Atomic-Scale Mechanism of Platinum Catalyst Restructuring under a Pressure of Reactant Gas. Sumaria, V., Nguyen, L., Tao, F. F., & Sautet, P. Journal of the American Chemical Society, 145(1):392–401, January, 2023. ![Atomic-Scale Mechanism of Platinum Catalyst Restructuring under a Pressure of Reactant Gas [link]](https://bibbase.org/img/filetypes/link.svg "link")
Paper doi abstract bibtex Heterogeneous catalysis is key for chemical transformations. Understanding how catalysts’ active sites dynamically evolve at the atomic scale under reaction conditions is a prerequisite for accurately determining catalytic mechanisms and predictably developing catalysts. We combine in situ time-dependent scanning tunneling microscopy observations and machine-learning-accelerated first-principles atomistic simulations to uncover the mechanism of restructuring of Pt catalysts under a pressure of carbon monoxide (CO). We show that a high CO coverage at a Pt step edge triggers the formation of atomic protrusions of low-coordination Pt atoms, which then detach from the step edge to create sub-nano-islands on the terraces, where under-coordinated sites are stabilized by the CO adsorbates. The fast and accurate machine-learning potential is key to enabling the exploration of tens of thousands of configurations for the CO-covered restructuring catalyst. These studies open an avenue to achieve an atomic-scale understanding of the structural dynamics of more complex metal nanoparticle catalysts under reaction conditions.
@article{sumaria_atomic-scale_2023,
title = {Atomic-{Scale} {Mechanism} of {Platinum} {Catalyst} {Restructuring} under a {Pressure} of {Reactant} {Gas}},
volume = {145},
issn = {0002-7863},
url = {https://doi.org/10.1021/jacs.2c10179},
doi = {10.1021/jacs.2c10179},
abstract = {Heterogeneous catalysis is key for chemical transformations. Understanding how catalysts’ active sites dynamically evolve at the atomic scale under reaction conditions is a prerequisite for accurately determining catalytic mechanisms and predictably developing catalysts. We combine in situ time-dependent scanning tunneling microscopy observations and machine-learning-accelerated first-principles atomistic simulations to uncover the mechanism of restructuring of Pt catalysts under a pressure of carbon monoxide (CO). We show that a high CO coverage at a Pt step edge triggers the formation of atomic protrusions of low-coordination Pt atoms, which then detach from the step edge to create sub-nano-islands on the terraces, where under-coordinated sites are stabilized by the CO adsorbates. The fast and accurate machine-learning potential is key to enabling the exploration of tens of thousands of configurations for the CO-covered restructuring catalyst. These studies open an avenue to achieve an atomic-scale understanding of the structural dynamics of more complex metal nanoparticle catalysts under reaction conditions.},
number = {1},
urldate = {2023-03-01},
journal = {Journal of the American Chemical Society},
author = {Sumaria, Vaidish and Nguyen, Luan and Tao, Franklin Feng and Sautet, Philippe},
month = jan,
year = {2023},
keywords = {0},
pages = {392--401},
}
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