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By systematically correlating experimental parameters (redox potentials\n                    <jats:italic>E<\/jats:italic>\n                    <jats:sub>1\/2<\/jats:sub>\n                    and acid dissociation constants p\n                    <jats:italic>K<\/jats:italic>\n                    <jats:sub>a<\/jats:sub>\n                    ), we constructed stepwise thermodynamic frameworks that reveal a continuous O\u2500H bond dissociation free energy (BDFE\n                    <jats:sub>O\u2010H<\/jats:sub>\n                    ) range spanning 68.5 to 106.7\u00a0kcal\/mol in these copper\u2013oxygen cores. Notably, while ligand substitution elicited only marginal variations in BDFE\n                    <jats:sub>O\u2010H<\/jats:sub>\n                    when maintaining a fixed overall charge of Cu\u2500O\u2500Cu structure, modulation of the Cu\u2500O\u2500Cu core charge demonstrated superior efficacy over conventional steric\/electronic ligand modifications for activating inert C\u2500H bonds. Mechanistic studies revealed an efficient concerted electron\u2013proton transfer (CEPT) pathway between the Cu\n                    <jats:sup>II<\/jats:sup>\n                    \u2500O\u2500Cu\n                    <jats:sup>II<\/jats:sup>\n                    and TEMPOH, achieving a remarkable second\u2010order rate constant of 1745.4 M\n                    <jats:sup>\u22121<\/jats:sup>\n                    s\n                    <jats:sup>\u22121<\/jats:sup>\n                    . This quantitative correlation between thermodynamic parameters and reaction kinetics provides fundamental principles for rational catalyst engineering.\n                  <\/jats:p>","DOI":"10.1002\/chem.71780","type":"journal-article","created":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T06:46:35Z","timestamp":1791614795000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Energetics of Proton\u2010Coupled Electron Transfer in Hydroxy\u2010Bridged Dicopper Complexes with\n                    <i>N<\/i>\n                    \u2010Heterocyclic Carbene (NHC) Ligands"],"prefix":"10.1002","author":[{"given":"Ning","family":"Ai","sequence":"first","affiliation":[{"name":"Center of Basic Molecular Science (CBMS), Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiao\u2010Ming","family":"Wang","sequence":"additional","affiliation":[{"name":"Center of Basic Molecular Science (CBMS), Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yu\u2010Hua","family":"Guo","sequence":"additional","affiliation":[{"name":"Center of Basic Molecular Science (CBMS), Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hong\u2010Tao","family":"Zhang","sequence":"additional","affiliation":[{"name":"Center of Basic Molecular Science (CBMS), Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8916-3986","authenticated-orcid":false,"given":"Han","family":"Li","sequence":"additional","affiliation":[{"name":"School of Petrochemical Engineering Changzhou University  Changzhou China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8808-9641","authenticated-orcid":false,"given":"Ming\u2010Tian","family":"Zhang","sequence":"additional","affiliation":[{"name":"Center of Basic Molecular Science (CBMS), Department of Chemistry Tsinghua University  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,9]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"crossref","first-page":"507","DOI":"10.1038\/417507a","article-title":"Understanding and Exploiting C\u2013H Bond Activation","volume":"417","author":"Labinger J. 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F.Dahl \u201cElectrochemical Analysis of Biocapped Triangular Cobalt Cyclopentadienyl Clusters [Co3(\u03b75\u2010C5H5\u2010xMex)3(\u03bc3\u2010X)(\u03bc3\u2010Y)]n(x = 0 1 5) Containing Mixed \u03c0\u2010Acceptor X and \u03c0\u2010Donor Y Capping Ligands [X = CO NO; Y = NSiMe3 NC(O)NH2 NH]: Pronounced Variations in Redox Behavior as a Function of Coordinating Ligands \u201d Journal of American Chemical Society 108 (1986): 5933\u20135594.","DOI":"10.1021\/ja00279a044"}],"container-title":["Chemistry \u2013 A European Journal"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/chemistry-europe.onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/chem.71780","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/chemistry-europe.onlinelibrary.wiley.com\/doi\/full-xml\/10.1002\/chem.71780","content-type":"application\/xml","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/chemistry-europe.onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/chem.71780","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,10]],"date-time":"2026-10-10T06:46:42Z","timestamp":1791614802000},"score":1,"resource":{"primary":{"URL":"https:\/\/chemistry-europe.onlinelibrary.wiley.com\/doi\/10.1002\/chem.71780"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,10,9]]},"references-count":47,"alternative-id":["10.1002\/chem.71780"],"URL":"https:\/\/doi.org\/10.1002\/chem.71780","archive":["Portico"],"relation":{},"ISSN":["0947-6539","1521-3765"],"issn-type":[{"value":"0947-6539","type":"print"},{"value":"1521-3765","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,10,9]]},"assertion":[{"value":"2026-08-01","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-09-29","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2026-10-09","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e71780"}}