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

• Published in: Nature communications Vol. 11; no. 1; p. 2455
• Main Authors: Zhao, Kun, Nie, Xiaowa, Wang, Haozhi, Chen, Shuo, Quan, Xie, Yu, Hongtao, Choi, Wonyong, Zhang, Guanghui, Kim, Bupmo, Chen, Jingguang G.
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 15.05.2020; Nature Publishing Group; Nature Portfolio
• Subjects: 639/301/299/886; 639/638/563/979; 639/638/675; 639/638/77/884; Acetone; Activation energy; Carbon; Carbon dioxide; Catalysts; Coordination; Copper; Coupling; Density functional theory; Electrocatalysts; Electrowinning; Encapsulation; Humanities and Social Sciences; multidisciplinary; Science; Science (multidisciplinary)
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-020-16381-8

Efficient electroreduction of CO 2 to multi-carbon products is a challenging reaction because of the high energy barriers for CO 2 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 CO 2 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 μg h −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 CO 2 activation and C–C coupling. The energetically favorable pathways for CH 3 COCH 3 production from CO 2 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 CO 2 to multi-carbon products. Efficient electroreduction of CO 2 to multi-carbon products is challenging. Here, the single atom Cu encapsulated on N-doped porous carbon catalysts are designed for reducing CO 2 to acetone at low overpotentials and the active sites are identified as Cu coordination with four pyrrole-N atoms.