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              <p>Dedicated in memory of Prof. Constantin Turta for his outstanding contribution to inorganic and coordination chemistry Abstract: We report herein on of the synthesis and characterization of a new mononuclear nickel complex NiL based on a thiosemicarbazone ligand that exhibits an electrocatalytic behavior for H2 evolution in DMF using trifluoroacetic acid (TFA) as the proton source. A maximum turnover frequency (TOFmax) 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.</p>
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