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A Molecular Copper Catalyst for Electrochemical Water Reduction with a Large Hydrogen‐Generation Rate Constant in Aqueous Solution
Author(s) -
Zhang Peili,
Wang Mei,
Yang Yong,
Yao Tianyi,
Sun Licheng
Publication year - 2014
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201408266
Subject(s) - chemistry , aqueous solution , electrochemistry , catalysis , electrolysis , inorganic chemistry , copper , reaction rate constant , ethylenediamine , electrolysis of water , hydrogen , glassy carbon , standard hydrogen electrode , hydrogen production , electrode , reference electrode , kinetics , cyclic voltammetry , organic chemistry , physics , quantum mechanics , electrolyte
Abstract The copper complex [(bztpen)Cu](BF 4 ) 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 ( 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] 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+ .