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Dynamic Behavior of Rh Species in Rh/Al_2O_3 Model Catalyst during Three-Way Catalytic Reaction: An Operando X-ray Absorption Spectroscopy Study

机译:Rh / Al_2O_3模型催化剂在三效催化过程中Rh物种的动态行为:操作X射线吸收光谱研究

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摘要

The dynamic behavior of Rh species in 1 wt% Rh/Al_(2)O_(3) catalyst during the three-way catalytic reaction was examined using a micro gas chromatograph, a NO_( x ) 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.
机译:使用微型气相色谱仪,NO_(x)仪,四极杆质谱仪和时间检查了1 wt%Rh / Al_(2)O_(3)催化剂在三元催化反应过程中Rh的动态行为-在SPring-8上操作XAS,BL01B1的公共光束线上的高分辨率X射线快速吸收光谱(XAS)测量。合并的数据表明,当气体从还原性气氛转换为氧化性气氛时,Rh物种的表面重排行为,随机还原过程和自催化氧化过程不同,反之亦然。这项研究证明了用于异相催化反应的功能强大的XAS系统的实现及其对理解催化剂活性金属物种动态行为的重要性。

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  • 来源
    《Journal of the American Chemical Society》 |2018年第1期|176-184|共9页
  • 作者单位

    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;

    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;

    Japan Synchrotron Radiation Research Institute, SPring-8, Sayo, Hyogo 679-5198, Japan;

    Japan Synchrotron Radiation Research Institute, SPring-8, Sayo, Hyogo 679-5198, Japan;

    Japan Synchrotron Radiation Research Institute, SPring-8, Sayo, Hyogo 679-5198, 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;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, 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;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, 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;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Graduate School of Engineering and Institute of Materials and Systems for Sustainability, Nagoya University, Nagoya 464-8603, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Graduate School of Engineering and Institute of Materials and Systems for Sustainability, Nagoya University, Nagoya 464-8603, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Integrated Science and Technology, Faculty of Science and Engineering, Oita University, 700 Dannoharu, Oita 870-1192, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Graduate School of Human and Environmental Studies, Kyoto University, Kyoto 606-8501, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Applied Chemistry and Biochemistry, Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto 860-8555, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Applied Chemistry and Biochemistry, Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto 860-8555, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Applied Chemistry and Biochemistry, Graduate School of Science and Technology, Kumamoto University, 2-39-1 Kurokami, Chuo, Kumamoto 860-8555, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Chemistry, School of Science, University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan;

    Elements Strategy Initiative for Catalysts & Batteries (ESICB), Kyoto University, 1-30 Goryo-Ohara, Nishikyo-ku, Kyoto 615-8245, Japan,Department of Chemistry, School of Science, University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-0033, Japan;

    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;

    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;

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  • 入库时间 2022-08-18 03:07:15

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