Polyketones from Carbon Dioxide and Ethylene by Integrating Electrochemical and Organometallic Catalysis
Henry M. Dodge, Benjamin S. Natinsky, Brandon Jolly, Haochuan Zhang, Yu Mu, Scott M. Chapp, Thi V. Tran, Paula L. Diaconescu, Loi H., Dunwei Wang, Chong Liu, Alexander J. M. Miller
Abstract
The utilization of carbon dioxide in polymer synthesis is an attractive strategy for sustainable materials. Electrochemical CO 2 reduction would offer a natural starting point for producing monomers, but the conditions of electrocatalysis are often drastically different from the conditions of coordination–insertion polymerization. Reported here is a strategy for coupling electrochemical and organometallic catalysts that enables polyketone synthesis from CO 2 and ethylene in a single multicompartment reactor. Polyketone materials that are CO 2 -derived up to 50 wt % 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.