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Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses
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Journal Article
Steering the structure and selectivity of CO2 electroreduction catalysts by potential pulses
2022
Overview
Convoluted selectivity trends and a missing link between reaction product distribution and catalyst properties hinder practical applications of the electrochemical CO
2
reduction reaction (CO
2
RR) for multicarbon product generation. Here we employ operando X-ray absorption and X-ray diffraction methods with subsecond time resolution to unveil the surprising complexity of catalysts exposed to dynamic reaction conditions. We show that by using a pulsed reaction protocol consisting of alternating working and oxidizing potential periods that dynamically perturb catalysts derived from Cu
2
O nanocubes, one can decouple the effect of the ensemble of coexisting copper species on the product distribution. In particular, an optimized dynamic balance between oxidized and reduced copper surface species achieved within a narrow range of cathodic and anodic pulse durations resulted in a twofold increase in ethanol production compared with static CO
2
RR conditions. This work thus prepares the ground for steering catalyst selectivity through dynamically controlled structural and chemical transformations.
The relationship between product selectivity and catalyst structure under dynamic reaction conditions has proved difficult to interpret in electrocatalytic CO
2
reduction. Here, the authors combine operando X-ray techniques with high time resolution to investigate control over product selectivity using potential pulses.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
