A1 Journal article (refereed)
The role of polaronic states in the enhancement of CO oxidation by single-atom Pt/CeO2 (2023)

Kauppinen, M. M., Daelman, N., López, N., & Honkala, K. (2023). The role of polaronic states in the enhancement of CO oxidation by single-atom Pt/CeO2. Journal of Catalysis, 423, Article 26-33. https://doi.org/10.1016/j.jcat.2023.04.014

JYU authors or editors

Kauppinen, Minttu
Honkala, Karoliina

Publication details

All authors or editors: Kauppinen, Minttu M.; Daelman, Nathan; López, Núria; Honkala, Karoliina

Journal or series: Journal of Catalysis

ISSN: 0021-9517

eISSN: 1090-2694

Publication year: 2023

Publication date: 28/03/2023

Volume: 423

Article number: 26-33

Publisher: Elsevier BV

Publication country: United States

Publication language: English

DOI: https://doi.org/10.1016/j.jcat.2023.04.014

Publication open access: Openly available

Publication channel open access: Partially open access channel

Publication is parallel published (JYX): https://jyx.jyu.fi/handle/123456789/86864

Web address of parallel published publication (pre-print): https://doi.org/10.26434/chemrxiv-2022-m0q59

Abstract

Single Atom Catalysts (SACs) have shown that the miniaturization of the active site implies new phenomena like dynamic charge transfer between isolated metal atoms and the oxide. To obtain direct proof of this character is challenging, as many experimental techniques provide averaged properties or have limitations with poorly conductive materials, leaving kinetic measurements from catalytic testing as the only reliable reference. Here we present an integrated Density Functional Theory-Microkinetic model including ground and metastable states to address the reactivity of Pt1/CeO2 for CO oxidation. Our results agree with experimentally available kinetic data in the literature and show that CO oxidation activity of Pt1/CeO2 is tunable via the electronic properties of the support. Particularly, samples with higher n-doping via oxygen depletion should be better in CO oxidation, as they help maintain the active state Pt0 of the catalyst. This provides an alternative strategy for tuning the performance of low-temperature oxidations in single-atom catalysts via charge transfer control.

Keywords: carbon monoxide; oxidation (active); catalysis; catalysts; platinum; density functional theory

Free keywords: single atom catalysts; CeO2; Pt; CO oxidation; density functional theory; microkinetic analysis; electronic ensemble; dynamic oxidation state

Fields of science: