“…21,22 In addition, only by looking deep into the surface/interface structures of catalysts can we establish the structure-performance relationship for CO 2 RR catalysis, which is of fundamental importance for developing more advanced electrocatalysts. 2,23 In this review, we start with an overview of the advanced methodologies for probing the structures of catalyst surfaces/ interfaces (including synchrotron-radiation-based X-ray absorption spectroscopy, atomic-resolution electron microscopy, and infrared spectroscopy), which could offer more indepth insights into catalytic structures at the atomic level. Subsequently, we present a systematic overview on the recent progress in customizing the surfaces/interfaces of CO 2 RR electrocatalysts, including atomic-site catalysts (e.g., single-atomic-site catalysts, diatomic-site catalysts), metal catalysts, and metal/oxide catalysts.…”