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Peer-reviewedCC BY 4.0Angewandte Chemie (International Ed. in English)

Vacuum‐Induced Surface Reconstruction of Mn–Ce Oxides for Low‐Temperature Coupled Redox Catalysis

  • Yong Yin1,2,3
  • Yide Jiang1
  • Zichen Xu1
  • Min Liu4,5
  • Emiliano Cortés6
  • Yifei Sun1,2
6 affiliations
  1. 1Key Laboratory of Agro‐Forestry Environmental Processes and Ecological Regulation of Hainan Province School of Environmental Science and Engineering Hainan University Haikou China
  2. 2Hainan International One Health Institute Hainan University Haikou Hainan China
  3. 3Hainan Province Key Laboratory of One Health Hainan University Haikou Hainan China
  4. 4Hunan Joint International Research Center For Carbon Dioxide Resource Utilization School of Physics Central South University Changsha Hunan China
  5. 5School of Metallurgy and Environment Central South University Changsha Hunan China
  6. 6Nanoinstitute Munich Faculty of Physics Ludwig‐Maximilians‐Universität München München Germany
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Abstract

Low‐temperature redox catalysis over mixed oxides is typically optimized by tuning bulk composition, yet the decisive chemistry occurs at the surface and subsurface interface. Here, we show that this interface can be deliberately reconstructed to enhance Mn–Ce oxide catalysis. Sequential vacuum annealing followed by reduced‐pressure O2 treatment induces near‐surface Mn enrichment in an as‐prepared Mn–Ce oxide while largely preserving the fluorite CeO2 framework. This reconstruction increases the near‐surface abundance of Mn‐containing species, modifies the Mn–Ce–O interfacial electronic and redox environment, and facilitates oxygen activation and redox cycling. Under coupled conditions, R‐MnCe achieved 95.5% NO x conversion at 100°C and complete chlorobenzene conversion at 200°C. In situ spectroscopy and DFT calculations reveal that interfacial electron redistribution lowers the oxygen activation barrier and sustains activated oxygen species that connect NH3‐SCR and chlorobenzene oxidation through a shared oxygen‐mediated pathway. These results highlight near‐surface reconstruction as a promising postsynthetic strategy for improving noble‐metal‐free mixed‐oxide catalysts.

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Cite

BibTeXRIS
BibTeX
@article{yin2026vacuuminduced,
  title = {{Vacuum‐Induced Surface Reconstruction of Mn–Ce Oxides for Low‐Temperature Coupled Redox Catalysis}},
  author = {Yong Yin and Yide Jiang and Zichen Xu and Min Liu and Emiliano Cortés and Yifei Sun},
  journal = {Angewandte Chemie (International Ed. in English)},
  year = {2026},
  month = sep,
  doi = {10.1002/anie.2739215},
  url = {https://doi.org/10.1002/anie.2739215},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Vacuum‐Induced Surface Reconstruction of Mn–Ce Oxides for Low‐Temperature Coupled Redox Catalysis
AU  - Yong Yin
AU  - Yide Jiang
AU  - Zichen Xu
AU  - Min Liu
AU  - Emiliano Cortés
AU  - Yifei Sun
PY  - 2026
DA  - 2026/09/21
JO  - Angewandte Chemie (International Ed. in English)
DO  - 10.1002/anie.2739215
UR  - https://doi.org/10.1002/anie.2739215
AB  - Low‐temperature redox catalysis over mixed oxides is typically optimized by tuning bulk composition, yet the decisive chemistry occurs at the surface and subsurface interface. Here, we show that this interface can be deliberately reconstructed to enhance Mn–Ce oxide catalysis. Sequential vacuum annealing followed by reduced‐pressure O2 treatment induces near‐surface Mn enrichment in an as‐prepared Mn–Ce oxide while largely preserving the fluorite CeO2 framework. This reconstruction increases the near‐surface abundance of Mn‐containing species, modifies the Mn–Ce–O interfacial electronic and redox environment, and facilitates oxygen activation and redox cycling. Under coupled conditions, R‐MnCe achieved 95.5% NO x conversion at 100°C and complete chlorobenzene conversion at 200°C. In situ spectroscopy and DFT calculations reveal that interfacial electron redistribution lowers the oxygen activation barrier and sustains activated oxygen species that connect NH3‐SCR and chlorobenzene oxidation through a shared oxygen‐mediated pathway. These results highlight near‐surface reconstruction as a promising postsynthetic strategy for improving noble‐metal‐free mixed‐oxide catalysts.
SN  - 1433-7851
SN  - 1521-3773
ER  -