期刊
CHEMCATCHEM
卷 9, 期 12, 页码 2262-2268出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.201600967
关键词
bioinorganic chemistry; electrochemistry; hydrogen; ligand effects; nickel
资金
- CNRS
- Academy of Sciences of Moldova [EDC25722]
- French National Research Agency (Labex program, ARCANE) [ANR-11-LABX-0003-01]
- COST Actions [CM1305, CM1202]
We report herein the synthesis and characterization of a new mononuclear nickel complex based on a thiosemicarbazone ligand that exhibits an electrocatalytic behavior for H-2 evolution in DMF using trifluoroacetic acid (TFA) as the proton source. Catalysis is observed at quite small overpotential values and a maximum turnover frequency (TOFmax) of 3080 s(-1) was extrapolated for 1M proton concentration using the foot-of-the wave analysis of cyclic voltammetry data. Gas analysis during controlled potential electrolysis experiments confirmed the catalytic nature of the process and production of dihydrogen with 80% faradaic yield. Quantum chemical calculations indicate that the catalytic mechanism involves first ligand-based reduction and protonation steps followed by metal-centered processes.
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