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Surface chemistry dictates stability and oxidation state of supported single metal catalyst atoms

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Abstract

Single atom catalysts receive considerable attention due to reducing noble metal utilization and potentially eliminating certain side reactions. Yet, the rational design of highly reactive and stable single atom catalysts is hampered by the current lack of fundamental insights at the single atom limit. Here, density functional theory calculations are performed for a prototype reaction, namely CO oxidation, over different single metal atoms supported on alumina. The governing reaction mechanisms and scaling relations are identified using microkinetic modeling and principal component analysis, respectively. A large change in the oxophilicity of the supported single metal atom leads to changes in the rate-determining step and the catalyst resting state. Multi-response surfaces are introduced and built cheaply using a descriptor-based, closed form kinetic model to describe simultaneously the activity, stability, and oxidation state of single metal atom catalysts. A double peaked volcano in activity is observed due to competing rate-determining steps and catalytic cycles. Reaction orders of reactants provide excellent kinetic signatures of the catalyst state. Importantly, the surface chemistry determines the stability, oxidation, and resting state of the catalyst.

Graphical abstract: Surface chemistry dictates stability and oxidation state of supported single metal catalyst atoms

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Supplementary files

Article information


Submitted
23 Nov 2019
Accepted
30 Dec 2019
First published
02 Jan 2020

This article is Open Access
All publication charges for this article have been paid for by the Royal Society of Chemistry

Chem. Sci., 2020, Advance Article
Article type
Edge Article

Surface chemistry dictates stability and oxidation state of supported single metal catalyst atoms

K. Alexopoulos and D. G. Vlachos, Chem. Sci., 2020, Advance Article , DOI: 10.1039/C9SC05944J

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