The effect of oxidation state of metal on hydrogen production electro-catalyzed by nickel complexes supported by maleonitriledithiolate ligand

Add time:10/01/2019    Source:sciencedirect.com

Two molecular electro-catalysts based on nickel complexes, [Ni(mnt)2]n − (n = 2 (1) and 1 (2)) are formed by the reactions of NiCl2·6H2O, Na2(mnt) and [BzPyN(CH3)2]Br or [4-ClBzPyN(CH3)2]Br (BzPyN(CH3)2 = 1-benzyl-4-(dimethylamino)pyridinium, mnt = 2.2-dicyanoethylene-1.1-dithiolate, and 4-ClBzPyN(CH3)2 = 4-Cl-benzyl-4-dimethylaminopyridinium). Electrochemical investigations show 1 and 2 can electrocatalyze hydrogen generation both from acetic acid and aqueous buffer solution. And complexes 1 and 2 afford a turnover frequency (TOF) of 282.95 and 504.25 mol of hydrogen per mole of catalyst per hour at an overpotential (OP) of 0.848 V from a neutral buffer, respectively, indicating that the nickel(III) complex constitutes the better active catalyst than the nickel(II) species.

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