts. Therefore, the removal of poisoning is proposed as a mechanism for improving the HOR on Pt-based catalysts.

DOI： 10.1021/acsaem.9b02274

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Language：Japanese   Publishing type：Research paper (scientific journal)  

The modification of Cu-exchanged zeolites with phosphorus represents a promising method to enhance their hydrothermal stability, which is of pivotal importance for catalysts that promote the selective catalytic reduction of NO with ammonia (NH –SCR). In this study, we investigated the reaction mechanism of NH –SCR catalyzed by a phosphorus-modified CHA zeolite that contains active Cu species (Cu-P-CHA), and assessed the effect of the phosphorus modification on the hydrothermal stability of the catalyst by employing in situ/operando spectroscopic methods. In their entirety, the combined results from in situ/operando IR, UV–vis, and XANES experiments revealed that the NH –SCR process over Cu-P-CHA proceeds via the reduction of Cu(II) to Cu(I) followed by a reoxidation of Cu(I) to Cu(II). In addition, we found that the phosphorus modification improved the hydrothermal durability of the catalyst by retaining a higher amount of the redox-active Cu species and the zeolite framework. 3 3 3

DOI： 10.1016/j.cattod.2020.07.084

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/ACSCATAL.9B04524

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

DOI： 10.1039/c9cy00158a

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

DOI： 10.1021/acscatal.9b00526

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

DOI： 10.1039/c9cc00582j

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：ECS Transactions  

The cell performance of anion exchange membrane fuel cells (AEMFCs) has been getting closer to that of proton exchange membrane fuel cells (PEMFCs) by improvement of hydrogen oxidation reaction (HOR) catalysts on anodes with the help of the state-of-the-art AEMs having high ion conductivity. However, development of the alkaline HOR catalysts is still demanded to reduce the usage of precious metals on AEMFC anode. Here, Pt/C catalyst is modified to improve the HOR activity using fifteen metals on the group 4-11 of the 4th and 5th period in the periodic table except for Tc, i.e., Ti, V, Cr, Mn, Fe, Co, Ni, Cu, Zr, Nb, Mo, Ru, Rh, Pd, Ag. In addition, the hydrogen binding energy of modified Pt/C and the oxophilicity of modifying metals are evaluated to reveal the mechanism of improved/lowered HOR activity.

DOI： 10.1149/09208.0733ecst

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Catalysis  

In situ and operando analyses are the methods to observe the real features of catalysts under the reaction conditions. These methods can clarify the dynamics of active species of catalysts and reaction scheme on catalyst surface through transient response method, kinetic study, temperature dependence of catalysts and products, and so on. In this review, progress in in situ and operando analyses is summarized with emphasis on environmental catalysts, i.e., catalysts for combustion, selective reduction of NO, automotive three-way catalysis, and related materials.

DOI： 10.1039/9781788016971-00242

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1002/CHEM.201902994

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1246/CL.190462

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/ACS.JPCC.9B03687

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Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1039/C9CP03943K

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

DOI： 10.1093/jmicro/dfy036

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Chemical Record  

Supported bimetallic catalysts have been studied because of their enhanced catalytic properties due to metal-metal interactions compared with monometallic catalysts. We focused on galvanic deposition (GD) as a bimetallization method, which achieves well-defined metal-metal interfaces by exchanging heterogeneous metals with different ionisation tendencies. We have developed Ni@Ag/SiO2 catalysts for CO oxidation, Co@Ru/Al2O3 catalysts for automotive three-way reactions and Pd−Co/Al2O3 catalysts for methane combustion by using the GD method. In all cases, the catalysts prepared by the GD method showed higher catalytic activity than the corresponding monometallic and bimetallic catalysts prepared by the conventional co-impregnation method. The GD method provides contact between noble and base metals to improve the electronic state, surface structure and reducibility of noble metals.

DOI： 10.1002/tcr.201700084

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：ChemCatChem  

The highly active species of Pd/Al2O3 catalysts for methane combustion was revealed by in situ time-resolved dispersive X-ray absorption fine structure (DXAFS) spectroscopy. By using CH4 as a reduction agent, PdO in Pd/Al2O3 is reduced in a 2-step model involving Pd0 nucleation and growth of Pd0 domain in a PdO particle. Kinetic analysis of the 2-step model reduction of PdO nanoparticles leads to a suggestion that partial formation of Pd0 in a PdO particle accelerates methane combustion.

