The effect of oxidation state of metal on electrochemical and photochemical driven hydrogen evolution catalyzed by nickel complexes of maleonitriledithiolate ligands
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Two nickel-based catalysts, TBA<sub>2</sub>[Ni<sup>II</sup>(mnt)<sub>2</sub>] <b>1</b> and TBA[Ni<sup>III</sup>(mnt)<sub>2</sub>] <b>2</b> are formed by the reactions of NiCl<sub>2</sub>·6H<sub>2</sub>O, Na<sub>2</sub>(mnt), and tetra-n-butylammoniumbromide (TBABr) without or with iodine (I<sub>2</sub>) (mnt = 2,2-dicyanoethylene-1,1-dithiolate), respectively. Under an overpotential (OP) of 941.6 mV, complexes <b>1</b> and <b>2</b> can electrocatalyze hydrogen evolution from acetic acid with a turnover frequency (TOF) of 36.3 and 148.31 mol H<sub>2</sub>/mol catalyst/h, respectively. Under blue light (<i>λ</i><sub>max</sub> = 469 nm), <b>1</b> or <b>2</b>, together with CdS nanorods (CdS NRs) as a photosensitizer, and ascorbic acid (H<sub>2</sub>A) as a sacrificial electron donor, can produce hydrogen with a turnover number (TON) of 7760 and 17,570 moles of H<sub>2</sub> per mole of catalyst during 35 h irradiation, respectively. The average value of apparent quantum yield (AQY) is ∼9.2% (complex <b>1</b>) and 28% (complex <b>2</b>), respectively. The results indicate that the nickel(III) complex has a better active activity for hydrogen production than the nickel(II) species.
提供机构：
Taylor & Francis
创建时间：
2020-01-31
