Synthesis, characterization, and electrochemistry of monophosphine-containing diiron propane-1,2-dithiolate complexes related to the active site of [FeFe]-hydrogenases

被引：30

作者：

Lin, Hui-Min ^{[1
]}

Li, Jian-Rong ^{[2
]}

Mu, Chao ^{[3
]}

Li, Ao ^{[3
]}

Liu, Xu-Feng ^{[1
]}

Zhao, Pei-Hua ^{[2
]}

Li, Yu-Long ^{[3
]}

Jiang, Zhong-Qing ^{[4
]}

Wu, Hong-Ke ^{[5
]}

机构：

[1] Ningbo Univ Technol, Sch Mat & Chem Engn, Ningbo 315211, Zhejiang, Peoples R China

[2] North Univ China, Sch Mat Sci & Engn, Taiyuan 030051, Shanxi, Peoples R China

[3] Sichuan Univ Sci & Engn, Coll Chem & Environm Engn, Zigong 643000, Peoples R China

[4] Zhejiang Sci Tech Univ, Dept Phys, Key Lab ATMMT, Minist Educ, Hangzhou 310018, Zhejiang, Peoples R China

[5] Zhejiang Univ Technol, Coll Chem Engn, Hangzhou 310014, Zhejiang, Peoples R China

来源：

APPLIED ORGANOMETALLIC CHEMISTRY | 2019年 / 33卷 / 11期

基金：

中国国家自然科学基金;

关键词：

diiron propane-1; 2-dithiolate; electrochemistry; monophosphine ligand; synthesis; X-ray crystallography; FE-ONLY HYDROGENASE; IRON HYDROGENASE; ELECTROCATALYTIC PROPERTIES; CRYSTAL-STRUCTURES; ELECTRON-TRANSFER; PROTON-REDUCTION; MODEL COMPLEXES; H-CENTER; COORDINATION; LIGANDS;

D O I：

10.1002/aoc.5196

中图分类号：

O69 [应用化学];

学科分类号：

081704 ;

摘要：

Five monophosphine-substituted diiron propane-1,2-dithiolate complexes as the active site models of [FeFe]-hydrogenases have been synthesized and characterized. Reactions of complex [Fe-2(CO)(6){mu-SCH2CH(CH3)S}] (1) with a monophosphine ligand tris(4-methylphenyl)phosphine, diphenyl-2-pyridylphosphine, tris(4-chlorophenyl)phosphine, triphenylphosphine, or tris(4-fluorophenyl)phosphine in the presence of the oxidative agent Me3NO center dot 2H(2)O gave the monophosphine-substituted diiron complexes [Fe-2(CO)(5)(L){mu-SCH2CH(CH3)S}] [L = P(4-C6H4CH3)(3), 2; Ph2P(2-C5H4N), 3; P(4-C6H4Cl)(3), 4; PPh3, 5; P(4-C6H4F)(3), 6] in 81%-94% yields. Complexes 2-6 have been characterized by elemental analysis, spectroscopy, and X-ray crystallography. In addition, electrochemical studies revealed that these complexes can catalyze the reduction of protons to H-2 in the presence of HOAc.

引用

页数：10

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