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

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

1.
a Tianjin Key Laboratory of Applied Catalysis Science and Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;

Corresponding author: Bin Li,
Received Date: 16 April 2015
Available Online: 23 May 2015
Fund Project: 国家自然科学基金(21103121, 21276187) (21103121, 21276187) 天津市自然科学基金(13JCQNJC05800) (13JCQNJC05800) 高等学校博士学科点专项科研基金(20121317110009). (20121317110009)

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.
- Mono iron hydrogenase,
- Model complex,
- Catalytic transfer hydrogenation,
- Functional analogue,
- Benzoquinone
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沈阳化工大学材料科学与工程学院沈阳 110142