Nitrogen-Adsorbed Hydrogen Species Promote CO<sub>2</sub> Methanation on Cu Single-Atom Electrocatalyst
Anxiang Guan, Yalei Fan, Shibo Xi, Haoliang Huang, Quan Zhang, Naixin Lyu, Bowen Wu, Yangshen Chen, Zhengzheng Liu, Chao Yang, Yali Ji, Miao Kan, Linjuan Zhang, Gengfeng Zheng
Abstract
Cu single-atom catalysts are considered as efficient candidates to boost the electrocatalytic CO2 reduction to CH4, but the source of *H species for the CH4 formation during the multiple electron–proton transfer process is still elusive. Herein, we reported a facile strategy for the large-scale preparation of Cu single-atom catalysts via a solid-state pyrolysis strategy, with a Cu content of 3.86 wt %. The Cu single atoms were coordinated by four nitrogen atoms, which allowed to accelerate water dissociation to form *H species and stabilize key intermediates toward CH4. The Cu single-atom catalyst exhibited an excellent CO2-to-CH4 electroreduction performance, including a Faradaic efficiency of 68.2%, a high partial current density of 493.1 mA cm–2, and a good electrochemical stability. This work suggests a potential means of the mass production of Cu single-atom catalysts, with understanding of the mechanism of the CO2 electroreduction to CH4.