State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), 116024 Dalian (China).
Angew Chem Int Ed Engl. 2014 Dec 8;53(50):13803-7. doi: 10.1002/anie.201408266. Epub 2014 Oct 14.
The copper complex (bztpen)Cu2 (bztpen=N-benzyl-N,N',N'-tris(pyridin-2-ylmethyl)ethylenediamine) displays high catalytic activity for electrochemical proton reduction in acidic aqueous solutions, with a calculated hydrogen-generation rate constant (k(obs)) of over 10000 s(-1). A turnover frequency (TOF) of 7000 h(-1) cm(-2) and a Faradaic efficiency of 96% were obtained from a controlled potential electrolysis (CPE) experiment with (bztpen)Cu in pH 2.5 buffer solution at -0.90 V versus the standard hydrogen electrode (SHE) over two hours using a glassy carbon electrode. A mechanism involving two proton-coupled reduction steps was proposed for the dihydrogen generation reaction catalyzed by (bztpen)Cu.
铜配合物(bztpen)Cu2（bztpen=N-苄基-N,N',N'-三(吡啶-2-基甲基)乙二胺）在酸性水溶液中对电化学质子还原具有高催化活性，其计算得到的氢生成速率常数（k(obs)）超过 10000 s(-1)。通过在 pH 2.5 缓冲溶液中使用玻璃碳电极在 -0.90 V 相对于标准氢电极（SHE）进行两小时的控制电位电解（CPE）实验，从(bztpen)Cu中获得了 7000 h(-1) cm(-2)的转换频率（TOF）和 96%的法拉第效率。提出了一种涉及两个质子耦合还原步骤的机制，用于(bztpen)Cu催化的氢气生成反应。
