期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 39, 页码 17104-17109出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202007445
关键词
CO(2)reduction; cobalt; electrocatalysis; heterogeneous catalysis; macrocycles
资金
- National Research Foundation (NRF), Prime Minister's Office, Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program
- academic research fund AcRF tier 1, Ministry of Education, Singapore [M4011784 RG6/17, M4012076 RG118/18]
- AME Individual Research Grant, Agency for Science, Technology, and Research (A*STAR), Singapore [A1983c0026]
- College of Engineering, Nanyang Technological University, Singapore [M4081887]
Metal complexes have been widely investigated as promising electrocatalysts for CO(2)reduction. Most of the current research efforts focus mainly on ligands based on pyrrole subunits, and the reported activities are still far from satisfactory. A novel planar and conjugated N-4-macrocyclic cobalt complex (Co(II)CPY) derived from phenanthroline subunits is prepared herein, and it delivers high activity for heterogeneous CO(2)electrocatalysis to CO in aqueous media, and outperforms most of the metal complexes reported so far. At a molar loading of 5.93x10(-8) mol cm(-2), it exhibits a Faradaic efficiency of 96 % and a turnover frequency of 9.59 s(-1)towards CO at -0.70 V vs. RHE. The unraveling of electronic structural features suggests that a synergistic effect between the ligand and cobalt in Co(II)CPY plays a critical role in boosting its activity. As a result, the free energy difference for the formation of *COOH is lower than that with cobalt porphyrin, thus leading to enhanced CO production.
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