Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), University of Science and Technology of China , Hefei 230026, China.
Hefei National Laboratory for Physical Sciences at the Microscale, University of Science and Technology of China , Hefei 230026, China.
J Am Chem Soc. 2017 Jun 21;139(24):8078-8081. doi: 10.1021/jacs.7b02736. Epub 2017 Jun 13.
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 CO. 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 CO (5273 h), with a Faradaic efficiency for CO production of over 71.9% and a current density of 10.48 mA cm 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.
单原子催化剂因其独特的电子和几何结构，相对于其体相对应物，往往对许多重要化学反应表现出意想不到的催化活性。在此，我们采用金属有机框架（MOFs）辅助制备含有单镍位点的催化剂，以实现 CO 的高效电化学还原。该合成方法基于 Zn 节点与吸附在 MOF 腔体内的 Ni 离子之间的离子交换。该单原子催化剂在 CO 的电化学还原中表现出优异的周转频率（5273 h），对 CO 生成的法拉第效率超过 71.9%，在 0.89 V 的过电势下，电流密度为 10.48 mA cm。我们的研究结果为在原子尺度上合理设计和精确调控纳米结构催化剂提供了一些指导。
