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Design of Single-Atom Co–N 5 Catalytic Site: A Robust Electrocatalyst for CO 2 Reduction with Nearly 100% CO Selectivity and Remarkable Stability

2018; American Chemical Society; Volume: 140; Issue: 12 Linguagem: Inglês

10.1021/jacs.8b00814

1943-2984

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,

Ionic liquids properties and applications

We develop an N-coordination strategy to design a robust CO2 reduction reaction (CO2RR) electrocatalyst with atomically dispersed Co-N5 site anchored on polymer-derived hollow N-doped porous carbon spheres. Our catalyst exhibits high selectivity for CO2RR with CO Faradaic efficiency (FECO) above 90% over a wide potential range from -0.57 to -0.88 V (the FECO exceeded 99% at -0.73 and -0.79 V). The CO current density and FECO remained nearly unchanged after electrolyzing 10 h, revealing remarkable stability. Experiments and density functional theory calculations demonstrate single-atom Co-N5 site is the dominating active center simultaneously for CO2 activation, the rapid formation of key intermediate COOH* as well as the desorption of CO.