Single‐Atom Electrocatalysts from Multivariate Metal–Organic Frameworks for Highly Selective Reduction of CO2 at Low Pressures

作者：Long Jiao, Weijie Yang, Gang Wan, Rui Zhang, Xusheng Zheng, Hua Zhou, Shu‐Hong Yu, Hai‐Long Jiang · 发表于：Angewandte Chemie International Edition · 年份：2020 · DOI：10.1002/anie.202008787 · 被引用次数：412 · 研究领域：CO2 Reduction Techniques and Catalysts、Metal-Organic Frameworks: Synthesis and Applications、Covalent Organic Framework Applications

Abstract 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 (M1‐N‐C; M=Fe, Co, Ni and Cu) has been developed starting from multivariate metal–organic frameworks (MOFs). The M1‐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 CO2 reduction, Ni1‐N‐C exhibited a very high CO Faradaic efficiency (FE) up to 96.8 % that far surpassed Fe1‐, Co1‐ and Cu1‐N‐C. Remarkably, the best‐performer, Ni1‐N‐C, even demonstrated excellent CO FE at low CO2 pressures, thereby representing a promising opportunity for the direct use of dilute CO2 feedstock.