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Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site

Author

Listed:
  • Yan Tang

    (Tsinghua University
    University of California, Los Angeles
    University of California, Los Angeles
    University of California, Los Angeles)

  • Chithra Asokan

    (University of California, Santa Barbara)

  • Mingjie Xu

    (University of California Irvine)

  • George W. Graham

    (University of California Irvine
    University of Michigan)

  • Xiaoqing Pan

    (University of California Irvine
    University of California Irvine
    University of California Irvine)

  • Phillip Christopher

    (University of California, Santa Barbara)

  • Jun Li

    (Tsinghua University
    Southern University of Science and Technology)

  • Philippe Sautet

    (University of California, Los Angeles
    University of California, Los Angeles
    University of California, Los Angeles)

Abstract

Single-atom catalysts are widely investigated heterogeneous catalysts; however, the identification of the local environment of single atoms under experimental conditions, as well as operando characterization of their structural changes during catalytic reactions are still challenging. Here, the preferred local coordination of Rh single atoms is investigated on TiO2 during calcination in O2, reduction in H2, CO adsorption, and reverse water gas shift (RWGS) reaction conditions. Theoretical and experimental studies clearly demonstrate that Rh single atoms adapt their local coordination and reactivity in response to various redox conditions. Single-atom catalysts hence do not have static local coordinations, but can switch from inactive to active structure under reaction conditions, hence explaining some conflicting literature accounts. The combination of approaches also elucidates the structure of the catalytic active site during reverse water gas shift. This insight on the real nature of the active site is key for the design of high-performance catalysts.

Suggested Citation

  • Yan Tang & Chithra Asokan & Mingjie Xu & George W. Graham & Xiaoqing Pan & Phillip Christopher & Jun Li & Philippe Sautet, 2019. "Rh single atoms on TiO2 dynamically respond to reaction conditions by adapting their site," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-12461-6
    DOI: 10.1038/s41467-019-12461-6
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    Cited by:

    1. Marti Checa & Addis S. Fuhr & Changhyo Sun & Rama Vasudevan & Maxim Ziatdinov & Ilia Ivanov & Seok Joon Yun & Kai Xiao & Alp Sehirlioglu & Yunseok Kim & Pankaj Sharma & Kyle P. Kelley & Neus Domingo &, 2023. "High-speed mapping of surface charge dynamics using sparse scanning Kelvin probe force microscopy," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Zheng Chen & Zhangyun Liu & Xin Xu, 2023. "Dynamic evolution of the active center driven by hemilabile coordination in Cu/CeO2 single-atom catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Lina Zhang & Shaolong Wan & Congcong Du & Qiang Wan & Hien Pham & Jiafei Zhao & Xingyu Ding & Diye Wei & Wei Zhao & Jiwei Li & Yanping Zheng & Hui Xie & Hua Zhang & Mingshu Chen & Kelvin H. L. Zhang &, 2024. "Generating active metal/oxide reverse interfaces through coordinated migration of single atoms," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    4. Bin Shao & Zhi-Qiang Wang & Xue-Qing Gong & Honglai Liu & Feng Qian & P. Hu & Jun Hu, 2023. "Synergistic promotions between CO2 capture and in-situ conversion on Ni-CaO composite catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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