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Molecular-level insights into the electronic effects in platinum-catalyzed carbon monoxide oxidation

Author

Listed:
  • Wenyao Chen

    (East China University of Science and Technology)

  • Junbo Cao

    (East China University of Science and Technology)

  • Jia Yang

    (Norwegian University of Science and Technology)

  • Yueqiang Cao

    (East China University of Science and Technology)

  • Hao Zhang

    (Soochow University
    Chinese Academy of Sciences)

  • Zheng Jiang

    (Chinese Academy of Sciences
    Chinese Academy of Sciences)

  • Jing Zhang

    (East China University of Science and Technology)

  • Gang Qian

    (East China University of Science and Technology)

  • Xinggui Zhou

    (East China University of Science and Technology)

  • De Chen

    (Norwegian University of Science and Technology)

  • Weikang Yuan

    (East China University of Science and Technology)

  • Xuezhi Duan

    (East China University of Science and Technology)

Abstract

A molecular-level understanding of how the electronic structure of metal center tunes the catalytic behaviors remains a grand challenge in heterogeneous catalysis. Herein, we report an unconventional kinetics strategy for bridging the microscopic metal electronic structure and the macroscopic steady-state rate for CO oxidation over Pt catalysts. X-ray absorption and photoelectron spectroscopy as well as electron paramagnetic resonance investigations unambiguously reveal the tunable Pt electronic structures with well-designed carbon support surface chemistry. Diminishing the electron density of Pt consolidates the CO-assisted O2 dissociation pathway via the O*-O-C*-O intermediate directly observed by isotopic labeling studies and rationalized by density-functional theory calculations. A combined steady-state isotopic transient kinetic and in situ electronic analyses identifies Pt charge as the kinetics indicators by being closely related to the frequency factor, site coverage, and activation energy. Further incorporation of catalyst structural parameters yields a novel model for quantifying the electronic effects and predicting the catalytic performance. These could serve as a benchmark of catalyst design by a comprehensive kinetics study at the molecular level.

Suggested Citation

  • Wenyao Chen & Junbo Cao & Jia Yang & Yueqiang Cao & Hao Zhang & Zheng Jiang & Jing Zhang & Gang Qian & Xinggui Zhou & De Chen & Weikang Yuan & Xuezhi Duan, 2021. "Molecular-level insights into the electronic effects in platinum-catalyzed carbon monoxide oxidation," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27238-z
    DOI: 10.1038/s41467-021-27238-z
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    References listed on IDEAS

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    1. Wenshuai Zhu & Zili Wu & Guo Shiou Foo & Xiang Gao & Mingxia Zhou & Bin Liu & Gabriel M. Veith & Peiwen Wu & Katie L. Browning & Ho Nyung Lee & Huaming Li & Sheng Dai & Huiyuan Zhu, 2017. "Taming interfacial electronic properties of platinum nanoparticles on vacancy-abundant boron nitride nanosheets for enhanced catalysis," Nature Communications, Nature, vol. 8(1), pages 1-7, August.
    2. Colleen Jackson & Graham T. Smith & David W. Inwood & Andrew S. Leach & Penny S. Whalley & Mauro Callisti & Tomas Polcar & Andrea E. Russell & Pieter Levecque & Denis Kramer, 2017. "Electronic metal-support interaction enhanced oxygen reduction activity and stability of boron carbide supported platinum," Nature Communications, Nature, vol. 8(1), pages 1-11, August.
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    Cited by:

    1. Tengfei Zhang & Peng Zheng & Jiajian Gao & Xiaolong Liu & Yongjun Ji & Junbo Tian & Yang Zou & Zhiyi Sun & Qiao Hu & Guokang Chen & Wenxing Chen & Xi Liu & Ziyi Zhong & Guangwen Xu & Tingyu Zhu & Fabi, 2024. "Simultaneously activating molecular oxygen and surface lattice oxygen on Pt/TiO2 for low-temperature CO oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

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