Selective electroreduction of CO2 to acetone by single copper atoms anchored on N-doped porous carbon

Efficient electroreduction of CO2 to multi-carbon products is a challenging reaction because of the high energy barriers for CO2 activation and C-C coupling, which can be tuned by designing the metal centers and coordination environments of catalysts. Here, we design single atom copper encapsulated on N-doped porous carbon (Cu-SA/NPC) catalysts for reducing CO2 to multi-carbon products. Acetone is identified as the major product with a Faradaic efficiency of 36.7% and a production rate of 336.1 mu gh(-1). Density functional theory (DFT) calculations reveal that the coordination of Cu with four pyrrole-N atoms is the main active site and reduces the reaction free energies required for CO2 activation and C-C coupling. The energetically favorable pathways for CH3COCH3 production from CO2 reduction are proposed and the origin of selective acetone formation on Cu-SA/NPC is clarified. This work provides insight into the rational design of efficient electrocatalysts for reducing CO2 to multi-carbon products. Efficient electroreduction of CO2 to multi-carbon products is challenging. Here, the single atom Cu encapsulated on N-doped porous carbon catalysts are designed for reducing CO2 to acetone at low overpotentials and the active sites are identified as Cu coordination with four pyrrole-N atoms.