Role of the azadithiolate cofactor in models for [FeFe]-hydrogenase: novel structures and catalytic implications.
作者： Matthew T. Olsen , Thomas B. Rauchfuss , Scott R. Wilson
DOI: 10.1021/JA103998V
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摘要: This paper summarizes studies on the redox behavior of synthetic models for [FeFe]-hydrogenases, consisting diiron dithiolato carbonyl complexes bearing amine cofactor and its N-benzyl derivative. Of specific interest are causes low reactivity oxidized toward H2, which contrasts with high activity these enzymes H2 oxidation. The acid−base properties model [Fe2[(SCH2)2NR](CO)3(dppv)(PMe3)]+ ([2]+ R = H [2′]+ CH2C6H5, dppv cis-1,2-bis(diphenylphosphino)ethylene)) indicate that addition followed by deprotonation (i) endothermic mixed valence (FeIIFeI) state (ii) exothermic diferrous (FeIIFeII) state. is shown to be unstable respect coordination Fe, a derivative was characterized crystallographically. differ strongly those containing versus derived f...
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