| 含膦配体二铁二硫五羰基配合物的合成、表征及电催化产氢性能 |
| Synthesis, characterization, and electrocatalytic hydrogen evolution of diiron dithiolato pentacarbonyl complexes bearing phosphine ligand |
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| 摘要: 本文报道了4个含膦配体二铁二硫五羰基配合物的合成和结构表征。起始配合物[Fe2(CO)6(μ-SCH2CH (CH2OOCH) S)](1)与三苯基膦、三环己基膦、三(2-甲氧基苯基)膦或三(4-三氟甲基苯基)膦和脱羰试剂Me3NO·2H2O反应，以59%~88%的产率制备了目标产物[Fe2(CO)5(L)(μ-SCH2CH (CH2OOCH) S)](L=PPh3(2)、PCy3(3)、P (2-C6H4OCH3)3(4)、P (4-C6H4CF3)3(5))。配合物2~5以元素分析、红外光谱、核磁共振以及单晶X射线衍射进行了表征。电化学性质研究表明配合物1~5均可以实现电化学催化质子还原产生氢气的功能，其中配合物1的催化产氢效率明显优于其它配合物。 |
| 关键词: 铁铁氢化酶 双铁配合物 X射线晶体学 产氢催化剂 |
| 基金项目: 浙江省自然科学基金(No.LY19B020002)、钒钛资源综合利用四川省重点实验室项目(No.2021FTSZ07)、化学合成与污染控制四川省重点实验室项目(No.CSPC201904)、四川省人社厅项目和四川轻化工大学项目(No.CX2021055)资助。 |
| Abstract: In this work, four diiron dithiolato pentacarbonyl complexes with phosphine ligands were synthesized and structurally characterized. The starting complex[Fe2(CO)6(μ-SCH2CH(CH2OOCH)S)] (1) reacted with triphenylphosphine, tricyclohexylphosphine, tris(2-methoxyphenyl)phosphine, or tris(4-(trifluoromethyl)phenyl)phosphine and Me3NO·2H2O as the decarbonylation agent to produce the target products[Fe2(CO)5(L)(μ-SCH2CH(CH2OOCH)S)] (L=PPh3 (2), PCy3 (3), P(2-C6H4OCH3)3 (4), P(4-C6H4CF3)3 (5)) in 59%-88% yields. Complexes 2-5 have been characterized by elemental analysis, IR, and NMR spectroscopy, together with single-crystal X-ray diffraction analysis. Electrochemical studies have revealed that complexes 1-5 could electro-catalyze the reduction of proton to hydrogen and complex 1 had better catalytic efficiency than other complexes. |
| Keywords: [FeFe]-hydrogenases diiron complex X-ray crystallography H2 evolving catalyst |
| 投稿时间：2022-12-09 修订日期：2023-05-07 |
| 摘要点击次数: 2003 |
| 全文下载次数: 822 |
| 刘旭锋,徐博,徐航,李玉龙.含膦配体二铁二硫五羰基配合物的合成、表征及电催化产氢性能[J].无机化学学报,2023,39(8):1619-1627. |
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