Design of Single-Atom Co–N5 Catalytic Site: A Robust Electrocatalyst for CO2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability

作者：Yuan Pan, Rui Lin, Yinjuan Chen, Shoujie Liu, Wei Zhu, Xing Cao, Wenxing Chen, Konglin Wu, Weng‐Chon Cheong, Yu Wang, Lirong Zheng, Jun Luo, Yan Lin, Yunqi Liu, Chenguang Liu, Jun Li, Qi Lu, Xin Chen, Dingsheng Wang, Qing Peng, Chen Chen, Yadong Li · 发表于：Journal of the American Chemical Society · 年份：2018 · DOI：10.1021/jacs.8b00814 · 被引用次数：1235 · 研究领域：CO2 Reduction Techniques and Catalysts、Carbon dioxide utilization in catalysis、Ionic liquids properties and applications

We develop an N-coordination strategy to design a robust CO 2 reduction reaction (CO 2 RR) electrocatalyst with atomically dispersed Co–N 5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO 2 RR with CO Faradaic efficiency (FE CO ) above 90% over a wide potential range from −0.57 to −0.88 V (the FE CO exceeded 99% at −0.73 and −0.79 V). The CO current density and FE CO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co–N 5 site is the dominating active center simultaneously for CO 2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.