Synthesis, characterization and catalytic reactivity of pentacoordinate iron dicarbonyl as a model of the [Fe]-hydrogenase active site

doi:10.1016/S1872-2067(15)60920-2

Chinese Journal of Catalysis ›› 2015, Vol. 36 ›› Issue (11): 2011-2019.DOI: 10.1016/S1872-2067(15)60920-2

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Synthesis, characterization and catalytic reactivity of pentacoordinate iron dicarbonyl as a model of the [Fe]-hydrogenase active site

Tianyong Zhang^a,b, Liao Sheng^a, Qiusheng Yang^c, Shuang Jiang^a, Yanhong Wang^a, Chaohui Jin^a, Bin Li^a

a Tianjin Key Laboratory of Applied Catalysis Science and Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
b Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin 300072, China;
c School of Chemical Engineering and Technology, Hebei University of Technology, Tianjin 300130, China

Received:2015-04-16 Revised:2015-05-23 Online:2015-11-02 Published:2015-11-02
Supported by:
This work was supported by the National Natural Science Foundation of China (21103121, 21276187), Tianjin Municipal Natural Science Foundation (13JCQNJC05800) and the Specialized Research Fund for the Doctoral Program of Higher Education (20121317110009).

Abstract

Abstract:

Two mono iron complexes Fe(CO)₂PR₃(NN) (R = Cy (3), Ph (4), NN = o-phenylenediamine dianion ligand, N₂H₂Ph^2-) derived from the ligand substitution of Fe(CO)₃I₂PR₃ by the NN ligand were isolated and structurally characterized by single crystal X-ray diffraction. They have a similar first coordination sphere and oxidation state of the iron center as the [Fe]-hydrogenase active site, and can be a model of it. IR demonstrated that the effect of the NN ligand on the coordinated CO stretching frequencies was due to its excellent electron donating ability. The reversible protonation/deprotonation of the NN ligand was identified by infrared spectroscopy and density functional theory computation. The NN ligand is an effective proton acceptor as the internal base of the cysteine thiolate ligand in [Fe]-hydrogenase. The electrochemical properties of complexes 3, 4 were investigated by cyclic voltammograms. Complex 3 catalyzed the transfer hydrogenation of benzoquinone to hydroquinone effectively under mild conditions.

Key words: Mono iron hydrogenase, Model complex, Catalytic transfer hydrogenation, Functional analogue, Benzoquinone

Tianyong Zhang, Liao Sheng, Qiusheng Yang, Shuang Jiang, Yanhong Wang, Chaohui Jin, Bin Li. Synthesis, characterization and catalytic reactivity of pentacoordinate iron dicarbonyl as a model of the [Fe]-hydrogenase active site[J]. Chinese Journal of Catalysis, 2015, 36(11): 2011-2019.

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Synthesis, characterization and catalytic reactivity of pentacoordinate iron dicarbonyl as a model of the [Fe]-hydrogenase active site

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