DOI： 10.1002/cctc.201800573

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

A series of ceria-supported Rh nanoparticles (NPs) that have various particle sizes of 2–7 nm was prepared to investigate the size effect of Rh NPs on NO reduction in NO–CO–C3H6–O2 under stoichiometric conditions. The turnover frequency (TOF) for NO reduction on Rh NPs increased drastically according to their particle size. The strong size dependence of the TOF was attributed to the oxidation states of Rh NPs but not to particle geometries, which include fractions of surface local sites (e.g., corner, edge, plane) and the surface crystal structures (e.g., Rh(1 1 1), (1 0 0)). The variation of the TOF with the Rh metal fraction suggested that Rh metal ensembles are highly active species for NO reduction.

DOI： 10.1002/cctc.201701842

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

The NOx reduction activity of NiFe2O4 in automotive three-way catalysis was enhanced by physical mixing with CeO2, MgO, ZrO2, and Al2O3, while the mixing with TiO2 and Nb2O5 did not promoted the catalytic activity. On both pure NiFe2O4 and the physically mixed catalysts, NO was mainly reduced by C3H6 under the NO-C3H6-CO-O2 reaction conditions, because the temperature dependence of NO conversion in NO-C3H6-CO-O2 reaction was the same as that in NO-C3H6-O2 reaction. The in-situ FT/IR measurement revealed that the NO reduction proceeded with (1) partial oxidation of C3H6 to surface carboxylates, i.e., acetate and formate as good reductants for NO, and (2) reduction of NO by surface carboxylates. The metal oxide additives did not have catalytic activity for partial oxidation of C3H6 nor for NO oxidation to NO2, except CeO2. The main promotion effect was attributed to storage and release of surface carboxylates by metal oxide additives.

DOI： 10.1016/j.cattod.2017.07.026

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

We report herein the first general catalytic system for the direct synthesis of N-substituted γ- and δ-lactams by reductive amination/cyclization of keto acids (including levulinic acid) with nitriles and H2 under mild conditions (7 bar H2, 110 °C, solvent free). The most effective catalyst, Pt and MoOx co-loaded TiO2 (Pt-MoOx/TiO2), shows a wide substrate scope, high turnover number (TON), and good reusability.

DOI： 10.1002/cctc.201701355

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

DOI： 10.1007/978-981-10-5137-1_5

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

The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/, -Al2O3 with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/-Al2O3 increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al2O3 for methane combustion.

DOI： 10.1002/anie.201709124

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

We studied the dynamic redox behavior of Cu species in zeolite matrix under NH3-SCR using in situ XAFS. Cu2+ species were slowly reduced to Cu+ in flowing NH3, and subsequent addition of NO promoted the reduction to Cu+. In the oxidation step, oxygen alone did not fully oxidize Cu+ to Cu2+, but the Cu+ species were completely oxidized to Cu2+ by NO-O-2. The oxidation step was slower than the reduction step, which suggested that the oxidation step (Cu+ -> Cu2+) is the slow step of the NH3-SCR reaction.

DOI： 10.1246/cl.170451

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

To elucidate the reaction mechanism of NO-C3H6-CO-O2 over NiFe2O4, we investigated the dynamics of the adsorbed and gaseous species during the reaction using operando Fourier transform infrared (FTIR). The NO reduction activity dependent on the C3H6 and CO concentrations suggested that NO is reduced by C3H6 under three-way catalytic conditions. From FTIR measurements and kinetic analysis, it was clarified that the acetate species reacted with NO-O2 to form N2 via NCO, and that the rate-limiting step of NO reduction was the reaction between CH3COO- and NO-O2. The NO reduction mechanism of the three-way catalyst on NiFe2O4 is different to that on platinum-group metal catalysts, on which NO reduction proceeds through N-O cleavage.

DOI： 10.1021/acsomega.7b00165

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

Glucose isomerization was performed using various titanate catalysts, which include SrTiO3, BaTiO3, CaTiO3, Na2Ti6O13, K2Ti6O13, and Sr3Ti2O7, prepared using a conventional solid-phase method. Among the titanates, SrTiO3, CaTiO3, and Na2Ti6O13 offered a relatively high fructose yield (32%) with a high selectivity (68-78%). The yields are comparable to yields reported previously using a Sn-modified BEA zeolite, which shows a high efficiency for glucose isomerization as a Lewis acid catalyst. A study of the mechanism of glucose isomerization on a SrTiO3 catalyst surface by using H-1 NMR spectroscopy suggested that the titanates catalyze the isomerization as base catalysts. Thus, the effect of the basicity of the titanates on glucose isomerization was investigated in terms of the base quantity and strength. The analysis was performed by using an acid-base titration method and FTIR spectroscopy with CHCl3 as a probe molecule. It is proposed that glucose isomerization on the titanates depends not only on the base amount but also on the base strength.

