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

Author

Listed:
  • Xiyang Wang

    (Tsinghua University
    University of Waterloo)

  • Qilei Yang

    (Tsinghua University)

  • Xinbo Li

    (College of Chemistry, Jilin University)

  • Zhen Li

    (Tsinghua University)

  • Chuan Gao

    (Tsinghua University)

  • Hui Zhang

    (Chinese Academy of Sciences)

  • Xuefeng Chu

    (Tsinghua University)

  • Carl Redshaw

    (University of Hull)

  • Shucheng Shi

    (Shanghai Tech University)

  • Yimin A. Wu

    (University of Waterloo)

  • Yongliang Ma

    (Tsinghua University)

  • Yue Peng

    (Tsinghua University)

  • Junhua Li

    (Tsinghua University)

  • Shouhua Feng

    (College of Chemistry, Jilin University)

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.

Suggested Citation

  • Xiyang Wang & Qilei Yang & Xinbo Li & Zhen Li & Chuan Gao & Hui Zhang & Xuefeng Chu & Carl Redshaw & Shucheng Shi & Yimin A. Wu & Yongliang Ma & Yue Peng & Junhua Li & Shouhua Feng, 2024. "Exploring the dynamic evolution of lattice oxygen on exsolved-Mn2O3@SmMn2O5 interfaces for NO Oxidation," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51473-9
    DOI: 10.1038/s41467-024-51473-9
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    References listed on IDEAS

    as
    1. Son Hoang & Yanbing Guo & Andrew J. Binder & Wenxiang Tang & Sibo Wang & Jingyue (Jimmy) Liu & Huan Tran & Xingxu Lu & Yu Wang & Yong Ding & Eleni A. Kyriakidou & Ji Yang & Todd J. Toops & Thomas R. P, 2020. "Activating low-temperature diesel oxidation by single-atom Pt on TiO2 nanowire array," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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