The dynamic behaviors of heterogeneous interfaces in electrocatalytic CO2 reduction

Abstract

The electrocatalytic CO₂ reduction reaction (CO₂RR) is a highly promising renewable energy technology that can convert greenhouse gases into valuable fuels and chemicals. However, under ordinary operating conditions, significant dynamic evolution behavior occurs on the catalyst surface, which is mainly manifested as surface morphology evolution and property changes, eventually leading to changes in the active sites of the reaction, affecting selectivity and efficiency. To develop efficient electrocatalytic systems with excellent performance, an essential prerequisite is to understand the underlying mechanism of surface dynamic evolution. Studying the influence of the external environment on dynamic evolution is as important as studying the intrinsic structural properties of catalysts. In this review, we first introduce the concept of dynamic evolution and then emphasize the influence of the external environment (applied potential, temperature, electrolyte, and impurities) on CO₂RR dynamic evolution. We also address the use of operando characterization techniques and pulsed CO₂ electrolysis methods for monitoring and controlling dynamic evolution behaviors under working conditions, along with theoretical methods, including ab initio calculations and machine learning that can simulate dynamic behavior. Finally, we present several current challenges and prospects for the development of techniques for controlling the CO₂RR dynamic evolution.