The faradaic efficiencies (FE) of 66.15-98.20 % and turnover numbers (TON) of 13.16-35.92 are achieved under the CPE experiments over 18 h periods at β2.00 V vs Fc+/Fc, respectively. The turnover frequencies (TOF) and overpotentials (ο¨) for hydrogen evolution by 1 - 5 (0.25 mM) in DMF are estimated to be 423-894 s-1 and 0.91-1.02 V with 67.32 mM TFA, respectively. The electrochemical behavior and electrocatalytic hydrogen-evolving activity were investigated using trifluoroacetic acid (TFA) as the proton source in combination with cyclic voltammetry (CV) and controlled potential electrolysis (CPE). The crystal structure analysis of 2 and 4οCH2Cl2 indicates the two complexes have almost perfect S2P2 square planar coordination environment defined by the 1,2-diarylethylene-1,2-dithiolate and bis(diphenylphosphine)amine ligands. Stimulated by the structural feature of the -hydrogenases active sites, five new heteroleptic 1,2-bis(p-substitutedphenyl)ethylene-1,2-dithiolate nickel complexes containing N-(p-methoxyphenyl)-bis(diphenylphosphine)-amine ligand, Ni (R = CH3O (1), CH3 (2), H (3), Br (4), and F (5)), were synthesized and characterized.
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