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Herein, we report a dual\u2010anion (C\/N) doped MnO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    (C\/N\u2013MnO\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    ) synthesized via a green, solvent\u2010free crystallization strategy, which exhibits excellent catalytic performance (95.3% benzyl alcohol conversion, &gt;99% benzonitrile selectivity) and broad substrate versatility (35 diverse alcohol substrates) under ambient conditions (25\u00b0C, 1 atm O\n                    <jats:sub>2<\/jats:sub>\n                    ) without external energy inputs. Structural analyses and theoretical calculations demonstrate that N\u2010doping introduces medium\u2010strong Lewis acidic Mn\u2013N sites to capture NH\n                    <jats:sub>3<\/jats:sub>\n                    , while C\u2010doping generates localized oxygen vacancies for O\n                    <jats:sub>2<\/jats:sub>\n                    activation. Crucially, kinetic isotope effect experiments and density functional theory (DFT) calculations prove that this anion dopant\u2010programmed relay catalysis successfully bypasses the MvK pathway, fundamentally shifting the rate\u2010determining step from initial alcohol dehydrogenation to the homolytic\n                    <jats:italic>\u03b1<\/jats:italic>\n                    \u2013C\u2013H bond scission of the aldimine intermediate. This work presents a paradigm shift in designing multifunctional non\u2010precious catalysts for ambient\u2010condition green organic transformations.\n                  <\/jats:p>","DOI":"10.1002\/anie.5879363","type":"journal-article","created":{"date-parts":[[2026,9,27]],"date-time":"2026-09-27T16:40:00Z","timestamp":1790527200000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Anion\u2010Doped Manganese Oxides Enabling Relay Catalysis for Aerobic Alcohol Ammoxidation"],"prefix":"10.1002","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-5256-6469","authenticated-orcid":false,"given":"Qingping","family":"Ke","sequence":"first","affiliation":[{"name":"School of Chemistry and Chemical Engineering Anhui University of Technology  Ma'anshan Anhui P. R. 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