Density functional theory calculations are performed for CO oxidation over single metal atoms supported on alumina. Both doped and adsorbed single atoms are considered as structural motifs of the highly-dispersed alumina-supported catalyst. Multiple catalytic cycles are considered on adsorbed single atoms, including carbonate-mediated and self-promoted CO oxidation, while a Mars van Krevelen mechanism is assumed on doped single atoms. Exact, first-principles microkinetic modeling is used to quantify the effect of reaction conditions and the rate-determining step(s) along with the most important reaction intermediates. Simulations provide insights into the active site, the dominant mechanism, and the oxidation state of the catalyst. Contrary to the common belief, we clearly show that under kinetically relevant conditions, the state of the catalyst may not be described by ab initio thermodynamics. The dominant catalytic cycle for CO oxidation on these active sites changes with metal and the activity, stability, and oxidation state show a complex nonlinear behavior.

Operando spectroscopy, kinetics, and stability of single atom catalysts for CO oxidation

Macromolecular Chemistry: The Second Century

[Author Benefits](https://scimeetings.acs.org/?utm_source=pubs_content_marketing&utm_medium=website&utm_campaign=0320_MCF_NPI_Launch_Spring_Homepage&ref=pubs_content_marketing)

[How to use SciMeetings](https://storage.googleapis.com/dl.morressier.com/acs/SciMeetings-ACSSpring2020-HowToGuide_M3020-Final.pdf)

[Frequently Asked Questions](https://storage.googleapis.com/dl.morressier.com/acs/SciMtng_ACSNMSp2020_FAQ_M3120_Final.pdf)

ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.