首页|含膦胺配体的1,2-二芳基乙烯-1,2-二硫醇镍配合物的合成、结构表征与电催化制氢性能

含膦胺配体的1,2-二芳基乙烯-1,2-二硫醇镍配合物的合成、结构表征与电催化制氢性能

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合成了10种含膦胺配体的1,2-二芳基乙烯1,2-二硫醇的镍配合物[(p-XC6H4N(PPh2)2)Ni(S2C2(C6H4Y-p)2)](1:X=Br,Y=CH3O;2:X=Br,Y=CH3;3:X=Br,Y=H;4:X=Br,Y=Br;5:X=Br,Y=F;6:X=F,Y=CH3O;7:X=F,Y=CH 3;8:X=F,Y=H;9:X=F,Y=Br;10:X=F,Y=F),通过元素分析、核磁共振谱、红外光谱和紫外-可见吸收光谱对镍配合物的结构进行了表征.配合物1·DMF的X-射线单晶衍射分析表明镍原子处于近乎完美的四方平面构型的S2P2配位环境中,通过循环伏安法测定了配合物在DMF溶液中的电化学性质以及在三氟乙酸(TFA)存在时的电催化制氢性能.研究结果表明:0.25 mmol配合物1-10在添加67.317 mM TFA时,其电催化制氢的转换频率和过电位分别为299.3～809.7 s-1和0.867～0.995 V.
Synthesis,structural characterization and properties of the electrocatalyticly prepared hydrogen of 1,2-diarylethylene-1,2-dithiolate nickel complexes with bis(diphenylphosphanyl)amine ligand
Ten nickel complexes bearing 1,2-diarylethylene-1,2-dithiolate and bis(diphenylphosphanyl)amine ligands,[(p-XC6H4N(PPh2)2)Ni(S2C2(C6H4Y-p)2)](1:X=Br,Y=CH3O;2:X=Br,Y=CH3;3:X=Br,Y=H;4:X=Br,Y=Br;5:X=Br,Y=F;6:X=F,Y=CH3O;7:X=F,Y=CH3;8:X=F,Y=H;9:X=F,Y=Br;10:X=F,Y=F),were synthesized and characterized by elemental analysis,nuclear magnetic resonance spectroscopies,infrared spectra,and ul-traviolet-visible absorption spectroscopies.The X-ray single crystal diffraction analysis of 1·DMF showed that the nickel atom is located in the S2 P2 coordination environment with an almost perfectly square planar.The electrochemical properties of the complexes in DMF solution and the electrocatalytic hydrogen evolution performance in the presence of trifluoroacetic acid(TFA)were determined by cyclic voltammetry.The research results indicated that the conversion frequencies and overpoten-tials of the electrocatalytic hydrogen evolution for 0.25 mmol complexes 1-10 in the presence of 67.317 mM TFA are 299.3-809.7 mmol-1and 0.867-0.995V,respectively.

bis(diphenylphosphanyl)amine1,2-diarylethylene-1,2-dithiolatenickel complexsynthesiselectrocatalyt-ic hydrogen evolution

纪润武、何毅、姚博馨、刘梦南、何佳钰、赵文怀、谢斌

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四川轻化工大学材料科学与工程学院, 四川 自贡 643000

四川轻化工大学化学与环境工程学院, 四川 自贡 643000

四川轻化工大学材料腐蚀与防护四川省重点实验室,四川 自贡 643000

膦胺 1,2-二芳基乙烯-1,2-二硫醇 镍配合物 合成 电催化制氢

四川省科技厅项目化学合成与污染控制四川省重点实验室项目四川轻化工大学研究生创新基金四川轻化工大学大学生创新创业训练计划

2023NSFSC0087CSPC202201y2020076CX2023007

2024

10.13603/j.cnki.51-1621/z.2024.04.012

内江师范学院学报
内江师范学院

内江师范学院学报

影响因子：0.299
ISSN：1671-1785
年,卷(期)：2024.39(4)
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