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

Wenyao Chen, Junbo Cao, Jia Yang, Yueqiang Cao, Hao Zhang, Zheng Jiang, Jing Zhang, Gang Qian, Xinggui Zhou, Chen De (), Weikang Yuan and Xuezhi Duan ()
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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
Zheng Jiang: 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
Chen De: Norwegian University of Science and Technology
Weikang Yuan: East China University of Science and Technology
Xuezhi Duan: East China University of Science and Technology

Nature Communications, 2021, vol. 12, issue 1, 1-11

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-27238-z

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