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Electrocatalytic CO 2 Reduction with Re‐Based Spiro Bipyridine Complexes: Effects of the Local Proton in the Second Coordination Sphere †
Author(s) -
Yang Yong,
Zhang Ziyun,
Zhang Zhenyu,
Tang Chao,
Chang Xiaoyong,
Duan Lele
Publication year - 2021
Publication title -
chinese journal of chemistry
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.28
H-Index - 41
eISSN - 1614-7065
pISSN - 1001-604X
DOI - 10.1002/cjoc.202000667
Subject(s) - chemistry , coordination sphere , steric effects , protonation , catalysis , phenol , stereochemistry , bipyridine , medicinal chemistry , proton , crystallography , crystal structure , ion , organic chemistry , physics , quantum mechanics
Main observation and conclusion We report herein a Re‐based tricarbonyl catalyst [ fac ‐Re(L1)(CO) 3 Cl] (Re1) bearing a spiro center and a phenol group as a local proton source in the second coordination sphere. Due to the large steric spiro group, dimerization of one‐electron reduced species was completely eliminated, improving the stability of Re1. Simultaneously, the phenol group in the second coordination sphere improves the formation of an H‐bonding chain that promotes the protonation of CO 2 reduction intermediates, boosting the electrocatalytic CO 2 reduction activity of Re1. Mechanistic studies reveal that the doubly reduced complex Re1b is active for CO 2 addition.