DOI： 10.1002/cctc.201700068

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

Combination catalyst systems composed of Pt/SiO2 and lanthanoid oxides (Pt/SiO2 + LOx) efficiently catalyze the hydrogenative ring-rearrangement of 5-(hydroxymethyl) furfural (HMF) in water to produce 3-(hydroxymethyl) cyclopentanol (HCPO), which can be a unique building block for new materials derived from biomass. We investigated the reason for the efficient hydrogenative ring-rearrangement on Pt/SiO2 + LOx in terms of the acid-base properties of reaction systems, since H+ and Lewis acids can affect the rearrangement of the furan ring. It is indicated that the ring-rearrangement efficiently proceeds under slightly acidic conditions (pH = 5-7) with moderate or a little weak Lewis acidity of lanthanoid oxides.

DOI： 10.1039/c7cy00712d

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

Recently, it has been reported that the morphology of Au nanoparticles (NPs) affects the catalytic activity of CO oxidation; twin crystal NPs show higher activity for CO oxidation than single-crystal NPs. In this study, density functional calculations have been carried out to investigate the morphology effect of Au NPs using CO as a probe molecule. In the case of Au NPs with a size of more than 2 nm, CO adsorption energy on the Au NPs is mainly determined by a coordination number (CN) of adsorption sites. CO binding to a multiple twin NP with a size of about 1 nm is stronger than that on a single-crystal NP with the same size. A simple CN explanation cannot be applied to the enhancement of CO binding to the small multiple twin NP. This enhancement is related to a deformation of the NP structure before and after CO adsorption. It is suggested that the multiple twin NP with a size of less than 1 nm, which shows the deformation upon CO adsorption, contributes to the higher activity for CO oxidation.

DOI： 10.3390/catal7060191

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

Pd/CoAl2O4/Al2O3 methane combustion catalysts were synthesized using a galvanic deposition (GD) method (PdCoAl-GD). This PdCoAl-GD catalyst showed higher activities and turnover frequencies (TOFs) than conventional Pd/Al2O3. According to X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) and scanning transmission electron microscopy (STEM) measurements, PdCoAl-GD was composed of a CoAl2O4 phase supported on gamma-Al2O3 and dispersed Pd nanoparticles of 2-7 nm in size on CoAl2O4. Operando Pd K-edge XAFS measurements indicated that the Pd in PdCoAl-GD was oxidized to highly active methane combustion PdO species at low temperatures. PdCoAl-GD also showed high activity (light-off tests) when PdO was initially present on the catalysts. Methane temperature-programmed reaction (CH4-TPR) measurements on PdCoAl-GD revealed that PdO was reduced by CH4 at low temperatures. The GD method used herein achieved PdO species that were effective for C-H activation.

DOI： 10.1039/c7ra06150a

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Chemistry Letters  

We studied the dynamic redox behavior of Cu species in zeolite matrix under NH3-SCR using in situ XAFS. Cu2+ species were slowly reduced to Cu+ in flowing NH3, and subsequent addition of NO promoted the reduction to Cu+. In the oxidation step, oxygen alone did not fully oxidize Cu+ to Cu2+, but the Cu+ species were completely oxidized to Cu2+ by NOO2. The oxidation step was slower than the reduction step, which suggested that the oxidation step (Cu+ ¼ Cu2+) is the slow step of the NH3-SCR reaction.

DOI： 10.1246/cl.170451

Scopus

Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：Catalysis Science and Technology  

Combination catalyst systems composed of Pt/SiO2 and lanthanoid oxides (Pt/SiO2 + LOx) efficiently catalyze the hydrogenative ring-rearrangement of 5-(hydroxymethyl)furfural (HMF) in water to produce 3-(hydroxymethyl)cyclopentanol (HCPO), which can be a unique building block for new materials derived from biomass. We investigated the reason for the efficient hydrogenative ring-rearrangement on Pt/SiO2 + LOx in terms of the acid-base properties of reaction systems, since H+ and Lewis acids can affect the rearrangement of the furan ring. It is indicated that the ring-rearrangement efficiently proceeds under slightly acidic conditions (pH = 5-7) with moderate or a little weak Lewis acidity of lanthanoid oxides.

DOI： 10.1039/c7cy00712d

Scopus

Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：COMODIA 2017 - 9th International Conference on Modeling and Diagnostics for Advanved Engine Systems  

DPF (Diesel Particulate Filter) is effective for trapping diesel soot from diesel engines. The trapped diesel soot is removed by combustion above 600°C using excess fuels, which results in reduction of fuel economy. An effective design of DPF is strongly required to improve DPF regeneration efficiency and fuel economy; however, the internal phenomenon of diesel soot combustion on DPF is still not clarified. For an effective design of DPF, in this study, we investigated the effect of diesel soot structure on combustion temperature using real diesel soot. Soot samples were characterized by means of various physicochemical techniques: XPS (X-ray photoelectron spectroscopy), EELS (Electron Energy Loss Spectroscopy), Raman spectroscopy, TEM (transmission electron microscopy), and elemental analysis. TEM images and Raman spectra of real diesel soot showed that the difference in the crystallinity of soot was small. XPS, EELS, and elemental analysis revealed that oxygen content, which is derived from surface functional groups of - COOH, -OH, and - C=O at defect sites, was strongly affected by the engine operating conditions. The ignition temperature of diesel soot was dependent on O/C ratio measured by elemental analysis. With the increase in oxygen content of diesel soot, combustion temperatures of soot became lower. It was concluded that the concentration of oxygen containing functional groups is an essential factor for the control of the ignition temperature of diesel soot.

