Tunable Molecular‐Scale Materials for Catalyzing the Low‐Overpotential Electrochemical Conversion of CO2

Abstract Electrochemical CO 2 reduction provides a clean and viable alternative for mitigating the environmental aspects of global greenhouse gas emissions. To date, the simultaneous goals of CO 2 reduction at high selectivity and activity have yet to be achieved. Here, the importance of engineering both sides of the electrode–electrolyte interface as a rational strategy for achieving this milestone is highlighted. An emphasis is placed on researchers contributing to the design of solid electrodes based on metal–organic frameworks (MOFs) and electrolytes based on room‐temperature ionic liquids (RTILs). Future research geared toward optimizing the electrode–electrolyte interface for efficient and selective CO 2 reduction can be achieved by understanding the structure of newly designed RTILs at the electrified interface, as well as structure–activity relationships in highly tunable MOF platforms.