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Isolated Diatomic Ni‐Fe Metal–Nitrogen Sites for Synergistic Electroreduction of CO 2
Author(s) -
Ren Wenhao,
Tan Xin,
Yang Wanfeng,
Jia Chen,
Xu Shumao,
Wang Kaixue,
Smith Sean C.,
Zhao Chuan
Publication year - 2019
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201901575
Subject(s) - catalysis , electrocatalyst , faraday efficiency , diatomic molecule , selectivity , chemistry , density functional theory , adsorption , electrolysis , metal , desorption , transition metal , inorganic chemistry , molecule , electrochemistry , computational chemistry , electrode , organic chemistry , electrolyte
Polynary single‐atom structures can combine the advantages of homogeneous and heterogeneous catalysts while providing synergistic functions based on different molecules and their interfaces. However, the fabrication and identification of such an active‐site prototype remain elusive. Here we report isolated diatomic Ni‐Fe sites anchored on nitrogenated carbon as an efficient electrocatalyst for CO 2 reduction. The catalyst exhibits high selectivity with CO Faradaic efficiency above 90 % over a wide potential range from −0.5 to −0.9 V (98 % at −0.7 V), and robust durability, retaining 99 % of its initial selectivity after 30 hours of electrolysis. Density functional theory studies reveal that the neighboring Ni‐Fe centers not only function in synergy to decrease the reaction barrier for the formation of COOH* and desorption of CO, but also undergo distinct structural evolution into a CO‐adsorbed moiety upon CO 2 uptake.