Scopus

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DOI： DOI: 10.1039/C6TA05517F

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DOI： DOI: 10.1039/c6cy00795c

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DOI： doi.org/10.1246/bcsj.20160102

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DOI： 10.1016/j.cattod.2014.05.046

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DOI： 10.1093/jmicro/dfu001

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DOI： dx.doi.org/10.1021/cs4001267

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DOI： DOI: 10.1039/c3cy00033h

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DOI： DOI: 10.1016/j.apcatb.2012.12.025

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DOI： 10.1016/j.cattod.2012.03.048

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DOI： DOI: 10.1039/C2RA22190J

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DOI： 10.1627/jpi.54.347

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DOI： 10.1002/cctc.201100171

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DOI： 10.1039/C1GC15835J

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DOI： 10.1039/C1RA00560J

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DOI： 10.1039/C0CY00077A

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The mechanistic cause of the dramatic activity improvement of alumina-supported silver (Ag/Al2O3)byH2 addition for the selective catalytic reduction of NO with propane (C3H8-SCR) was investigated by catalytic and spectroscopic studies. In situ UV-vis, in situ EXAFS, IR, and microcalorimetric experiments show that
H2 reduction of Ag+ ions on Ag/Al2O3 at 573 K yields protons on alumina and partially reduced Agn clusters, which are subsequently aggregated to larger Ag clusters. During H2 + O2 and H2-assisted C3H8-SCR reactions, Ag+ ions and Agn .+ coexist. Reoxidation with O2 results in the redispersion of the cluster to Ag+ ion, accompanying a reaction of protons. The relationship between cluster size, redox properties, and catalytic activity is examined using Ag/Al2O3 of different Ag loadings. The steady-state NO reduction rate correlates fairly well with the amount of Agn .+ during the H2-assisted C3H8-SCR reaction. It is shown that Agn .+ is the active species, whereas monomeric Ag+ ion and metallic Ag particles are inactive. With Ag loading, the Ag+ reduction rate increases and the rate of cluster reoxidation decreases. A balance between the rate of reduction and reoxidation of Ag species is an important factor that controls the size and oxidation state of the Ag species and consequently the catalytic activity of Ag/Al2O3. ESR has provided evidence, for the first time, for the in situ generation of superoxide ions in H2 + O2 and H2-assisted C3H8-SCR reactions. The comprehensive reason for the hydrogen effect in HC-SCR is discussed, focusing on the role of the cluster and protons on the reductive O2 activation to superoxide ion.

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Selective catalytic reduction of NO by hydrocarbons (HC-SCR) is one of the promising technologies for removal of NO in exhausts containing excess oxygen, such as diesel and lean burn gasoline engines. Supported Ag catalysts, especially Ag/Al2O3, are thought to be the promising candidates for use in diesel exhausts, as con.rmed by several reports on engine bench tests. The HC-SCR performance of supported Ag catalysts is very sensitive to the reaction conditions, especially the type of hydrocarbons and the addition of H2. The control of reaction conditions would be key for practical use. The current research of supported Ag catalysts is reviewed from the viewpoints of practical use and the reaction mechanism, i.e., the reaction scheme, the role of surface adsorbed species, and the structure of active Ag species.

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Involvement of active sites in the selective oxidation of propane was investigated using (VO)2P2O7 catalysts promoted by Sb, Ti, Zr, Hf, Cu, and Ce. Based on X-ray diffraction patterns, infrared spectra, and Raman spectra, the formation of a (VO)2P2O7 phase was con.rmed for all of the promoted catalysts; no other phases were detected. After the addition of Sb, Ti, and Zr, the selectivity to acrylic acid increased, whereas Cu-, Ce-, and Hf-promoted catalysts showed lower selectivity than pure (VO)2P2O7. The effect of promoters on the activity and selectivity for the propane oxidation was investigated on the basis of the nature of surface active sites. The surface V=O species, evaluated by the nitric oxide.ammonia rectangular pulse technique, decreased with the addition of the promoters. A proportional correlation between the number of surface V=O species and reaction rate of propane clari.ed that the surface V=O species is the controlling factor for the catalytic activity of propane oxidation. In the case of Sb-, Ti-, and Zr-promoted catalysts, the selectivity to acrylic acid increased signi.cantly. The selectivity was compared with the number and strength of Bronsted and Lewis acid sites estimated from dimethylpyridine temperature-programmed desorption. A good correlation was observed between the selectivity to acrylic acid and the surface concentration of Lewis acid sites. It was experimentally demonstrated that Lewis acid sites represent the key factor in selective oxidation.

