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However, the stabilization of oxidation states to enable effective intermediate adsorption\u2013desorption behavior remains a critical challenge for enhancing formate yield. Herein, we synthesize a rigid\/soft layered oxides (CuInAlO\n                    <jats:sub>4<\/jats:sub>\n                    ) with rigid Al\u2013O framework and soft Cu\u2013O active units. Spin\u2010polarized electrons derived from the unpaired electrons in the dz\n                    <jats:sup>2<\/jats:sup>\n                    orbital of CuO\n                    <jats:sub>5<\/jats:sub>\n                    units transfer to the empty 5s\/5p orbitals of In\n                    <jats:sup>3<\/jats:sup>\n                    \u207a via the superexchange interaction of 3d(Cu)\u00a0\u2212\u00a02p(O)\u00a0\u2212\u00a05s\/5p(In). The enhanced spin polarization promotes spin\u2010orbit coupling between metal sites (Cu, In) and *OCHO intermediates (O), forming In\u2500*O\u2500CH\u2500O*\u2500Cu electronic bridge and greatly improving the formation efficiency of formate. CuInAlO\n                    <jats:sub>4<\/jats:sub>\n                    catalyst achieves exceptional formate selectivity (faradaic efficiency of 95% at 500\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    , energy efficiency of 80.3%, overpotential of 180\u00a0mV), outperforming conventional In\u2500O*\u2500CH\u2500O*\u2500In pathways by reducing the *OCHO\u2010to\u2010HCOOH energy barrier by 1.31\u00a0eV. Experimental and theoretical analyses reveal that the rigid AlO\n                    <jats:sub>5<\/jats:sub>\n                    units stabilize metal\u2010oxygen bonds, preventing oxygen dissolution, while accelerating formate production kinetics through spin\u2010polarized charge transfer.\n                  <\/jats:p>","DOI":"10.1002\/anie.202517481","type":"journal-article","created":{"date-parts":[[2025,12,17]],"date-time":"2025-12-17T08:51:23Z","timestamp":1765961483000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":8,"title":["Spin\u2010Polarization in Rigid\/Soft Layered Oxide Catalyst Regulates Key Intermediates for Efficient CO\n                    <sub>2<\/sub>\n                    \u2010to\u2010Formate Conversion"],"prefix":"10.1002","volume":"65","author":[{"given":"Yangyang","family":"Zhang","sequence":"first","affiliation":[{"name":"School of Materials Science and Engineering Anhui University  Hefei Anhui 230601 China"},{"name":"Hefei National Research Center for Physical Sciences at the Microscale Department of Materials Science and Engineering University of Science and Technology of China  Hefei Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4887-536X","authenticated-orcid":false,"given":"Genqiang","family":"Zhang","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale Department of Materials Science and Engineering University of Science and Technology of China  Hefei Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiangqiang","family":"Song","sequence":"additional","affiliation":[{"name":"School of Chemical Engineering Zhengzhou University  Zhengzhou 450001 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yanxu","family":"Chen","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale Department of Materials Science and Engineering University of Science and Technology of China  Hefei Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifan","family":"Li","sequence":"additional","affiliation":[{"name":"Hefei National Research Center for Physical Sciences at the Microscale Department of Materials Science and Engineering University of Science and Technology of China  Hefei Anhui 230026 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyao","family":"Yu","sequence":"additional","affiliation":[{"name":"School of Materials Science and Engineering Anhui University  Hefei Anhui 230601 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fuqiang","family":"Huang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Artificial Intelligent Creation Extreme Energy Materials Ministry of Education State Key Lab of Metal Matrix Composites 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