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Exploring the dynamic evolution of lattice oxygen on exsolved-Mn2O3@SmMn2O5 interfaces for NO Oxidation

Wang, Xiyang; Yang, Qilei; Li, Xinbo; Li, Zhen; Gao, Chuan; Zhang, Hui; Chu, Xuefeng; Redshaw, Carl; Shi, Shucheng; Wu, Yimin A.; Ma, Yongliang; Peng, Yue; Li, Junhua; Feng, Shouhua

Authors

Xiyang Wang

Qilei Yang

Xinbo Li

Zhen Li

Chuan Gao

Hui Zhang

Xuefeng Chu

Profile image of Carl Redshaw

Professor Carl Redshaw C.Redshaw@hull.ac.uk
Professor of Inorganic Materials Chemistry and REF Lead for Chemistry

Shucheng Shi

Yimin A. Wu

Yongliang Ma

Yue Peng

Junhua Li

Shouhua Feng



Abstract

Lattice oxygen in metal oxides plays an important role in the reaction of diesel oxidation catalysts, but the atomic-level understanding of structural evolution during the catalytic process remains elusive. Here, we develop a Mn2O3/SmMn2O5 catalyst using a non-stoichiometric exsolution method to explore the roles of lattice oxygen in NO oxidation. The enhanced covalency of Mn–O bond and increased electron density at Mn3+ sites, induced by the interface between exsolved Mn2O3 and mullite, lead to the formation of highly active lattice oxygen adjacent to Mn3+ sites. Near-ambient pressure X-ray photoelectron and absorption spectroscopies show that the activated lattice oxygen enables reversible changes in Mn valence states and Mn-O bond covalency during redox cycles, reducing energy barriers for NO oxidation and promoting NO2 desorption via the cooperative Mars-van Krevelen mechanism. Therefore, the Mn2O3/SmMn2O5 exhibits higher NO oxidation activity and better resistance to hydrothermal aging compared to a commercial Pt/Al2O3 catalyst.

Citation

Wang, X., Yang, Q., Li, X., Li, Z., Gao, C., Zhang, H., Chu, X., Redshaw, C., Shi, S., Wu, Y. A., Ma, Y., Peng, Y., Li, J., & Feng, S. (2024). Exploring the dynamic evolution of lattice oxygen on exsolved-Mn2O3@SmMn2O5 interfaces for NO Oxidation. Nature communications, 15(1), Article 7613. https://doi.org/10.1038/s41467-024-51473-9

Journal Article Type Article
Acceptance Date Aug 8, 2024
Online Publication Date Sep 2, 2024
Publication Date Dec 1, 2024
Deposit Date Sep 6, 2024
Publicly Available Date Sep 9, 2024
Journal Nature Communications
Electronic ISSN 2041-1723
Publisher Nature Publishing Group
Peer Reviewed Peer Reviewed
Volume 15
Issue 1
Article Number 7613
DOI https://doi.org/10.1038/s41467-024-51473-9
Keywords Catalytic mechanisms; Nanoscale materials; Pollution remediation
Public URL https://hull-repository.worktribe.com/output/4796228

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https://creativecommons.org/licenses/by-nc-nd/4.0/

Copyright Statement
© The Author(s) 2024.
Open Access This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License, which permits any non-commercial use, sharing, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if you modified the licensed material. You do not have permission under this licence to share adapted material derived from this article or parts of it. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by-nc-nd/4.0/.




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