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However, it is plagued by a compromised catalytic performance due to the severe hydrogen evolution reaction (HER). Here, two types of silver chalcogenolate cluster\u2010based MOFs were synthesized through ligand engineering by anchoring Ag\n                    <jats:sub>12<\/jats:sub>\n                    clusters with tri\u2010topic imidazole and pyridyl ligands respectively. The imidazole\u2010based MOF\n                    <jats:bold>\n                      Ag\n                      <jats:sub>12<\/jats:sub>\n                      THIT\n                    <\/jats:bold>\n                    demonstrated outstanding performance for the electroreduction of CO\n                    <jats:sub>2<\/jats:sub>\n                    to CO. In acidic electrolyte of pH\u00a0\u2248\u00a02, it achieved a Faradaic efficiency (FE) of 98.5% with a commercial current density of 328.0\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    at\u00a0\u2212\u00a01.6\u00a0V versus RHE. Moreover, the CO partial current density (\n                    <jats:italic>j<\/jats:italic>\n                    <jats:sub>CO<\/jats:sub>\n                    ) reached a maximum of 447.2\u00a0mA cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    with a FE\n                    <jats:sub>CO<\/jats:sub>\n                    of 96.8% at\u00a0\u2212\u00a01.7\u00a0V versus RHE. No obvious degradation was observed during 70\u00a0h of continuous operation, and the performance significantly outperformed those of pyridyl\u2010based MOFs\n                    <jats:bold>\n                      Ag\n                      <jats:sub>12<\/jats:sub>\n                      TPEB\n                    <\/jats:bold>\n                    and\n                    <jats:bold>\n                      Ag\n                      <jats:sub>12<\/jats:sub>\n                      TPMA\n                    <\/jats:bold>\n                    . Mechanistic studies revealed that the imidazole ligand endows\n                    <jats:bold>\n                      Ag\n                      <jats:sub>12<\/jats:sub>\n                      THIT\n                    <\/jats:bold>\n                    with enhanced Lewis basicity and superior\n                    <jats:italic>\u03c3<\/jats:italic>\n                    \u2010donating ability, thereby strengthening the ligand field with an upshifted\n                    <jats:italic>d<\/jats:italic>\n                    \u2010band center and reduced energy barriers. This ligand effect facilitates more efficient electron transfer to *COOH intermediates, thus promoting acidic CO\n                    <jats:sub>2<\/jats:sub>\n                    to CO conversion.\n                  <\/jats:p>","DOI":"10.1002\/anie.202518779","type":"journal-article","created":{"date-parts":[[2026,1,10]],"date-time":"2026-01-10T13:51:10Z","timestamp":1768053070000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":15,"title":["Regulation of the\n                    <i>D<\/i>\n                    \u2010Band Center Through Ligand Engineering in Silver Cluster\u2010Based MOFs Enhances Acidic CO\n                    <sub>2<\/sub>\n                    Electroreduction"],"prefix":"10.1002","volume":"65","author":[{"given":"Yuan\u2010Yuan","family":"Liu","sequence":"first","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xin","family":"Wang","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi\u2010Zhao","family":"Liang","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu","family":"Ma","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bing\u2010Zi","family":"Cai","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yi\u2010Bo","family":"Zhou","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhan\u2010Gang","family":"Han","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8912-0241","authenticated-orcid":false,"given":"Xiao\u2010Jia","family":"Zhao","sequence":"additional","affiliation":[{"name":"Hebei Technology Innovation Center for Energy Conversion Materials and Devices Hebei Key Laboratory of Inorganic Nano\u2010Materials College of Chemistry and Materials Science Hebei Normal University  Shijiazhuang Hebei 050024 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