Jiao Long, Yang Weijie, Wan Gang, Zhang Rui, Zheng Xusheng, Zhou Hua, Yu Shu-Hong, Jiang Hai-Long
Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Soft Matter Chemistry, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Department of Power Engineering, School of Energy, Power and Mechanical Engineering, North China Electric Power University, Baoding, 071003, P. R. China.
Angew Chem Int Ed Engl. 2020 Nov 9;59(46):20589-20595. doi: 10.1002/anie.202008787. Epub 2020 Sep 1.
Single-atom catalysts (SACs) are of great interest because of their ultrahigh activity and selectivity. However, it is difficult to construct model SACs according to a general synthetic method, and therefore, discerning differences in activity of diverse single-atom catalysts is not straightforward. Herein, a general strategy for synthesis of single-atom metals implanted in N-doped carbon (M -N-C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal-organic frameworks (MOFs). The M -N-C catalysts, featuring identical chemical environments and supports, provided an ideal platform for differentiating the activity of single-atom metal species. When employed in electrocatalytic CO reduction, Ni -N-C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe -, Co - and Cu -N-C. Remarkably, the best-performer, Ni -N-C, even demonstrated excellent CO FE at low CO pressures, thereby representing a promising opportunity for the direct use of dilute CO feedstock.
单原子催化剂（SACs）因其超高的活性和选择性而备受关注。然而，按照通用的合成方法构建模型单原子催化剂很困难，因此，辨别不同单原子催化剂的活性差异并非易事。在此，我们从多元金属有机框架（MOFs）出发，开发了一种合成嵌入氮掺杂碳中的单原子金属（M -N-C；M = Fe、Co、Ni和Cu）的通用策略。具有相同化学环境和载体的M -N-C催化剂为区分单原子金属物种的活性提供了理想平台。当用于电催化CO还原时，Ni -N-C表现出高达96.8%的非常高的CO法拉第效率（FE），远远超过Fe -、Co -和Cu -N-C。值得注意的是，表现最佳的Ni -N-C在低CO压力下甚至也表现出优异的CO FE，从而为直接使用稀CO原料提供了一个有前景的机会。