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Silver-alumina catalysts prepared by sol.gel method (Ag-Al2O3) and impregnation method (Ag/Al2O3) were studied for the selective catalytic reduction (SCR) of NO by higher alkanes (n-hexane and n-octane). UV.VIS and Ag K-edge XAFS results established the structure of the catalysts; below 2 wt.%, highly dispersed Ag+ ions are predominant Ag species, while at higher Ag loading, Agn clusters are predominant. A relationship between the structure of Ag species and their catalytic function for SCR by n-octane was clari.ed. Ag+ ions are responsible for the selective reduction of NO to N2, while the Agn clusters are responsible for the hydrocarbon combustion and N2O formation. The mechanism of SCR by n-hexane on Ag-Al2O3, which mainly consists of Ag+ ions, were investigated by in situ FTIR spectroscopy. During NO + n-hexane + O2 reaction, the acetate produced via the partial oxidation of n-hexane and the nitrates produced via the oxidation of NO were main adspecies in the steady-state condition at 473.623 K. The acetate, which was stable in O2 or NO, was reactive in NO+O2. Nitrates, which were relatively stable in n-hexane, were quite reactive toward n-hexane+O2. The rate of nitrates reaction in n-hexane+O2 was close to the steady-state rate of NO reduction over wide range of temperature, indicating that the nitrate is a possible intermediate in the SCR. A proposed mechanism, suggesting the reaction of nitrates with partially oxidized hydrocarbon species as a crucial step, explains the steady-state kinetic results. At relatively high NO concentration or at low temperature, nitrates should inhibit the reaction by strongly adsorbing on the catalyst surface.

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Total pages：12   Responsible for pages：75-86   Language：Japanese Book type：Scholarly book

一昨年に報道された排気ガス規制偽装の報道は記憶に新しいかと思われますが、ディーゼルエンジンの需要は新興国市場で伸び、また日本でも従来のイメージから脱却し、燃料代が安く、熱の効率が良いディーゼルエンジンがあらためて注目されています。欧米では日本と事情は異なりますがそれぞれ独自の需要と市場を形成しています。しかしながら各市場・規制が要求するレベルで排出ガスをクリーンにすることが最大の課題となっております。そこで弊社では排出ガス浄化技術においてキーマテリアルである触媒およびそのシステムの開発、要素技術に焦点をあてた書籍を発刊します。

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DOI： doi:10.20731/zeoraito.24.2.60

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DOI： doi:10.20731/zeoraito.18.2.58

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Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：Wiley Blackwell  

We report herein the first general catalytic system for the direct synthesis of N-substituted γ- and δ-lactams by reductive amination/cyclization of keto acids (including levulinic acid) with nitriles and H2 under mild conditions (7 bar H2, 110 °C, solvent free). The most effective catalyst, Pt and MoOx co-loaded TiO2 (Pt-MoOx/TiO2), shows a wide substrate scope, high turnover number (TON), and good reusability.

DOI： 10.1002/cctc.201701355

Scopus

J-GLOBAL

J-GLOBAL

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)  

DOI： 10.1007/978-981-10-5137-1_5

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/, -Al2O3 with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/-Al2O3 increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al2O3 for methane combustion.

DOI： 10.1002/anie.201709124

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/, -Al2O3 with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/-Al2O3 increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al2O3 for methane combustion.

DOI： 10.1002/anie.201709124

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

The particle size effect of Pd nanoparticles supported on alumina with various crystalline phases on methane combustion was investigated. Pd/, -Al2O3 with weak metal-support interaction showed a volcano-shaped dependence of the catalytic activity on the size of Pd particles, and the catalytic activity of the strongly interacted Pd/-Al2O3 increased with the particle size. Based on a structural analysis of Pd nanoparticles using CO adsorption IR spectroscopy and spherical aberration-corrected scanning/transmission electron microscopy, the dependence of catalytic activity on Pd particle size and the alumina crystalline phase was due to the fraction of step sites on Pd particle surface. The difference in fraction of the step site is derived from the particle shape, which varies not only with Pd particle size but also with the strength of metal-support interaction. Therefore, this interaction perturbs the particle size effect of Pd/Al2O3 for methane combustion.

