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Ionic Exchange of Metal–Organic Frameworks to Access Single Nickel Sites for Efficient Electroreduction of CO2

Zhao, Changming, Dai, Xinyao, Yao, Tao, Chen, Wenxing, Wang, Xiaoqian, Wang, Jing, Yang, Jian, Wei, Shiqiang, Wu, Yuen, Li, Yadong
Journal of the American Chemical Society 2017 v.139 no.24 pp. 8078-8081
carbon dioxide, carbon monoxide, catalysts, catalytic activity, chemical reactions, coordination polymers, geometry, ions, nickel, zinc
Single-atom catalysts often exhibit unexpected catalytic activity for many important chemical reactions because of their unique electronic and geometric structures with respect to their bulk counterparts. Herein we adopt metal–organic frameworks (MOFs) to assist the preparation of a catalyst containing single Ni sites for efficient electroreduction of CO₂. The synthesis is based on ionic exchange between Zn nodes and adsorbed Ni ions within the cavities of the MOF. This single-atom catalyst exhibited an excellent turnover frequency for electroreduction of CO₂ (5273 h–¹), with a Faradaic efficiency for CO production of over 71.9% and a current density of 10.48 mA cm–² at an overpotential of 0.89 V. Our findings present some guidelines for the rational design and accurate modulation of nanostructured catalysts at the atomic scale.