A Thiosemicarbazone-Nickel(II) Complex as Efficient Electrocatalyst for Hydrogen Evolution

Tatiana Straistari (1) , Jennifer Fize (2) , Sergiu Shova (3) , Marius Réglier (1) , Vincent Artero (2) , Maylis Orio (1)

1 ISM2 - Institut des Sciences Moléculaires de Marseille
2 LCBM - UMR 5249 - Laboratoire de Chimie et Biologie des Métaux
3 Institute of Applied Physics, Academy of Sciences of Moldova

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.

Domaines: Chimie

Tatiana Straistari, Jennifer Fize, Sergiu Shova, Marius Réglier, Vincent Artero, et al.. A Thiosemicarbazone-Nickel(II) Complex as Efficient Electrocatalyst for Hydrogen Evolution. ChemCatChem, 2017, ⟨10.1002/cctc.201600967⟩. ⟨hal-02191296⟩