Faculty Profiles - NAGAOKA Katsutoshi

Papers - NAGAOKA Katsutoshi

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Realization of Ideal Ba Promoter State by Simultaneous Incorporation with Co into Carbon‐protective Framework for Ammonia Synthesis Catalyst Reviewed

K. Kanishka, H. De Silva, Katsutoshi Sato, Takahiro Naito, Takaaki Toriyama, Tomokazu Yamamoto, Ryotaro Aso, Yasukazu Murakami, Pradeep R. Varadwaj, Ryoji Asahi, Koji Inazu, Katsutoshi Nagaoka

Advanced Energy Materials Vol. 15 ( 8 ) 2024.12

Efficient metallic Ni as a bifunctional electrocatalyst for integrating continuous PET plastic upcycling with hydrogen production Reviewed International coauthorship

Xin Li, Jiyi Sun, Huijing Ma, Xia Long, Tianqi Li, Yuto Shimoyama, Takahiro Naito, Katsutoshi Sato, Hiroshi Yamada, Katsutoshi Nagaoka, Yixin Zhao, Xufang Qian

Applied Catalysis B: Environment and Energy Vol. 371 2025.8

Atomic behaviors in PdRu solid-solution nanoparticles on CeO2-ZrO2 support for the three-way catalytic reaction Reviewed Open Access

Okkyun Seo, Akhil Tayal, Jaemyung Kim, Kohei Kusada, Tomokazu Yamamoto, Jiayi Tang, Satoshi Hiroi, Chulho Song, Katsutoshi Sato, Katsutoshi Nagaoka, Masaaki Haneda, Kazuo Kato, Syo Matsumura, Hiroshi Kitagawa, Osami Sakata

Materials Today Catalysis Vol. 7 page： 100078 - 100078 2024.12

Significant low-temperature activity of tetragonal type ZrO2-supported Ru catalysts for CO2 methanation Reviewed

Katsutoshi Sato, Hitomi Higuchi, Katsutoshi Nagaoka

Chemistry Letters Vol. 53 ( 10 ) 2024.10

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

Abstract

Conversion of CO2 with H2 to CH4 is a potential route for the utilization of CO2. Because CO2 methanation is an exothermic reaction, the equilibrium yield decreases with increasing temperature. A catalyst that exhibits high activity at low temperatures is thus highly desirable. We report here that a tetragonal-type ZrO2 supported Ru catalyst prepared by low-temperature calcination showed significant low-temperature activity for CO2 methanation. We surmise that an intermediate formate species formed over the tetragonal-type ZrO2 and enhanced the catalytic activity.

DOI： 10.1093/chemle/upae178

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Rapid start-up of carbon-free H2 production by ammonia oxidative decomposition over Co/Ce0.5Zr0.5O2 with microwave irradiation Reviewed Open Access

Takahiro Matsunaga, Sachika Hayashi, Hiroshi Yamada, Katsutoshi Sato, Katsutoshi Nagaoka

iScience Vol. 27 ( 8 ) page： 110452 - 110452 2024.8

Barium-doped Iron Nanoparticles supported on MgO as an Efficient Catalyst for Ammonia Synthesis under Mild Reaction Conditions Reviewed Open Access

Kohei Era, Katsutoshi Sato, Shin-ichiro Miyahara, Takahiro Naito, Kanishka De Silva, Saeid Akrami, Hiroshi Yamada, Takaaki Toriyama, Takehiro Tamaoka, Tomokazu Yamamoto, Yasukazu Murakami, Koji Inazu, Katsutoshi Nagaoka

Sustainable Energy and Fuels Vol. 8 ( 12 ) page： 2593 - 2600 2024.5

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

To realize a carbon-neutral society, developing highly active and inexpensive catalysts for ammonia (NH3) production working at moderate conditions (<400 °C, <10 MPa) using hydrogen fabricated from the electrolysis of...

