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A Thiosemicarbazone–Nickel(II) Complex as Efficient Electrocatalyst for Hydrogen Evolution
Author(s) -
Straistari Tatiana,
Fize Jennifer,
Shova Sergiu,
Réglier Marius,
Artero Vincent,
Orio Maylis
Publication year - 2017
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201600967
Subject(s) - electrocatalyst , overpotential , catalysis , nickel , chemistry , protonation , cyclic voltammetry , faraday efficiency , inorganic chemistry , ligand (biochemistry) , electrolysis , trifluoroacetic acid , voltammetry , yield (engineering) , materials science , organic chemistry , electrolyte , electrochemistry , ion , biochemistry , receptor , electrode , metallurgy
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 (TOF max ) of 3080 s −1 was extrapolated for 1 m 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.