Citation: Zhao Yingjie, Yu Xin, Hu Huilan, Hu Xinlong, Raje Sakthi, Angamuthu Raja, Tung Chen-Ho, Wang Wenguang. Synthetic[FeFe]-H₂ase models bearing phosphino thioether chelating ligands[J]. Chinese Chemical Letters, ;2018, 29(11): 1651-1655. doi: 10.1016/j.cclet.2018.03.013 shu

Synthetic[FeFe]-H₂ase models bearing phosphino thioether chelating ligands

a.
School of Chemistry and Chemical Engineering, Shandong University, Ji'nan 250100, China
b.
Laboratory of Inorganic Synthesis and Bioinspired Catalysis(LISBIC), Department of Chemistry, Indian Institute of Technology Kanpur, Kanpur 208016, India

Corresponding author: Wang Wenguang, wwg@sdu.edu.cn
Received Date: 16 December 2017
Revised Date: 7 March 2018
Accepted Date: 12 March 2018
Available Online: 14 November 2018

Figures(9)

A series of {2Fe3S} complexes bearing phosphino thioether chelating ligand were synthesized on the basis of Fe₂(Me₂pdt)(1, 2-Cy₂PC₆H₄SMe)(CO)₄ (Me₂pdt=Me₂C(CH₂S^-)₂, 1). The disubstituted Fe(Ⅰ)Fe(Ⅰ) compound 1 exhibits a reversible one-electron redox even for[Fe(Ⅰ)Fe(Ⅱ)]^+/0 couple. Based on the oxidation of 1 to[1]⁺, the tri-substituted[Fe(Ⅰ)Fe(Ⅱ)]⁺ cationic complex[Fe₂(Me₂pdt)(1, 2-Cy₂PC₆H₄SMe) (PPh₃)(CO)₃]⁺ ([2]⁺) was synthesized. Reduction of[2]⁺ provided the neutral tri-substituted Fe(Ⅰ)Fe(Ⅰ) compound 2. The substitution of the CO in 1 ligand by PPh₃ results in an anodic shift of the Fe^ⅡFe^I/Fe_IFe_I couple of 470 mV. Most importantly, this substitution also leads to the Fe-Fe bonds in 1 and 2 with large Lewis basicity difference, i.e. △pK_a^MeCN~10.
- [FeFe]-H₂ases models,
- Mixed-valence Fe(Ⅰ)Fe(Ⅱ),
- Phosphino thioether ligand,
- Diiron bridging hydride,
- Lewis-acid basicity
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Synthetic[FeFe]-H2ase models bearing phosphino thioether chelating ligands

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Synthetic[FeFe]-H₂ase models bearing phosphino thioether chelating ligands