DOI： 10.1039/d4se00411f

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Effects of the Topological Structure of Different Cu-Zeolites on the Relationship between Soot and NOx Removal on NH3–SCRF Reviewed

Zhimu Ye, Pengcheng Zhao, Xincheng Tang, Takeshi Hagio, Katsutoshi Sato, Katsutoshi Nagaoka, Xinling Li

Energy & Fuels Vol. 38 page： 2212 - 2223 2024.1

Catalytic Behavior of K‐doped Fe/MgO Catalysts for Ammonia Synthesis Under Mild Reaction Conditions Reviewed Open Access

Kohei Era, Katsutoshi Sato, Shin‐ichiro Miyahara, Takahiro Naito, Kanishka De Silva, Saeid Akrami, Hiroshi Yamada, Takaaki Toriyama, Tomokazu Yamamoto, Yasukazu Murakami, Ken‐ichi Aika, Koji Inazu, Katsutoshi Nagaoka

ChemSusChem Vol. 16 ( 22 ) page： e202300942 2023.11

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

Abstract

An important part of realizing a carbon‐neutral society using ammonia will be the development of an inexpensive yet efficient catalyst for ammonia synthesis under mild reaction conditions (<400 °C, <10 MPa). Here, we report Fe/K(3)/MgO, fabricated via an impregnation method, as a highly active catalyst for ammonia synthesis under mild reaction conditions (350 °C, 1.0 MPa). At the mentioned conditions, the activity of Fe/K(3)/MgO (17.5 mmol h−1 gcat−1) was greater than that of a commercial fused iron catalyst (8.6 mmol h−1 gcat−1) currently used in the Haber‐Bosch process. K doping was found to increase the ratio of Fe0 on the surface and turnover frequency of Fe in our Fe/K(3)/MgO catalyst. In addition, increasing the pressure to 3.0 MPa at the same temperature led to a significant improvement of the ammonia synthesis rate to 29.6 mmol h−1 gcat−1, which was higher than that of two more expensive, benchmark Ru‐based catalysts, which are also potential alternative catalysts. A kinetics analysis revealed that the addition of K enhanced the ammonia synthesis activity at ≥300 °C by changing the main adsorbed species from NH to N which can accelerate dissociative adsorption of nitrogen as the rate limiting step in ammonia synthesis.

DOI： 10.1002/cssc.202300942

The Effect of Ru Precursor and Support on the Hydrogenation of Aromatic Aldehydes/Ketones to Alcohols Reviewed Open Access

Chandan Chaudhari, Katsutoshi Sato, Shin-ichiro Miyahara, Tomokazu Yamamoto, Takaaki Toriyama, Syo Matsumura, Kohei Kusuda, Hiroshi Kitagawa, Katsutoshi Nagaoka

CHEMCATCHEM Vol. 14 ( 16 ) 2022.8

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

Supported Ru catalysts were prepared by using different Ru precursors and examined for the hydrogenation of benzaldehyde to CHM. The catalyst prepared from Ru-3(CO)(12) precursor and HT support exhibited high yield of CHM. Moderate acidic and basic nature of HT was favourable to control the selectivity for CHM. The physicochemical properties analysis revealed that highly dispersed Ru nanoparticles were effective for the hydrogenation of benzaldehyde. Ru-CO/HT catalyst was tolerant to different functional groups and was stable until 7(th) cycle of recycle study.

DOI： 10.1002/cctc.202200241

Co Nanoparticle Catalysts Encapsulated by BaO–La2O3 Nanofractions for Efficient Ammonia Synthesis Under Mild Reaction Conditions Reviewed Open Access

Shin-ichiro Miyahara, Katsutoshi Sato, Kotoko Tsujimaru, Yuichiro Wada, Yuta Ogura, Takaaki Toriyama, Tomokazu Yamamoto, Syo Matsumura, Koji Inazu, Katsutoshi Nagaoka

ACS Omega Vol. 7 ( 28 ) page： 24452 - 24460 2022.7

Operando Spectroscopic Study of the Dynamics of Ru Catalyst during Preferential Oxidation of CO and the Prevention of Ammonia Poisoning by Pt Reviewed Open Access

Katsutoshi Sato, Shuhei Zaitsu, Godai Kitayama, Sho Yagi, Yuto Kayada, Yoshihide Nishida, Yuichiro Wada, Katsutoshi Nagaoka

