Importance of Charge Transfer Descriptor for the Computational Screening of Electrocatalysts

Abstract

Listen

Translate article

Electrochemistry has become a key player in establishing a global sustainable energy landscape. Unfortunately, most electrochemical processes are limited in their efficiency and selectivity which has prevented them from replacing carbon-intensive industrial processes. Computational simulations have the potential to conquer the vast chemical space and reveal so far unconsidered new electrocatalysts and boost the performance of these devices. This, however, requires the knowledge of computationally accessible activity and selectivity descriptors. In this work, and by the example of electrochemical CO2 reduction, it is shown that the conventionally considered adsorption energy descriptor is not enough to distinguish product selectivity among catalysts. Including specifically the electrochemical environment in the quantum chemical calculations, we find that a charge-transfer descriptor is separately re- quired, such as the work function or the potential of zero charge. With this, experimental trends in product selectivity can be well described, thus providing a new set of descriptors for high-throughput screening of electrocatalysts.