Novel efficient and inexpensive catalytic processes that interconvert electrical energy and chemical bonds are needed for sustainable fuel cell technologies. The oxygen reduction reaction (ORR) is a redox reaction with broad application in most types of fuel cells. Decades of intense research have been invested in developing alternative catalysts to platinum for ORR. In this talk, we discuss efforts within the Center for Molecular Electrocatalysis to develop electrocatalysts based on Fe phorphyrin and bathophen macrocycles, and iron- and nitrogen-doped carbon (Fe-N-C) materials. Our strategy is to exploit the well-defined nature of homogeneous catalysts to obtain a detailed quantitation of the factors that control reactivity, which then can be used to inform the design of heterogeneous catalysts. We show how integrating theory and computation with experimental investigations it is possible to gather a fundamental understanding of the factors that modulate rates, selectivity and overpotentials. Specifically, we show how tuning inductive and through-space effects of the scaffold embedding the metal center, as well as the surrounding reaction medium, it is possible to rationally control catalysis.

Short- and long-range regulation of electrocatalytic oxygen reduction

ACS Spring 2022

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