Tris(N-pyrrolidinyl)phosphine Substituted Diiron Dithiolate Related to Iron-only Hydrogenase Active Site: Synthesis, Characterization and Electrochemical Properties

侯军; 彭孝军; 周志有; 孙世刚; 赵兴; 高尚

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Tris(N-pyrrolidinyl)phosphine Substituted Diiron Dithiolate Related to Iron-only Hydrogenase Active Site: Synthesis, Characterization and Electrochemical Properties

首发时间：2006-11-13

Hou Jun ¹ Peng Xiaojun ¹ Zhou Zhiyou ² Sun Shigang ² Zhao Xing ¹ Gao Shang ¹

1、Dalian University of Technology
2、Xiamen University

Abstract：A tris(N-pyrrolidinyl)phosphine (P(NC4H8)3) monosubstituted complex, [(μ-pdt)Fe2(CO)5P(NC4H8)3], 2, was synthesized as a functional model of the hydrogen-producing capability of the iron hydrogenase active site. The structure was fully characterized by X-ray crystallography. IR and electrochemical studies have indicated that the (P(NC4H8)3) ligand has better electron-donating ability than that of those phosphine ligands, such as PMe3, PTA ( 1, 3, 5-triaza-7-phosphaadamantane), PMe2Ph PPh3, and P(OEt)3. The electrocatalytic activity of 2 was recorded in CH3CN in the absence and presence of weak acid, HOAc. The cathodic shift of potential at –1.98 V and the dependence of current on acid concentration have indicated that complex 2 can catalyze the reduction of protons to hydrogen at its Fe0FeI level in the presence of HOAc.

keywords： Bioinorganic chemistry, Fe-only hydrogenase, Phosphine ligand

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Tris(N-pyrrolidinyl)phosphine Substituted Diiron Dithiolate Related to Iron-only Hydrogenase Active Site: Synthesis, Characterization and Electrochemical Properties

侯军 ¹ 彭孝军 ¹ 周志有 ² 孙世刚 ² 赵兴 ³ 高尚 ³

1、大连理工大学
2、厦门大学
3、大连理工大学

摘要：A tris(N-pyrrolidinyl)phosphine (P(NC4H8)3) monosubstituted complex, [(μ-pdt)Fe2(CO)5P(NC4H8)3], 2, was synthesized as a functional model of the hydrogen-producing capability of the iron hydrogenase active site. The structure was fully characterized by X-ray crystallography. IR and electrochemical studies have indicated that the (P(NC4H8)3) ligand has better electron-donating ability than that of those phosphine ligands, such as PMe3, PTA ( 1, 3, 5-triaza-7-phosphaadamantane), PMe2Ph PPh3, and P(OEt)3. The electrocatalytic activity of 2 was recorded in CH3CN in the absence and presence of weak acid, HOAc. The cathodic shift of potential at –1.98 V and the dependence of current on acid concentration have indicated that complex 2 can catalyze the reduction of protons to hydrogen at its Fe0FeI level in the presence of HOAc.

关键词： Bioinorganic chemistry, Fe-only hydrogenase, Phosphine ligand

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1. 高等学校博士学科点专项科研基金资助课题（20030141024）

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Hou Jun ,Peng Xiaojun ,Zhou Zhiyou ,et al. Tris(N-pyrrolidinyl)phosphine Substituted Diiron Dithiolate Related to Iron-only Hydrogenase Active Site: Synthesis, Characterization and Electrochemical Properties[EB/OL]. Beijing:Sciencepaper Online[2006-11-13]. https://www.paper.edu.cn/releasepaper/content/200611-318.

No.9499838731163414****

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论文编号	200611-318
论文题目	Tris(N-pyrrolidinyl)phosphine Substituted Diiron Dithiolate Related to Iron-only Hydrogenase Active Site: Synthesis, Characterization and Electrochemical Properties
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