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Here, generalizable structure\u2013activity relationships apply to a series of heterodinuclear polymerization catalysts featuring Co(III) and s\u2010block metals M(I\/II) (M=Na(I), K(I), Ca(II), Sr(II), Ba(II)). These are shown to apply to polycarbonate production by the ring\u2010opening copolymerizations (ROCOP) of cyclohexene oxide (CHO) and carbon dioxide (CO<jats:sub>2<\/jats:sub>), conducted at high (20\u2005bar) and low (1\u2005bar) CO<jats:sub>2<\/jats:sub> pressures, and to polyester production by copolymerization of cyclohexene oxide and phthalic anhydride (PA). For the CHO\/PA and high\u2010pressure CHO\/CO<jats:sub>2<\/jats:sub> copolymerizations, activity increases exponentially with s\u2010block metal acidity peaking at the Co(III)K(I) catalyst, whilst for the low\u2010pressure CHO\/CO<jats:sub>2<\/jats:sub> copolymerization it increases linearly to the same metal combination. The polymerization kinetics fit second order rate laws and the correlations support dinuclear metallate mechanistic hypotheses. These relationships help understand and identify key metal complex structural features in synergic polymerization catalysis.<\/jats:p>","DOI":"10.1002\/anie.202422497","type":"journal-article","created":{"date-parts":[[2025,1,6]],"date-time":"2025-01-06T10:14:13Z","timestamp":1736158453000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Structure\u2010Activity Relationships for s\u2010Block Metal\/Co(III) Heterodinuclear Catalysts in Cyclohexene Oxide Ring\u2010Opening Copolymerizations"],"prefix":"10.1002","volume":"64","author":[{"ORCID":"https:\/\/orcid.org\/0000-0003-1715-2775","authenticated-orcid":false,"given":"Frederica","family":"Butler","sequence":"first","affiliation":[{"name":"Department of Chemistry University of Oxford  12 Mansfield Road Oxford OX1 3TA United Kingdom"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0004-7309-4519","authenticated-orcid":false,"given":"Francesca","family":"Fiorentini","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Oxford  12 Mansfield Road Oxford OX1 3TA United Kingdom"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-0659-4661","authenticated-orcid":false,"given":"Katharina H. 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