DOI： 10.1002/anie.201709124

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：CHEMICAL SOC JAPAN  

We studied the dynamic redox behavior of Cu species in zeolite matrix under NH3-SCR using in situ XAFS. Cu2+ species were slowly reduced to Cu+ in flowing NH3, and subsequent addition of NO promoted the reduction to Cu+. In the oxidation step, oxygen alone did not fully oxidize Cu+ to Cu2+, but the Cu+ species were completely oxidized to Cu2+ by NO-O-2. The oxidation step was slower than the reduction step, which suggested that the oxidation step (Cu+ -> Cu2+) is the slow step of the NH3-SCR reaction.

DOI： 10.1246/cl.170451

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：CHEMICAL SOC JAPAN  

We studied the dynamic redox behavior of Cu species in zeolite matrix under NH3-SCR using in situ XAFS. Cu2+ species were slowly reduced to Cu+ in flowing NH3, and subsequent addition of NO promoted the reduction to Cu+. In the oxidation step, oxygen alone did not fully oxidize Cu+ to Cu2+, but the Cu+ species were completely oxidized to Cu2+ by NO-O-2. The oxidation step was slower than the reduction step, which suggested that the oxidation step (Cu+ -> Cu2+) is the slow step of the NH3-SCR reaction.

DOI： 10.1246/cl.170451

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：American Chemical Society  

To elucidate the reaction mechanism of NO-C3H6-CO-O2 over NiFe2O4, we investigated the dynamics of the adsorbed and gaseous species during the reaction using operando Fourier transform infrared (FTIR). The NO reduction activity dependent on the C3H6 and CO concentrations suggested that NO is reduced by C3H6 under three-way catalytic conditions. From FTIR measurements and kinetic analysis, it was clarified that the acetate species reacted with NO-O2 to form N2 via NCO, and that the rate-limiting step of NO reduction was the reaction between CH3COO- and NO-O2. The NO reduction mechanism of the three-way catalyst on NiFe2O4 is different to that on platinum-group metal catalysts, on which NO reduction proceeds through N-O cleavage.

DOI： 10.1021/acsomega.7b00165

Scopus

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：American Chemical Society  

To elucidate the reaction mechanism of NO-C3H6-CO-O2 over NiFe2O4, we investigated the dynamics of the adsorbed and gaseous species during the reaction using operando Fourier transform infrared (FTIR). The NO reduction activity dependent on the C3H6 and CO concentrations suggested that NO is reduced by C3H6 under three-way catalytic conditions. From FTIR measurements and kinetic analysis, it was clarified that the acetate species reacted with NO-O2 to form N2 via NCO, and that the rate-limiting step of NO reduction was the reaction between CH3COO- and NO-O2. The NO reduction mechanism of the three-way catalyst on NiFe2O4 is different to that on platinum-group metal catalysts, on which NO reduction proceeds through N-O cleavage.

DOI： 10.1021/acsomega.7b00165

Scopus

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：American Chemical Society  

To elucidate the reaction mechanism of NO-C3H6-CO-O2 over NiFe2O4, we investigated the dynamics of the adsorbed and gaseous species during the reaction using operando Fourier transform infrared (FTIR). The NO reduction activity dependent on the C3H6 and CO concentrations suggested that NO is reduced by C3H6 under three-way catalytic conditions. From FTIR measurements and kinetic analysis, it was clarified that the acetate species reacted with NO-O2 to form N2 via NCO, and that the rate-limiting step of NO reduction was the reaction between CH3COO- and NO-O2. The NO reduction mechanism of the three-way catalyst on NiFe2O4 is different to that on platinum-group metal catalysts, on which NO reduction proceeds through N-O cleavage.

DOI： 10.1021/acsomega.7b00165

Scopus

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Glucose isomerization was performed using various titanate catalysts, which include SrTiO3, BaTiO3, CaTiO3, Na2Ti6O13, K2Ti6O13, and Sr3Ti2O7, prepared using a conventional solid-phase method. Among the titanates, SrTiO3, CaTiO3, and Na2Ti6O13 offered a relatively high fructose yield (32%) with a high selectivity (68-78%). The yields are comparable to yields reported previously using a Sn-modified BEA zeolite, which shows a high efficiency for glucose isomerization as a Lewis acid catalyst. A study of the mechanism of glucose isomerization on a SrTiO3 catalyst surface by using H-1 NMR spectroscopy suggested that the titanates catalyze the isomerization as base catalysts. Thus, the effect of the basicity of the titanates on glucose isomerization was investigated in terms of the base quantity and strength. The analysis was performed by using an acid-base titration method and FTIR spectroscopy with CHCl3 as a probe molecule. It is proposed that glucose isomerization on the titanates depends not only on the base amount but also on the base strength.