JACS Au Vol. 2 ( 7 ) page： 1627 - 1637 2022.5

Direct high-purity hydrogen production from ammonia by using a membrane reactor combining V-10mol%Fe hydrogen permeable alloy membrane with Ru/Cs<inf>2</inf>O/Pr<inf>6</inf>O<inf>11</inf> ammonia decomposition catalyst Reviewed Open Access

Kaori Omata, Katsutoshi Sato, Katsutoshi Nagaoka, Hiroshi Yukawa, Yoshihisa Matsumoto, Tomonori Nambu

International Journal of Hydrogen Energy Vol. 47 ( 13 ) page： 8372 - 8381 2022.2

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

The hydrogen production capabilities of the membrane reactor combining V-10 mol%Fe hydrogen permeable alloy membrane with Ru/Cs2O/Pr6O11 ammonia decomposition catalyst are studied. The ammonia conversion is improved by 1.7 times compared to the Ru/Cs2O/Pr6O11 catalyst alone by removing the produced hydrogen through the V-10mol%Fe alloy membrane during the ammonia decomposition. 79% of the hydrogen atoms contained in the ammonia gas are extracted directly as high-purity hydrogen gas. Both the Ru/Cs2O/Pr6O11 catalyst and the V-10 mol% Fe alloy membrane are highly durable, and the initial performance of the hydrogen separation rate lasts for more than 3000 h. The produced hydrogen gas conforms to ISO 14687–2:2019 Grade D for fuel cell vehicles because the ammonia and nitrogen concentrations are less than 0.1 ppm and 100 ppm, respectively.

DOI： 10.1016/j.ijhydene.2021.12.191

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Rh-PVP Catalyzed Reductive Amination of Phenols by Ammonia or Amines to Cyclohexylamines under Solvent-free Conditions Reviewed Open Access

Chandan Chaudhari, Katsutoshi Sato, Saeki Rumi, Yoshihide Nishida, Masaya Shiraishi, Katsutoshi Nagaoka

Chemistry Letters Vol. 51 ( 1 ) page： 81 - 84 2022.1

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

Colloidal metal nanoparticles were examined for reductive amination of phenol by ammonia under mild reaction conditions. The results showed that Rh-PVP was the most active catalyst for reductive amination reaction. Linear, cyclic, and amino alcohols were used as nucleophiles and converted to primary/secondary/tertiary amines. Using this strategy, the synthesis of an industrially important chemical, N-cyclohexyl- 2-pyrrolidone was explored.

DOI： 10.1246/cl.210574

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Nitrile hydrogenation to secondary amines under ambient conditions over palladium-platinum random alloy nanoparticles Reviewed Open Access

Yoshihide Nishida, Katsutoshi Sato, Chandan Chaudhari, Hiroshi Yamada, Takaaki Toriyama, Tomokazu Yamamoto, Syo Matsumura, Susan Meñez Aspera, Hiroshi Nakanishi, Masaaki Haneda, Katsutoshi Nagaoka

Catalysis Science and Technology Vol. 12 ( 13 ) page： 4128 - 4137 2022

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

Catalytic hydrogenation of nitriles is a cost-effective and green method for synthesizing amines and imines, which have many industrial applications. However, this reaction generally requires harsh reaction conditions and produces a mixture of amine and imine products due to its chemodiversity. Therefore, it is a challenge to selectively hydrogenate nitriles to a single product under ambient conditions (1 bar of H2 at 25 °C). Here, we report an effective method for selective hydrogenation of nitriles that does not require heat, pressurization, or long reaction times. We achieved this by means of bimetalization between palladium (Pd) and platinum (Pt) nanoparticles, which resulted in a catalyst that showed high yield of secondary amines. Although Pd and Pt are thermodynamically immiscible, we have successfully alloyed the two metals by means of rapid chemical reduction assisted by microwave heating. X-ray absorption spectroscopy suggested the formation of heteroatomic Pdδ+Ptδ− sites via charge transfer between neighboring Pd and Pt atoms in the alloy structure. Moreover, Fourier transform IR spectroscopy and scanning transmission electron microscopy-energy-dispersive X-ray spectroscopy indicated that decreasing the size of the PdPt (50 : 50) nanoparticles improved the degree of alloying and facilitated the formation of electron-enriched Ptδ− species. On the basis of kinetics studies and density functional theory calculations, we concluded that cyano group activation, which was the rate-determining step over monometallic Pd and Pt catalysts, was accelerated over the heteroatomic Pdδ+Ptδ− sites because of strong back-donation from electron-enriched Ptδ− species to the carbon atom of the cyano groups. The PdPt random alloy nanoparticles catalyzed the reactions of various aromatic and heterocyclic nitriles, and the corresponding secondary amines were selectively obtained in just a few hours.

DOI： 10.1039/d1cy02302k

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Co/Ba/La2O3 catalyst for ammonia synthesis under mild reaction conditions Reviewed

Katsutoshi Nagaoka, Shin-ichiro Miyahara, Katsutoshi Sato, Yuta Ogura, Kotoko Tsujimaru, Yuichiro Wada, Takaaki Toriyama, Tomokazu Yamamoto, Syo Matsumura, Koji Inazu

2021.12

Barium oxide encapsulating cobalt nanoparticles supported on magnesium oxide: Active non-noble metal catalysts for ammonia synthesis under mild reaction conditions Reviewed Open Access

Katsutoshi Sato, Katsutoshi Nagaoka, Shin Ichiro Miyahara, Kotoko Tsujimaru, Yuichiro Wada, Takaaki Toriyama, Tomokazu Yamamoto, Syo Matsumura, Koji Inazu, Hirono Mohri, Takeshi Iwasa, Tetsuya Taketsugu

ACS Catalysis Vol. 11 ( 21 ) page： 13050 - 13061 2021.11

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

To realize a carbon-free society, catalysts are needed for the synthesis of ammonia under mild reaction conditions (<400 °C, <10 MPa) that use hydrogen produced from renewable energy. Ru-based catalysts are currently the most promising candidates; however, Ru is expensive and of low abundance. Here, we discovered that the encapsulation of Co nanoparticles with BaO enhanced the ammonia synthesis activity of Co and that a simple Ba-doped Co/MgO catalyst prereduced at an unusually high temperature of 700 °C (Co@BaO/MgO-700red) showed outstanding ammonia synthesis activity. The ammonia synthesis rate (24.6 mmol gcat−1 h−1) and turnover frequency (0.246 s−1) of the catalyst at 350 °C and 1.0 MPa were about 80 and 250 times higher, respectively, than those of the nondoped parent catalyst. At the same temperature but higher pressure (3.0 MPa), the ammonia synthesis rate was increased to 48.4 mmol gcat−1 h−1, which is higher than that of active Ru-based catalysts. In addition, at 1.0 MPa, our catalyst produced ammonia even at temperatures as low as 150 °C. Scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy investigations revealed that after reduction at 700 °C, the Co nanoparticles had become encapsulated by a nanofraction of BaO. The mechanism underlying the formation of this unique structure was considered to comprise reduction of oxidic Co to metallic Co, decomposition of BaCO3 to BaO, and migration of BaO and Co nanoparticles. Spectroscopic and density functional theory investigations revealed that adsorption of N2 on the Co atoms at the catalyst surface weakened the N2 triple bond to the strength of a double bond due to electron donation from Ba2+ of BaO via adjacent Co atoms; this weakening accelerated the cleavage of the triple bond, which is the rate-determining step for ammonia synthesis.

DOI： 10.1021/acscatal.1c02887

Ammonia synthesis over lanthanoid oxide–supported ruthenium catalysts Reviewed Open Access

Shin ichiro Miyahara, Katsutoshi Sato, Yukiko Kawano, Kazuya Imamura, Yuta Ogura, Kotoko Tsujimaru, Katsutoshi Nagaoka

Catalysis Today Vol. 376 page： 36 - 40 2021.9

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

Ammonia synthesis catalysts with high activity under mild reaction conditions for use in synthetic chemical processes powered by renewable energy are needed. Here, we investigated the physicochemical properties and ammonia synthesis activity of lanthanoid oxide–supported Ru catalysts. The basicity of the Ru/lanthanoid oxide catalysts, as estimated by CO2 temperature-programmed desorption, was higher than that of Ru/MgO, a representative catalyst with high ammonia synthesis activity, and a positive relationship was observed between basicity and turnover frequency. The turnover frequency of Ru/Pr2O3 and Ru/La2O3 (both 0.24 s−1) was eight times that of Ru/MgO (0.03 s−1). A kinetic analysis revealed that hydrogen poisoning, which is a typical drawback of oxide-supported Ru catalysts, was markedly retarded in the Ru/lanthanoid oxide catalysts. As a result, the ammonia synthesis rate of the Ru/Pr2O3 catalyst increased with increasing reaction pressure, reaching 49 mmol g−1 h−1 at 400 °C and 1.0 MPa, which was 12 times that of Ru/MgO under the same conditions.

