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<p>Despite many CO<sub>2</sub> use strategies being reliant on fast and selective CO<sub>2</sub> insertion reactions into metal-alkoxide bonds, in-depth studies into this chemistry remain rare. Here the effect of CO<sub>2</sub> pressure on the CO<sub>2</sub> insertion chemistry is studied using epoxide–CO<sub>2</sub> copolymerizations. Five high-performance literature catalysts are investigated under systematically varied CO<sub>2</sub> pressures, revealing kinetic profiles indicative of CO<sub>2</sub> insertion equilibria. For each catalyst, two key parameters describing the CO<sub>2</sub> insertion chemistry are determined: the equilibrium constant, <i>K</i><sub>eq</sub>, and the saturation CO<sub>2</sub> pressure above which catalytic performance is maximized, <i>P</i><sub>threshold</sub>. Generalizable correlations between copolymerization activity, <i>K</i><sub>eq</sub> and <i>P</i><sub>threshold</sub> are uncovered and used to predict performances for four further catalyst–monomer combinations. These correlations are a direct link between CO<sub>2</sub> insertion chemistry and process operating conditions, providing a mechanistic framework and testing protocols to accelerate future catalyst development. These results should help deliver efficient scalable CO<sub>2</sub> use technologies, operating with minimal energy.</p><p></p>

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Understanding low-pressure CO2 insertion chemistry in epoxide–CO2 copolymerization catalysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年4月30日

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  • Rosie Thorogood,
  • Katharina H. S. Eisenhardt,
  • Madeleine L. Smith,
  • Charlotte K. Williams

摘要

Despite many CO2 use strategies being reliant on fast and selective CO2 insertion reactions into metal-alkoxide bonds, in-depth studies into this chemistry remain rare. Here the effect of CO2 pressure on the CO2 insertion chemistry is studied using epoxide–CO2 copolymerizations. Five high-performance literature catalysts are investigated under systematically varied CO2 pressures, revealing kinetic profiles indicative of CO2 insertion equilibria. For each catalyst, two key parameters describing the CO2 insertion chemistry are determined: the equilibrium constant, Keq, and the saturation CO2 pressure above which catalytic performance is maximized, Pthreshold. Generalizable correlations between copolymerization activity, Keq and Pthreshold are uncovered and used to predict performances for four further catalyst–monomer combinations. These correlations are a direct link between CO2 insertion chemistry and process operating conditions, providing a mechanistic framework and testing protocols to accelerate future catalyst development. These results should help deliver efficient scalable CO2 use technologies, operating with minimal energy.