DOI： 10.1002/cctc.201700068

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Combination catalyst systems composed of Pt/SiO2 and lanthanoid oxides (Pt/SiO2 + LOx) efficiently catalyze the hydrogenative ring-rearrangement of 5-(hydroxymethyl) furfural (HMF) in water to produce 3-(hydroxymethyl) cyclopentanol (HCPO), which can be a unique building block for new materials derived from biomass. We investigated the reason for the efficient hydrogenative ring-rearrangement on Pt/SiO2 + LOx in terms of the acid-base properties of reaction systems, since H+ and Lewis acids can affect the rearrangement of the furan ring. It is indicated that the ring-rearrangement efficiently proceeds under slightly acidic conditions (pH = 5-7) with moderate or a little weak Lewis acidity of lanthanoid oxides.

DOI： 10.1039/c7cy00712d

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Glucose isomerization was performed using various titanate catalysts, which include SrTiO3, BaTiO3, CaTiO3, Na2Ti6O13, K2Ti6O13, and Sr3Ti2O7, prepared using a conventional solid-phase method. Among the titanates, SrTiO3, CaTiO3, and Na2Ti6O13 offered a relatively high fructose yield (32%) with a high selectivity (68-78%). The yields are comparable to yields reported previously using a Sn-modified BEA zeolite, which shows a high efficiency for glucose isomerization as a Lewis acid catalyst. A study of the mechanism of glucose isomerization on a SrTiO3 catalyst surface by using H-1 NMR spectroscopy suggested that the titanates catalyze the isomerization as base catalysts. Thus, the effect of the basicity of the titanates on glucose isomerization was investigated in terms of the base quantity and strength. The analysis was performed by using an acid-base titration method and FTIR spectroscopy with CHCl3 as a probe molecule. It is proposed that glucose isomerization on the titanates depends not only on the base amount but also on the base strength.

DOI： 10.1002/cctc.201700068

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：WILEY-V C H VERLAG GMBH  

Glucose isomerization was performed using various titanate catalysts, which include SrTiO3, BaTiO3, CaTiO3, Na2Ti6O13, K2Ti6O13, and Sr3Ti2O7, prepared using a conventional solid-phase method. Among the titanates, SrTiO3, CaTiO3, and Na2Ti6O13 offered a relatively high fructose yield (32%) with a high selectivity (68-78%). The yields are comparable to yields reported previously using a Sn-modified BEA zeolite, which shows a high efficiency for glucose isomerization as a Lewis acid catalyst. A study of the mechanism of glucose isomerization on a SrTiO3 catalyst surface by using H-1 NMR spectroscopy suggested that the titanates catalyze the isomerization as base catalysts. Thus, the effect of the basicity of the titanates on glucose isomerization was investigated in terms of the base quantity and strength. The analysis was performed by using an acid-base titration method and FTIR spectroscopy with CHCl3 as a probe molecule. It is proposed that glucose isomerization on the titanates depends not only on the base amount but also on the base strength.

DOI： 10.1002/cctc.201700068

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：MDPI AG  

Recently, it has been reported that the morphology of Au nanoparticles (NPs) affects the catalytic activity of CO oxidation; twin crystal NPs show higher activity for CO oxidation than single-crystal NPs. In this study, density functional calculations have been carried out to investigate the morphology effect of Au NPs using CO as a probe molecule. In the case of Au NPs with a size of more than 2 nm, CO adsorption energy on the Au NPs is mainly determined by a coordination number (CN) of adsorption sites. CO binding to a multiple twin NP with a size of about 1 nm is stronger than that on a single-crystal NP with the same size. A simple CN explanation cannot be applied to the enhancement of CO binding to the small multiple twin NP. This enhancement is related to a deformation of the NP structure before and after CO adsorption. It is suggested that the multiple twin NP with a size of less than 1 nm, which shows the deformation upon CO adsorption, contributes to the higher activity for CO oxidation.

DOI： 10.3390/catal7060191

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：MDPI AG  

Recently, it has been reported that the morphology of Au nanoparticles (NPs) affects the catalytic activity of CO oxidation; twin crystal NPs show higher activity for CO oxidation than single-crystal NPs. In this study, density functional calculations have been carried out to investigate the morphology effect of Au NPs using CO as a probe molecule. In the case of Au NPs with a size of more than 2 nm, CO adsorption energy on the Au NPs is mainly determined by a coordination number (CN) of adsorption sites. CO binding to a multiple twin NP with a size of about 1 nm is stronger than that on a single-crystal NP with the same size. A simple CN explanation cannot be applied to the enhancement of CO binding to the small multiple twin NP. This enhancement is related to a deformation of the NP structure before and after CO adsorption. It is suggested that the multiple twin NP with a size of less than 1 nm, which shows the deformation upon CO adsorption, contributes to the higher activity for CO oxidation.

