Polyketones from Carbon Dioxide and Ethylene by Integrating Electrochemical and Organometallic Catalysis

The utilization of carbon dioxide in polymer synthesis is an attractive strategy for sustainable materials. Electrochemical CO2 reduction would offer a natural starting point for producing monomers, but the conditions of electrocatalysis are often drastically different from the conditions of organometallic coordination-insertion polymerization. Reported here is a strategy for integrating electrochemical and organometallic catalysts that enables polyketone synthesis from CO2 and ethylene in a single multicompartment reactor. Polyketone materials that are up to 50% derived from CO2 can be prepared in this way. Potentiostatic control over the CO-producing catalyst enables the controlled generation of low-pressure CO, which in conjunction with a palladium phosphine sulfonate organometallic catalyst enables copolymerization to nonalternating polyketones with the CO content tuned based on the applied current density