Miao, Qiyang; Lu, Chengbao; Xu, Qing; Yang, Shuai; Liu, Minghao; Liu, Sijia; Yu, Chengbing; Zhuang, Xiaodong; Jiang, Zheng; Zeng, Gaofeng

CHEMICAL ENGINEERING JOURNAL

2022, 450, 1385-8947

Miao, Qiyang; Lu, Chengbao; Xu, Qing; Yang, Shuai; Liu, Minghao; Liu, Sijia; Yu, Chengbing; Zhuang, Xiaodong; Jiang, Zheng; Zeng, Gaofeng

Electrocatalytic CO2 reduction (CO2RR) is critical in addressing CO2 emissions. Single atom catalysts, are attracting considerable attention for CO2RR because of their high atom utilization efficiencies and tailored electron states. However, the catalytic sites remain limited and developing novel catalytic centers is a significant and challenge. Herein, for the first time, we fabricated CoN2O2 sites in 2D carbon for use in CO2RR via template pyrolysis of covalent organic frameworks (COFs). After forming the COF on the surface of Mg/Al-LDH, the obtained catalyst displayed a layered morphology with a thickness of approximately 36 nm and had abundant CoN2O2 sites (4.27 wt% Co). The catalyst showed a remarkable catalytic activity towards CO2RR, with Faradaic efficiencies of 80.2-96.5 % at applied potentials between -0.6 and -1.0 V. Theoretical calculations showed that the CoN2O2 sites favor the stretching and cleavage of COOH* at the Co active centers, accelerating the rate-determining step of COOH* formation.