DOI： 10.3390/catal7060191

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：MDPI AG  

Recently, it has been reported that the morphology of Au nanoparticles (NPs) affects the catalytic activity of CO oxidation; twin crystal NPs show higher activity for CO oxidation than single-crystal NPs. In this study, density functional calculations have been carried out to investigate the morphology effect of Au NPs using CO as a probe molecule. In the case of Au NPs with a size of more than 2 nm, CO adsorption energy on the Au NPs is mainly determined by a coordination number (CN) of adsorption sites. CO binding to a multiple twin NP with a size of about 1 nm is stronger than that on a single-crystal NP with the same size. A simple CN explanation cannot be applied to the enhancement of CO binding to the small multiple twin NP. This enhancement is related to a deformation of the NP structure before and after CO adsorption. It is suggested that the multiple twin NP with a size of less than 1 nm, which shows the deformation upon CO adsorption, contributes to the higher activity for CO oxidation.

DOI： 10.3390/catal7060191

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Pd/CoAl2O4/Al2O3 methane combustion catalysts were synthesized using a galvanic deposition (GD) method (PdCoAl-GD). This PdCoAl-GD catalyst showed higher activities and turnover frequencies (TOFs) than conventional Pd/Al2O3. According to X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) and scanning transmission electron microscopy (STEM) measurements, PdCoAl-GD was composed of a CoAl2O4 phase supported on gamma-Al2O3 and dispersed Pd nanoparticles of 2-7 nm in size on CoAl2O4. Operando Pd K-edge XAFS measurements indicated that the Pd in PdCoAl-GD was oxidized to highly active methane combustion PdO species at low temperatures. PdCoAl-GD also showed high activity (light-off tests) when PdO was initially present on the catalysts. Methane temperature-programmed reaction (CH4-TPR) measurements on PdCoAl-GD revealed that PdO was reduced by CH4 at low temperatures. The GD method used herein achieved PdO species that were effective for C-H activation.

DOI： 10.1039/c7ra06150a

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Pd/CoAl2O4/Al2O3 methane combustion catalysts were synthesized using a galvanic deposition (GD) method (PdCoAl-GD). This PdCoAl-GD catalyst showed higher activities and turnover frequencies (TOFs) than conventional Pd/Al2O3. According to X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) and scanning transmission electron microscopy (STEM) measurements, PdCoAl-GD was composed of a CoAl2O4 phase supported on gamma-Al2O3 and dispersed Pd nanoparticles of 2-7 nm in size on CoAl2O4. Operando Pd K-edge XAFS measurements indicated that the Pd in PdCoAl-GD was oxidized to highly active methane combustion PdO species at low temperatures. PdCoAl-GD also showed high activity (light-off tests) when PdO was initially present on the catalysts. Methane temperature-programmed reaction (CH4-TPR) measurements on PdCoAl-GD revealed that PdO was reduced by CH4 at low temperatures. The GD method used herein achieved PdO species that were effective for C-H activation.

DOI： 10.1039/c7ra06150a

Web of Science

Language：English   Publishing type：Rapid communication, short report, research note, etc. (scientific journal)   Publisher：ROYAL SOC CHEMISTRY  

Pd/CoAl2O4/Al2O3 methane combustion catalysts were synthesized using a galvanic deposition (GD) method (PdCoAl-GD). This PdCoAl-GD catalyst showed higher activities and turnover frequencies (TOFs) than conventional Pd/Al2O3. According to X-ray diffraction (XRD), X-ray absorption fine structure (XAFS) and scanning transmission electron microscopy (STEM) measurements, PdCoAl-GD was composed of a CoAl2O4 phase supported on gamma-Al2O3 and dispersed Pd nanoparticles of 2-7 nm in size on CoAl2O4. Operando Pd K-edge XAFS measurements indicated that the Pd in PdCoAl-GD was oxidized to highly active methane combustion PdO species at low temperatures. PdCoAl-GD also showed high activity (light-off tests) when PdO was initially present on the catalysts. Methane temperature-programmed reaction (CH4-TPR) measurements on PdCoAl-GD revealed that PdO was reduced by CH4 at low temperatures. The GD method used herein achieved PdO species that were effective for C-H activation.

DOI： 10.1039/c7ra06150a

Web of Science

Event date： 2021.3

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自動車の燃費向上に伴って、排気ガスの平均温度が低下し、触媒の低温領域での活性向上が求められている。本講演では、Galvanic Deposition法による卑金属とのバイメタル化と担体の修飾により低温領域での触媒燃焼活性を向上させた例を紹介する。

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