The Interactive Dynamics of Nanocatalyst Structure and Microenvironment during Electrochemical CO2 Conversion

In the pursuit of a decarbonized society, electrocatalytic CO2 conversion has drawn tremendous research interest in recent years as a promising route to recycling CO2 into more valuable chemicals. To achieve high catalytic activity and selectivity, nanocatalysts of diverse structures and compositions have been designed. However, the dynamic structural transformation of the nanocatalysts taking place under operating conditions makes it difficult to study active site configurations present during the CO2 reduction reaction (CO2RR). In addition, although recognized as consequential to the catalytic performance, the reaction microenvironment generated near the nanocatalyst surface during CO2RR and its impact are still an understudied research area. In this Perspective, we discuss current understandings and difficulties associated with investigating such dynamic aspects of both the surface reaction site and its surrounding reaction environment as a whole. We further highlight the interactive influence of the structural transformation and the microenvironment on the catalytic performance of nanocatalysts. We also present future research directions to control the structural evolution of nanocatalysts and tailor their reaction microenvironment to achieve an ideal catalyst for improved electrochemical CO2RR.