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Herein, we devise a \u201cspin\u2010selective electron donation\u201d strategy to tune specific\n                    <jats:italic>d<\/jats:italic>\n                    orbital electrons of Pd inspired by the Dewar\u2212Chatt\u2212Duncanson model theory. Co\u2212S\u2212Pd bridges with different spin\u2010states of Co\n                    <jats:sup>III<\/jats:sup>\n                    have been constructed in a series of Pd\u2013PdS\n                    <jats:sub>2<\/jats:sub>\n                    \u2013Co\n                    <jats:sub>x<\/jats:sub>\n                    HNSs with tunable Co content. Experiments and theoretical calculations indicate that low\u2010spin Co\n                    <jats:sup>III<\/jats:sup>\n                    (t\n                    <jats:sub>2g<\/jats:sub>\n                    <jats:sup>6<\/jats:sup>\n                    e\n                    <jats:sub>g<\/jats:sub>\n                    <jats:sup>0<\/jats:sup>\n                    ) with fully occupied t\n                    <jats:sub>2g<\/jats:sub>\n                    orbitals and empty  orbitals can accurately alter the  electron of Pd by \u03c3\u2010donation via the Co\u2212S\u2212Pd bridge. In contrast, the unfilled\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>xy<\/jats:sub>\n                    orbital of high\u2010spin Co\n                    <jats:sup>III<\/jats:sup>\n                    (t\n                    <jats:sub>2g<\/jats:sub>\n                    <jats:sup>5<\/jats:sup>\n                    e\n                    <jats:sub>g<\/jats:sub>\n                    <jats:sup>1<\/jats:sup>\n                    ) is essential for controlling the\n                    <jats:italic>d<\/jats:italic>\n                    <jats:sub>xy<\/jats:sub>\n                    electron of Pd via \u03c0\u2010donation. Benefiting from  state optimization by \u03c3\u2010donation, Pd\u2013PdS\n                    <jats:sub>2<\/jats:sub>\n                    \u2013Co\n                    <jats:sub>4.0<\/jats:sub>\n                    delivers superior performance toward various bio\u2010alcohols (ethanol, ethylene glycol, and glycerol) with enhanced C\u2500C bond cleavage. Furthermore, coupling the glycerol oxidation reaction with the CO\n                    <jats:sub>2<\/jats:sub>\n                    reduction reaction (GOR||CO\n                    <jats:sub>2<\/jats:sub>\n                    RR), the electricity consumption of GOR||CO\n                    <jats:sub>2<\/jats:sub>\n                    RR drops 46.4% compared to the state\u2010of\u2010art system (OER||CO\n                    <jats:sub>2<\/jats:sub>\n                    RR). Moreover, anodic Faraday efficiency (FE) of formic acid can be attainable at more than 90% at low voltage regions.\n                  <\/jats:p>","DOI":"10.1002\/anie.202506032","type":"journal-article","created":{"date-parts":[[2025,4,25]],"date-time":"2025-04-25T02:15:49Z","timestamp":1745547349000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Enhancing C\u2500C Bond Cleavage of Glycerol Electrooxidation Through Spin\u2010Selective Electron Donation in\u00a0Pd\u2013PdS\n                    <sub>2<\/sub>\n                    \u2013Co\n                    <sub>x<\/sub>\n                    Heterostructural Nanosheets"],"prefix":"10.1002","volume":"64","author":[{"given":"Pei","family":"Liu","sequence":"first","affiliation":[{"name":"College of sciences Henan Agricultural University  Zhengzhou 450000 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hao","family":"Ma","sequence":"additional","affiliation":[{"name":"Institute of Technology for Carbon Neutrality, Shenzhen Institute of Advanced Technology Chinese Academy of Sciences  Shenzhen 518055 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuchen","family":"Qin","sequence":"additional","affiliation":[{"name":"College of sciences Henan Agricultural University  Zhengzhou 450000 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Junjun","family":"Li","sequence":"additional","affiliation":[{"name":"Department of Chemistry, School of Science Tianjin University  Tianjin 300072 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fengwang","family":"Li","sequence":"additional","affiliation":[{"name":"School of Chemical and Biomolecular Engineering and ARC Centre of Excellence for Green Electrochemical Transformation of Carbon Dioxide The University of Sydney  Sydney NSW 2006 Australia"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jinyu","family":"Ye","sequence":"additional","affiliation":[{"name":"Key Laboratory of Physical Chemistry of Solid Surfaces, college of Chemistry and Chemical Engineering Xiamen University  Xiamen Fujian 361005 P.R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qiudi","family":"Guo","sequence":"additional","affiliation":[{"name":"College of sciences Henan Agricultural University  Zhengzhou 450000 P.R. 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