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

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....

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Published in:Angewandte Chemie 2020-11, Vol.132 (46), p.20770-20776
Main Authors: Jiao, Long, Yang, Weijie, Wan, Gang, Zhang, Rui, Zheng, Xusheng, Zhou, Hua, Yu, Shu‐Hong, Jiang, Hai‐Long
Format: Article
Language:English
Subjects:
Carbon dioxide
Catalysts
Chemistry
CO2 reduction
Copper
electrocatalysis
Electrocatalysts
Iron
low pressure
Metal-organic frameworks
Metals
Multivariate analysis
Nickel
Selectivity
Single atom catalysts
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Summary: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. A series of porphyrinic multivariate metal–organic frameworks (MTV‐MOFs) were pyrolyzed to generate a range of single‐atom metals implanted in N‐doped carbon (M1‐N‐C; M=Fe, Co, Ni and Cu). The M1‐N‐C model catalysts, with an almost identical carbon support environment, demonstrated different activities toward CO2 electroreduction. The best performer, Ni1‐N‐C, achieved highly selective reduction of CO2 even at low pressures.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.202008787