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Uncovering Structure-Activity Relationships in Sustainable Polymerisation Catalysis

Presentation given by Frederica Butler at the UK Catalysis Hub summer conference 2025. Uncovering structure-activity relationships in homogeneous polymerisation catalysis is essential in informing a rational approach to improve catalyst performance. This talk presents generalisable structure-activity relationships for a series of Co(III)M(I/II) heterodinuclear catalysts, where M(I/II) = Na(I), K(I), Ca(II), Sr(II), Ba(II), as applied to the ring-opening copolymerisation of epoxides with carbon dioxide and with anhydrides.1, 2 These copolymerisation reactions enable the controlled, atom economic synthesis of polycarbonates and polyesters, both important polymers for a future circular materials economy. Catalytic activity was found to correlate with M(I/II) Lewis acidity, peaking when M = K(I), and this finding proved to be general across different monomer combinations. These activity-acidity relationships provide insights into intermetallic synergy, as well as information on the distinct role of each metal in the polymerisation mechanism. References: (1) Butler, F.; Fiorentini, F.; Eisenhardt, K. H. S.; Williams, C. K. Structure-Activity Relationships for s-Block Metal/Co(III) Heterodinuclear Catalysts in Cyclohexene Oxide Ring-Opening Copolymerizations. Angew. Chem. Int. Ed. 2025, e202422497. (2) Fiorentini, F.; Diment, W. T.; Deacy, A. C.; Kerr, R. W. F.; Faulkner, S.; Williams, C. K. Understanding catalytic synergy in dinuclear polymerization catalysts for sustainable polymers. Nat. Commun. 2023, 14 (1), 4783.