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一种具有五齿胺-吡啶配体的水溶性铜配合物的电催化水氧化反应。

Electrocatalytic water oxidation by a water-soluble copper complex with a pentadentate amine-pyridine ligand.

作者信息

Xu Ziyi, Zheng Zilin, Chen Qi, Wang Jiayi, Yu Kaishan, Xia Xin, Shen Junyu, Zhang Qijian

机构信息

Jiangsu Laboratory of Advanced Functional Materials, School of Materials Engineering, Changshu Institute of Technology, Changshu 215500, P. R. China.

出版信息

Dalton Trans. 2021 Aug 21;50(31):10888-10895. doi: 10.1039/d1dt01821c. Epub 2021 Jul 26.

DOI:10.1039/d1dt01821c
PMID:34308951
Abstract

A water-soluble copper complex with a diamine-tripyridine ligand was synthesized successfully and well characterized. It was found to be catalytically active for the water oxidation reaction under basic conditions. Based on the electrochemical test result, this copper complex displayed an apparent rate constant (k) of 0.81 s for the oxygen evolution reaction in 0.1 M phosphate buffer solution at pH 11.0. More importantly, the copper complex remained stable over 3 h of a bulk electrolysis experiment at 1.60 V with a Faradaic efficiency of 90.7% for O evolution, and the decrement of current density was only 1.9%. These results suggest that the pentadentate copper complex is an efficient and durable homogeneous Earth-abundant electrocatalyst for water oxidation.

摘要

成功合成了一种具有二胺-三吡啶配体的水溶性铜配合物,并对其进行了充分表征。发现该配合物在碱性条件下对水氧化反应具有催化活性。根据电化学测试结果,在pH为11.0的0.1 M磷酸盐缓冲溶液中,该铜配合物对析氧反应的表观速率常数(k)为0.81 s⁻¹。更重要的是,在1.60 V下进行3 h的本体电解实验时,该铜配合物保持稳定,析氧法拉第效率为90.7%,电流密度仅下降1.9%。这些结果表明,五齿铜配合物是一种高效且耐用的地球丰富型均相水氧化电催化剂。

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Inorg Chem. 2023 Apr 10;62(14):5303-5314. doi: 10.1021/acs.inorgchem.3c00477. Epub 2023 Mar 29.
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Theoretical study on the mechanism of water oxidation catalyzed by a mononuclear copper complex: important roles of a redox non-innocent ligand and HPO anion.单核铜配合物催化水氧化机理的理论研究:氧化还原非无辜配体和HPO阴离子的重要作用
RSC Adv. 2023 Mar 14;13(12):8352-8359. doi: 10.1039/d3ra00648d. eCollection 2023 Mar 8.