Synthesis, structures and electrochemical properties of nitro- and amino-functionalized diiron azadithiolates as active site models of Fe-only hydrogenases

QC 20100525
Complex [{(mu-SCH2)(2)N(4-NO2C6H4)}Fe-2(CO)(6)] (4) was prepared by the reaction of the dianionic intermediate [(mu-S)(2)Fe-2(CO)(6)](2-) and N,N-bis(chloromethyl)-4-nitroaniline as a biomimetic model of the active site of Fe-only hydrogenase. The reduction of 4 by Pd-C/H-2 under a neutral condition afforded complex [{(mu-SCH2)(2)N(4-NH2C6H4)}Fe-2(CO)(6)] (5) in 67% yield. Both complexes were characterized by IR, H-1 and C-13 NMR spectroscopy and MS spectrometry. The molecular structure of 4, as determined by X-ray analysis, has a butterfly 2Fe2S core and the aryl group on the bridged-N atom slants to the Fe(2) site. Cyclic voltammograms of 4 and 5 were studied to evaluate their redox properties. It was found that complex 4 catalyzed electrochemical proton reduction in the presence of acetic acid. A plausible mechanism of the electrocatalytic proton reduction is discussed.

Ingår i:Chemistry - A European Journal: Wiley10:18, s. 4474-44790947-65391521-3765

Av författaren/redakt...: Liu, T. B.; Wang, M.; Shi, Z.; Cui, H. G.; Dong, W. B.; Chen, J. S.; visa fler...; Akermark, B.; Sun, Licheng C.; visa färre...

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