We performed extensive first-principles-based calculations to highlight the reaction mechanisms of CO oxidation Au1/h-BN in reaction conditions. A reaction network was constructed firstly based on calculated first-principles thermodynamics data on newly proposed variants of Langmuir–Hinshelwood type pathways, as well as all other previously proposed potential reaction mechanisms. Then, microkinetics simulations were performed to highlight the performance of Au1/h-BN, together with the mechanisms that have major contribution to CO conversion. Langmuir–Hinshelwood type pathways and with their variants are found the dominant pathways for CO conversion. Specifically, conventional revised Langmuir–Hinshelwood pathway is the dominant pathway at high temperatures where CO mediated activation of O2 and thermodriven dissociation of cyclic intermediates are favored, while coadsorbed reaction species mediated dissociation of peroxide intermediate is the preferred pathway at low temperatures with high CO partial pressure. The findings highlight the vital role of reaction condition dependent thermostability of reaction species in determining the reaction mechanism of CO conversion over single atom catalysts (SACs) and may help to rationalize the current understanding to superior catalytic performance of SACs.

Reaction network for CO oxidation on Au1/h-BN: A first-principles investigation

ACS Fall 2021

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