期刊
CHEMSUSCHEM
卷 13, 期 12, 页码 3277-3282出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cssc.202000153
关键词
electrocatalysis; ligand effects; nickel; O-O bond formation; water oxidation
资金
- Fundamental Research Funds for the Central Universities [DUT19LK44]
- Natural Science Foundation of Liaoning Province [2019-MS-051]
- National Natural Science Foundation of China [21403028]
- National Basic Research Program of China (973 program) [2014CB239402]
- Swedish Research Council [2017-00935]
- Swedish Energy Agency
- K & A Wallenberg Foundation
Water oxidation is the bottleneck reaction in artificial photosynthesis. Exploring highly active and stable molecular water oxidation catalysts (WOCs) is still a great challenge. In this study, a water-soluble Ni-II complex bearing a redox non-innocent tetraamido macrocyclic ligand (TAML) is found to be an efficient electrocatalyst for water oxidation in neutral potassium phosphate buffer. Controlled-potential electrolysis experiments show that it can sustain at a steady current of approximately 0.2 mA cm(-2) for >7 h at 1.75 V versus normal hydrogen electrode (NHE) without the formation of NiOx. Electrochemical and spectroelectrochemical tests show that the redox-active ligand, as well as HPO42- in the buffer, participate in the catalytic cycle. More importantly, catalytically active intermediate [Ni-III(TAML(2-))-O-.] is formed via several proton-coupled electron transfer processes and reacts with H2O with the assistance of base to release molecular oxygen. Thus, the employment of redox non-innocent ligands is a useful strategy for designing effective molecular WOCs.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据