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Effects of halogen ligands of complexes supported by bis(methylthioether)pyridine on catalytic activities for electrochemical and photochemical driven hydrogen evolution
Reactions of bis(methylthioether)pyridine (btep) with CuX2 (X = Br and Cl) form two new complexes, [Cu(btep)Br-2] and [Cu(btep)Cl-2], respectively, which have been determined by X-ray crystallography. Both of them can serve as catalysts for electrochemical and photochemical driven hydrogen evolution. Under an overpotential (OP) of 837.6 mV, [Cu(btep)Br-2] or [Cu(btep)Cl-2] can electrocatalyze hydrogen evolution from a neutral water with a turnover frequency (TOF) of 373 and 120 mol of hydrogen per mole of catalyst per hour (mol H-2/mol catalyst/h), respectively. Under blue light, mixing with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H(2)A) as a sacrificial electron donor, the photolysis of an aqueous solution (pH 4.5) with [Cu(btep)Br-2] or [Cu(btep)Cl-2] can provide 6180 and 5120 mol of H-2 per mole of catalyst (mol of H-2 (mol of cat)(-1)) during 48-h irradiation with an average apparent quantum yield of 16.7% and 11.0%, respectively. The results show that [Cu(btep)Br-2] shows a more efficient activity for H-2 generation than [Cu(btep)Cl-2]. Several electrochemical and photochemical measurements and analysis are carried out to study catalytic mechanism for H-2 production.
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Reference:
Copper catalysis in organic synthesis – NCBI,
,Special Issue “Fundamentals and Applications of Copper-Based Catalysts”