Scalable strategy to fabricate single Cu atoms coordinated carbons for efficient electroreduction of CO2 to CO

Abstract Developing efficient, selective, and stable single-atom electrocatalysts for CO2 reduction reaction (CO2RR) is attractive but still remains a challenging, especially for scalable production with low-cost. Among the non-precious metal single-atom electrocatalysts, Cu single-atom electrocatalysts are rarely explored for the efficient CO2-to-CO conversion. Herein, we reported a facile and scalable strategy to prepare the Cu single-atom catalyst (Cu SAs/NC) with exceptional CO production performances. Atomically dispersed Cu–N4 moieties are unambiguously verified by HAADF-STEM and XANES measurements. The as-prepared Cu SAs/NC catalyst delivers a high CO faradaic efficiency of 92% at −0.7 VRHE as well as the excellent durability over 30 h successive electrolysis. It should be noted that this is one of the rare examples of efficient CO production on Cu single-atom electrocatalyst. Besides, the 20-g + samples can be readily fabricated in one batch and exhibit the almost identical CO2RR performances. Furthermore, the combined experimental and theoretical calculation results identify the genuine active Cu–N4 sites are responsible for the high selectivity and efficiency of CO production. This work provides a novel strategy for scalable single-atom electrocatalysts in stable quality and offers new insights into the efficient CO2-to-CO conversion on Cu single-atom electrocatalyst.