Exclusive Ni–N4 Sites Realize Near-Unity CO Selectivity for Electrochemical CO2 Reduction

作者：Xiaogang Li, Wentuan Bi, Minglong Chen, Yuexiang Sun, Huanxin Ju, Wensheng Yan, Junfa Zhu, Xiaojun Wu, Wangsheng Chu, Changzheng Wu, Yi Xie · 发表于：Journal of the American Chemical Society · 年份：2017 · DOI：10.1021/jacs.7b09074 · 被引用次数：931 · 研究领域：CO2 Reduction Techniques and Catalysts、Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques

Electrochemical reduction of carbon dioxide (CO 2 ) to value-added carbon products is a promising approach to reduce CO 2 levels and mitigate the energy crisis. However, poor product selectivity is still a major obstacle to the development of CO 2 reduction. Here we demonstrate exclusive Ni–N 4 sites through a topo-chemical transformation strategy, bringing unprecedentedly high activity and selectivity for CO 2 reduction. Topo-chemical transformation by carbon layer coating successfully ensures preservation of the Ni–N 4 structure to a maximum extent and avoids the agglomeration of Ni atoms to particles, providing abundant active sites for the catalytic reaction. The Ni–N 4 structure exhibits excellent activity for electrochemical reduction of CO 2 with particularly high selectivity, achieving high faradaic efficiency over 90% for CO in the potential range from −0.5 to −0.9 V and gives a maximum faradaic efficiency of 99% at −0.81 V with a current density of 28.6 mA cm –2 . We anticipate exclusive catalytic sites will shed new light on the design of high-efficiency electrocatalysts for CO 2 reduction.