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Integrated Experimental–Theoretical Approach To Determine Reliable Molecular Reaction Mechanisms on Transition-Metal Oxide Surfaces

Authors :
Yongping Zheng
Sean Dillon
Nickolas Ashburn
Kyeongjae Cho
Yves J. Chabal
Sampreetha Thampy
Julia W. P. Hsu
Source :
ACS Applied Materials & Interfaces. 11:30460-30469
Publication Year :
2019
Publisher :
American Chemical Society (ACS), 2019.

Abstract

By combining experimental and theoretical approaches, we investigate the quantitative relationship between molecular desorption temperature and binding energy on d and f metal oxide surfaces. We demonstrate how temperature-programmed desorption can be used to quantitatively correlate the theoretical surface chemistry of metal oxides (via on-site Hubbard U correction) to gas surface interactions for catalytic reactions. For this purpose, both CO and NO oxidation mechanisms are studied in a step-by-step reaction process for perovskite and mullite-type oxides, respectively. Additionally, we show solutions for over-binding issues found in COx, NOx, SOx, and other covalently bonded molecules that must be considered during surface reaction modeling. This work shows the high reliability of using TPD and density functional theory in conjunction to create accurate surface chemistry information for a variety of correlated metal oxide materials.

Details

ISSN :
19448252 and 19448244
Volume :
11
Database :
OpenAIRE
Journal :
ACS Applied Materials & Interfaces
Accession number :
edsair.doi.dedup.....d68a873a4a6f9550ceb2d21e5196051a
Full Text :
https://doi.org/10.1021/acsami.9b09700