Dynamic Behavior of Rh Species of Rh/Al2O3 Model Catalyst During Three-Way Catalytic Reaction – An Operando XAS Study,Journal of the American Chemical Society

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Dynamic Behavior of Rh Species of Rh/Al2O3 Model Catalyst During Three-Way Catalytic Reaction – An Operando XAS Study
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2017-12-26 , DOI: 10.1021/jacs.7b07114
Hiroyuki Asakura _{1,

2} , Saburo Hosokawa _{1,

2} , Toshiaki Ina ₃ , Kazuo Kato ₃ , Kiyofumi Nitta ₃ , Kei Uera ₃ , Tomoya Uruga _{3,

4} , Hiroki Miura _{1,

5,

6} , Tetsuya Shishido _{1,

5,

6} , Junya Ohyama _{1,

7} , Atsushi Satsuma _{1,

7} , Katsutoshi Sato _{1,

8} , Akira Yamamoto _{1,

9} , Satoshi Hinokuma _{1,

10} , Hiroshi Yoshida _{1,

10} , Masato Machida _{1,

10} , Seiji Yamazoe _{1,

11} , Tatsuya Tsukuda _{1,

11} , Kentaro Teramura _{1,

2} , Tsunehiro Tanaka _{1,

2}

Affiliation

Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan
Department of Molecular Engineering, Graduate School of Engineering, Kyoto University, Kyotodaigaku Katsura, Nishikyo-ku, Kyoto 615-8510, Japan
Japan Synchrotron Radiation Research Institute, SPring-8, Sayo, Hyogo 679-5198, Japan
Innovation Research Center for Fuel Cells, The University of Electro-Communications, 1-5-1 Chofugaoka, Chofu, Tokyo 182-8585, Japan
Department of Applied Chemistry, Graduate School of Urban Environmental Sciences, Tokyo Metropolitan University, 1-1 Minami-Osawa, Hachioji, Tokyo 192-0397, Japan
Research Center for Hydrogen Energy-Based Society, Tokyo Metropolitan University, 1-1 Minami-Osawa, Hachioji, Tokyo 192-0397, Japan
Graduate School of Engineering and Institute of Materials and Systems for Sustainability, Nagoya University, Nagoya 464-8603, Japan
Department of Integrated Science and Technology, Faculty of Science and Engineering, Oita University, 700 Dannoharu, Oita 870-1192, Japan
Graduate School of Human and Environmental Studies, Kyoto University, Kyoto 606-8501, Japan
Department of Applied Chemistry and Biochemistry, Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto 860-8555, Japan
Department of Chemistry, School of Science, University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan

The dynamic behavior of Rh species in 1 wt% Rh/Al2O3 catalyst during the three-way catalytic reaction was examined using a micro gas chromatograph, a NOx meter, a quadrupole mass spectrometer, and time-resolved quick X-ray absorption spectroscopy (XAS) measurements at a public beamline for XAS, BL01B1 at SPring-8, operando. The combined data suggest different surface rearrangement behavior, random reduction processes, and autocatalytic oxidation processes of Rh species when the gas is switched from a reductive to an oxidative atmosphere and vice versa. This study demonstrates an implementation of a powerful operando XAS system for heterogeneous catalytic reactions and its importance for understanding the dynamic behavior of active metal species of catalysts.

中文翻译：

Rh/Al2O3 模型催化剂在三元催化反应过程中 Rh 物种的动态行为 - Operando XAS 研究

使用微型气相色谱仪、NOx 计、四极杆质谱仪和时间分辨快速 X 射线吸收光谱 (XAS) 检测了三元催化反应过程中 Rh 物种在 1 wt% Rh/Al2O3 催化剂中的动态行为) 在公共光束线上进行的 XAS 测量，BL01B1 在 SPring-8，operando。综合数据表明，当气体从还原气氛切换到氧化气氛时，Rh 物质的表面重排行为、随机还原过程和自催化氧化过程不同，反之亦然。本研究展示了用于多相催化反应的强大操作 XAS 系统的实施及其对理解催化剂活性金属物种动态行为的重要性。

更新日期：2017-12-26

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