Electrocatalytic water oxidation influenced by the ratio between Cu2+and a multiply branched peptide ligand

被引:7
作者
Szyrwiel, Lukasz [1 ,2 ]
Lukacs, David [3 ]
Ishikawa, Tetsuya [2 ]
Brasun, Justyna [4 ]
Szczukowski, Lukasz [5 ]
Szewczuk, Zbigniew [6 ]
Setner, Bartosz [6 ]
Pap, Jozsef S. [3 ]
机构
[1] European Xray Free Electron Laser Facil GmbH, D-22869 Schenefeld, Germany
[2] European XFEL GmbH, Holzkoppel 4, D-22869 Schenefeld, Germany
[3] MTA Ctr Energy Res, Surface Chem & Catalysis Dept, 29-33,Konkoly Thege Str, H-1121 Budapest, Hungary
[4] Wroclaw Med Univ, Dept Inorgan Chem, Borowska 211a, PL-50552 Wroclaw, Poland
[5] Wroclaw Med Univ, Dept Chem Drugs, Borowska 211a, PL-50552 Wroclaw, Poland
[6] Univ Wroclaw, Fac Chem, F Joliot Curie 14, PL-50383 Wroclaw, Poland
关键词
Copper; Water oxidation; Peptide; Branched peptide; MOLECULAR CATALYSTS; COPPER(II) COMPLEX; BINDING;
D O I
10.1016/j.catcom.2019.01.004
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A multiply branched peptide, H-Gly-Dap(H-Gly)-Dap(H-Gly-Dap(H-Gly))-Gly-NH2 (Dap = L-2,3-diaminopropionic acid) has been designed to furnish multi-Cu2+ centers exhibiting electrocatalytic activity in water oxidation. Each branching moiety serves as binding pocket for one cupric ion. UV-vis, CD and EPR spectroscopy suggest {NH2,N-,N-,NH2}(eq), set for the first two coordinated Cu2+ ions, whereas a different mode for the third that in turn changes the electrochemical behavior of the complex. This third Cu2+ triggers water oxidation at lower (similar to 60 my) overpotential, increased catalytic current and 4 times as high O-2 evolution rate compared to the 2:1 metal-to-ligand stoichiometry.
引用
收藏
页码:5 / 9
页数:5
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