A Molecular Copper Catalyst for Electrochemical Water Reduction with a Large Hydrogen-Generation Rate Constant in Aqueous Solution.

Angewandte Chemie (International ed. in English)

PubMedID: 25314646

Zhang P, Wang M, Yang Y, Yao T, Sun L. A Molecular Copper Catalyst for Electrochemical Water Reduction with a Large Hydrogen-Generation Rate Constant in Aqueous Solution. Angew Chem Int Ed Engl. 2014;.
The copper complex [(bztpen)Cu](BF4 )2 (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 (kobs ) 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](2+) 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](2+) .