DOI： 10.1016/j.cattod.2020.08.031

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One-pot synthesis of cyclohexylamine and: N -aryl pyrroles via hydrogenation of nitroarenes over the Pd<inf>0.5</inf>Ru<inf>0.5</inf>-PVP catalyst Reviewed

Chandan Chaudhari, Katsutoshi Sato, Yasuyuki Ikeda, Kenji Terada, Naoya Abe, Katsutoshi Nagaoka

New Journal of Chemistry Vol. 45 ( 22 ) page： 9743 - 9746 2021.6

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

The direct synthesis of cyclohexylamine via the hydrogenation of nitrobenzene over monometallic (Pd, Ru or Rh) and bimetallic (PdxRu1-x) catalysts was studied. The Pd0.5Ru0.5-PVP catalyst was the most effective catalyst for this reaction. The catalyst can be reused and applied for the synthesis of N-aryl pyrroles and quinoxalines from nitrobenzenes.

DOI： 10.1039/d1nj00922b

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Highly Stable and Active Solid-Solution-Alloy Three-Way Catalyst by Utilizing Configurational-Entropy Effect Reviewed

Kohei Kusada, Dongshuang Wu, Yusuke Nanba, Michihisa Koyama, Tomokazu Yamamoto, Xuan Quy Tran, Takaaki Toriyama, Syo Matsumura, Ayano Ito, Katsutoshi Sato, Katsutoshi Nagaoka, Okkyun Seo, Chulho Song, Yanna Chen, Natalia Palina, Loku Singgappulige Rosantha Kumara, Satoshi Hiroi, Osami Sakata, Shogo Kawaguchi, Yoshiki Kubota, Hiroshi Kitagawa

Advanced Materials Vol. 33 ( 16 ) page： e2005206 2021.4

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

Since 1970, people have been making every endeavor to reduce toxic emissions from automobiles. After the development of a three-way catalyst (TWC) that concurrently converts three harmful gases, carbon monoxide (CO), hydrocarbons (HCs), and nitrogen oxides (NOx), Rh became an essential element in automobile technology because only Rh works efficiently for catalytic NOx reduction. However, due to the sharp price spike in 2007, numerous efforts have been made to replace Rh in TWCs. Nevertheless, Rh remains irreplaceable, and now, the price of Rh is increasing significantly again. Here, it is demonstrated that PdRuM ternary solid-solution alloy nanoparticles (NPs) exhibit highly durable and active TWC performance, which will result in a significant reduction in catalyst cost compared to Rh. This work provides insights into the design of highly durable and efficient functional alloy NPs, guiding how to best take advantage of the configurational entropy in addition to the mixing enthalpy.

DOI： 10.1002/adma.202005206

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Boosting ammonia synthesis under mild reaction conditions by precise control of the basic oxideru interface

Katsutoshi Sato, Katsutoshi Nagaoka

Chemistry Letters Vol. 50 ( 4 ) page： 687 - 696 2021.4

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

Strong basic oxidesupported Ru catalysts are easily prepared and handled, and they have been used as effective catalysts for ammonia synthesis under mild reaction conditions since the 1970s. Recent research has revealed that precise control of the boundary states between the basic oxide (i.e., rare-earth oxide, alkali earth oxide), oxygen defect sites, and Ru nanoparticles can be used to enhance ammonia synthesis under mild reaction conditions and inhibit hydrogen poisoning, which is a typical drawback of strong basic oxidesupported Ru catalysts.

DOI： 10.1246/CL.200855

DOI： 10.1246/cl.200855

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Papers - NAGAOKA Katsutoshi