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In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation

Author

Listed:
  • Max J. Hülsey

    (National University of Singapore)

  • Bin Zhang

    (National University of Singapore)

  • Zhirui Ma

    (National University of Singapore)

  • Hiroyuki Asakura

    (Kyoto University
    Kyoto University)

  • David A. Do

    (Dalhousie University)

  • Wei Chen

    (National University of Singapore
    National University of Singapore)

  • Tsunehiro Tanaka

    (Kyoto University
    Kyoto University)

  • Peng Zhang

    (Dalhousie University)

  • Zili Wu

    (Oak Ridge National Laboratory)

  • Ning Yan

    (National University of Singapore)

Abstract

Single-atom catalysts have recently been applied in many applications such as CO oxidation. Experimental in situ investigations into this reaction, however, are limited. Hereby, we present a suite of operando/in situ spectroscopic experiments for structurally well-defined atomically dispersed Rh on phosphotungstic acid during CO oxidation. The identification of several key intermediates and the steady-state catalyst structure indicate that the reactions follow an unconventional Mars-van Krevelen mechanism and that the activation of O2 is rate-limiting. In situ XPS confirms the contribution of the heteropoly acid support while in situ DRIFT spectroscopy consolidates the oxidation state and CO adsorption of Rh. As such, direct observation of three key components, i.e., metal center, support and substrate, is achieved, providing a clearer picture on CO oxidation on atomically dispersed Rh sites. The obtained information are used to engineer structurally similar catalysts that exhibit T20 values up to 130 °C below the previously reported Rh1/NPTA.

Suggested Citation

  • Max J. Hülsey & Bin Zhang & Zhirui Ma & Hiroyuki Asakura & David A. Do & Wei Chen & Tsunehiro Tanaka & Peng Zhang & Zili Wu & Ning Yan, 2019. "In situ spectroscopy-guided engineering of rhodium single-atom catalysts for CO oxidation," Nature Communications, Nature, vol. 10(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09188-9
    DOI: 10.1038/s41467-019-09188-9
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    Cited by:

    1. Chengcheng Zhu & Li Xu & Yazi Liu & Jiang Liu & Jin Wang & Hanjun Sun & Ya-Qian Lan & Chen Wang, 2024. "Polyoxometalate-based plasmonic electron sponge membrane for nanofluidic osmotic energy conversion," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    2. Khandelwal, Akshat & Maarisetty, Dileep & Baral, Saroj Sundar, 2022. "Fundamentals and application of single-atom photocatalyst in sustainable energy and environmental applications," Renewable and Sustainable Energy Reviews, Elsevier, vol. 167(C).

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