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Regulation of Coordination Number over Single Co Sites: Triggering the Efficient Electroreduction of CO 2

2017; Wiley; Volume: 57; Issue: 7 Linguagem: Inglês

10.1002/anie.201712451

1521-3773

Xiaoqian Wang, Chen Zhao, Xuyan Zhao, Tao Yao, Wenxing Chen, Rui You, Changming Zhao, Geng Wu, Jing Wang, Weixin Huang, Jinlong Yang, Xun Hong, Shiqiang Wei, Yuen Wu, Yadong Li,

Electrocatalysts for Energy Conversion

Abstract The design of active, selective, and stable CO 2 reduction electrocatalysts is still challenging. A series of atomically dispersed Co catalysts with different nitrogen coordination numbers were prepared and their CO 2 electroreduction catalytic performance was explored. The best catalyst, atomically dispersed Co with two‐coordinate nitrogen atoms, achieves both high selectivity and superior activity with 94 % CO formation Faradaic efficiency and a current density of 18.1 mA cm −2 at an overpotential of 520 mV. The CO formation turnover frequency reaches a record value of 18 200 h −1 , surpassing most reported metal‐based catalysts under comparable conditions. Our experimental and theoretical results demonstrate that lower a coordination number facilitates activation of CO 2 to the CO 2 .− intermediate and hence enhances CO 2 electroreduction activity.