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Electrocatalytic water oxidation influenced by the ratio between Cu2+ and a multiply branched peptide ligand
Catalysis Communications ( IF 3.7 ) Pub Date : 2019-01-03 , DOI: 10.1016/j.catcom.2019.01.004
Łukasz Szyrwiel , Dávid Lukács , Tetsuya Ishikawa , Justyna Brasun , Łukasz Szczukowski , Zbigniew Szewczuk , Bartosz Setner , József S. Pap

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 (~60 mV) overpotential, increased catalytic current and 4 times as high O2 evolution rate compared to the 2:1 metal-to-ligand stoichiometry.



中文翻译:

Cu 2+与多支肽配体之间的比例影响电催化水氧化

设计了多分支肽H-Gly-Dap(H-Gly)-Dap(H-Gly-Dap(H-Gly))-Gly-NH 2(Dap =  L -2,3-二氨基丙酸)提供在水氧化中具有电催化活性的多Cu 2+中心。每个分支部分充当一个铜离子的结合袋。的UV-vis,CD和EPR光谱学建议{NH 2,N -,N -,NH 2 }当量的前两个位Cu集2+离子,而以不同的模式用于第三,在依次改变的电化学行为复杂的。第三Cu 2+与金属与配体的化学计量比为2:1相比,可在较低的(〜60 mV)过电势下触发水氧化,增加催化电流,并以4倍高的O 2释放速率触发水氧化。

更新日期:2019-01-03
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