Electrocatalytic CO2 Reduction with Re-Based Spiro Bipyridine Complexes:Effects of the Local Proton in the Second Coordination Sphere

• 作者: Yong Yang Ziyun Zhang Zhenyu Zhang Chao Tang Xiaoyong Chang Lele Duan
• 来源期刊: 中国化学（英文版）
• 年，卷（期）: 2021,（5）
• 所属期刊栏目: Concise Reports
• 页码范围: 1281-1287
• 页数: 7页
• 语种: 英文
• DOI: 10.1002/cjoc.202000667

摘要

Main observation and conclusion We report herein a Re-based tricarbonyl catalyst [fac-Re(L1)(CO)3Cl] (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 com-pletely 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 CO2 reduction intermediates,boosting the electrocatalytic CO2 reduction activity of Re1.Mechanistic studies reveal that the doubly reduced complex Re1b is active for CO2 addition.