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Here, we show that this interface can be deliberately reconstructed to enhance Mn\u2013Ce oxide catalysis. Sequential vacuum annealing followed by reduced\u2010pressure O\n                    <jats:sub>2<\/jats:sub>\n                    treatment induces near\u2010surface Mn enrichment in an as\u2010prepared Mn\u2013Ce oxide while largely preserving the fluorite CeO\n                    <jats:sub>2<\/jats:sub>\n                    framework. This reconstruction increases the near\u2010surface abundance of Mn\u2010containing species, modifies the Mn\u2013Ce\u2013O interfacial electronic and redox environment, and facilitates oxygen activation and redox cycling. Under coupled conditions, R\u2010MnCe achieved 95.5% NO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    conversion at 100\u00b0C and complete chlorobenzene conversion at 200\u00b0C. In situ spectroscopy and DFT calculations reveal that interfacial electron redistribution lowers the oxygen activation barrier and sustains activated oxygen species that connect NH\n                    <jats:sub>3<\/jats:sub>\n                    \u2010SCR and chlorobenzene oxidation through a shared oxygen\u2010mediated pathway. These results highlight near\u2010surface reconstruction as a promising postsynthetic strategy for improving noble\u2010metal\u2010free mixed\u2010oxide catalysts.\n                  <\/jats:p>","DOI":"10.1002\/anie.2739215","type":"journal-article","created":{"date-parts":[[2026,9,22]],"date-time":"2026-09-22T05:51:17Z","timestamp":1790056277000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Vacuum\u2010Induced Surface Reconstruction of Mn\u2013Ce Oxides for Low\u2010Temperature Coupled Redox Catalysis"],"prefix":"10.1002","author":[{"given":"Yong","family":"Yin","sequence":"first","affiliation":[{"name":"Key Laboratory of Agro\u2010Forestry Environmental Processes and Ecological Regulation of Hainan Province School of Environmental Science and Engineering Hainan University  Haikou China"},{"name":"Hainan International One Health Institute Hainan University  Haikou Hainan China"},{"name":"Hainan Province Key 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