Facile synthesis and functionality-dependent electrochemistry of Fe-only hydrogenase mimics

Inorganic Chemistry
Gang SiLi-Zhu Wu

Abstract

A series of azadithiolate (adt)-bridged Fe-only hydrogenase model complexes, Fe2(CO)6(mu-adt)C6H4I-4 (1), Fe2(CO)6(mu-adt)C6H4C[triple bond]CR [R = C6H4NO2-4 (2), C6H4CHO-4 (3), C6H4NH2-4 (4), C6H4COOH-4 (5), C6H4COOCH2CH3-4 (6), C6H4F-4 (7), C6H5 (8), C6H4OCH3-4 (9), C6H4N(CH3)2-4 (10)], [Fe2(CO)5(PPh3)(mu-adt)C6H4I-4 (11), and Fe2(CO)5(PPh3)(mu-adt)C6H4C[triple bond]CC6H4NO2-4 (12), have been synthesized in high yields under mild conditions. The linear geometry and rigidity of a triple bond act as an effective bridge to anchor a functionality ranging from electron-donating to electron-accepting, even coordinative groups in the adt model complexes. X-ray crystal analysis of 2, 3, and 6-12 reveals that the model complexes retain the butterfly structure of Fe2S2 model analogues. A rigid phenylacetylene offers excellent control over the distance between the functional group and the active site of Fe2S2 model complexes. The unusual Fe-Fe distance and the angles found in the molecular packing of 6 are originated from the intriguing intermolecular C-H...O and C-H...S interactions. More importantly, electrochemical studies reveal that all of the complexes can catalyze electrochemical reduction of protons to molecular hydrogen, but th...Continue Reading

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Citations

Jun 28, 2011·Chemical Communications : Chem Comm·Hong-Yan WangLi-Zhu Wu
Jun 4, 2016·Chemical Reviews·Yulong Li, Thomas B Rauchfuss
Aug 12, 2009·Journal of Inorganic Biochemistry·Ulf-Peter ApfelWolfgang Weigand
Mar 20, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Laith R AlmazahrehWolfgang Weigand
Jul 14, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Hassan Abul-FutouhWolfgang Weigand
Sep 15, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Ramona KositzkiMichael Haumann
Jun 15, 2010·Chemistry, an Asian Journal·Wen-Guang WangLi-Zhu Wu
Feb 5, 2011·Dalton Transactions : an International Journal of Inorganic Chemistry·Yu-Chiao LiuMing-Hsi Chiang
Apr 1, 2009·Dalton Transactions : an International Journal of Inorganic Chemistry·Wen-Guang WangLi-Zhu Wu
Jan 6, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Wen-Guang WangLi-Zhu Wu
Mar 1, 2011·European Journal of Inorganic Chemistry·Raja AngamuthuThomas B Rauchfuss
Aug 22, 2012·Dalton Transactions : an International Journal of Inorganic Chemistry·Hui-Min WenChang-Neng Chen
Dec 12, 2020·Chemical Society Reviews·Julian T KleinhausUlf-Peter Apfel

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