The Electrochemical Conversion of CO2 with Molecular Co Catalysts: Modulating Activity and Reaction Selectivity by Controlling a Catalyst's Coordination Environment

Friday, October 8, 2021 - 1:10pm
Event Type: 

Charles McCrory

Dr. Charles McCrory, University of Michigan

Host: Dr. VanVeller

The selective electrochemical reduction of CO2 in the CO2 reduction reaction (CO2RR) is a crucial strategy for storing energy from intermittent sources in the form of chemical bonds (e.g. solar fuels).  State-of-the-art solid-state catalysts produce useful products, but typically do so non-selectively with H2 production from competitive water reduction.  Alternatively, molecular catalysts show promise for the selective reduction of CO2 to single products, but usually perform with lower activity compared to their solid-state analogues.  My research group is focused on the development of new catalytic systems for the CO2RR that operate with the selectivity of molecular catalysts but the activity of solid-state catalysts.

In this talk, I will present some of our work using polymer encapsulation to increase the catalytic activity and selectivity of molecular catalysts for the CO2RR.  In particular, we show that encapsulating cobalt phthalocyanine within a coordinating polyvinylpyridine polymer leads to a dramatic enhancement in its activity and selectivity for the CO2RR in aqueous phosphate solution. Using a combination of electroanalytical studies and in situ electrochemical X-ray absorbance measurements, we demonstrate that the encapsulating polymer modulates all coordination spheres surrounding the catalyst active site, and that this has a profound impact on the catalytic performance and mechanism.