Atomically Thin Two-Dimensional Solids: An Emerging Platform for CO₂ Electroreduction

Benefiting from the high specific surface area and the ensuing novel electronic structures, atomically thin two-dimensional (2D) solids have drawn intense interest in the field of carbon dioxide (CO2) catalysis. Here we review the major advantages of atomically thin 2D solids for electrochemical CO2 reduction, and special emphasis will be paid to the recent advances in fine characterization and controllable tailoring of the local atomic and electronic structure. Because surface atoms in atomically thin 2D solids are comparable to the overall atoms, we highlight surface modifications, such as molecular functionalization, heteroatom incorporation, and defect engineering, as effective ways to manipulate the reactivity. Finally, the major challenges and opportunities for future development of this field are discussed. As a well-defined model system, atomically thin 2D solids offer practical possibilities to study the structure–catalytic activity relationship at the atomic level.