高金索

(高级工程师)

 硕士生导师
学位:博士
性别:男
毕业院校:中国科学院大连化学物理研究所
所在单位:环境学院
电子邮箱:jsgao@dlut.edu.cn

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Improvement of Electrochemical Water Oxidation by Fine-Tuning the Structure of Tetradentate N-4 Ligands of Molecular Copper Catalysts

发表时间:2019-03-11 点击次数:

论文名称:Improvement of Electrochemical Water Oxidation by Fine-Tuning the Structure of Tetradentate N-4 Ligands of Molecular Copper Catalysts
论文类型:期刊论文
第一作者:Shen, Junyu
通讯作者:Wang, M (reprint author), Dalian Univ Technol, DUT KTH Joint Educ & Res Ctr Mol Devices, State Key Lab Fine Chem, Dalian 116024, Peoples R China.
合写作者:Wang, Mei,Gao, Jinsuo,Han, Hongxian,Liu, Hong,Sun, Licheng
发表刊物:CHEMSUSCHEM
收录刊物:SCIE、EI、PubMed、Scopus
卷号:10
期号:22,SI
页面范围:4581-4588
ISSN号:1864-5631
关键字:copper; electrocatalysis; homogeneous catalysis; N ligands; water oxidation
摘要:Two copper complexes, [(L1)Cu(OH2)](BF4)(2) [1; L1 = N,N'-dimethyl-N,N'-bis(pyridin-2-ylmethyl)-1,2-diaminoethane] and [(L2)Cu(OH2)](BF4)(2) [2, L2 = 2,7-bis(2-pyridyl)-3,6-diaza-2,6-octadiene], were prepared as molecular water oxidation catalysts. Complex 1 displayed an overpotential (eta) of 1.07V at 1 mAcm(-2) and an observed rate constant (k(obs)) of 13.5 s(-1) at eta 1.0 V in pH 9.0 phosphate buffer solution, whereas 2 exhibited a significantly smaller eta (0.70 V) to reach 1 mAcm(-2) and a higher k(obs) (50.4 s(-1)) than 1 under identical test conditions. Additionally, 2 displayed better stability than 1 in controlled potential electrolysis experiments with a faradaic efficiency of 94% for O-2 evolution at 1.58 V, when a casing tube was used for the Pt cathode. A possible mechanism for 1- and 2-catalyzed O-2 evolution reactions is discussed based on the experimental evidence. These comparative results indicate that fine-tuning the structures of tetradentate N-4 ligands can bring about significant change in the performance of copper complexes for electrochemical water oxidation.
发表时间:2017-11-23