Fe-S complexes containing five-membered heterocycles: novel models for the active site of hydrogenases with unusual low reduction potential.
Three biomimetic 2Fe2S complexes [{(micro-SCH2)2NCH2(2-C4H3O)}](Fe2(CO)6), [{(micro-SCH2)2 NCH2(2-C4H3S)}](Fe2(CO)6) and [{(micro-SCH2)2NCH2(5-Br-2-C4H2S)}Fe2(CO)6] were prepared as models for the active site of Fe-only hydrogenase by the convergent process from [(micro-S2)Fe2(CO)6] and N,N-bis(hydromethyl)-2-furan and thiophene. The structures of these complexes were identified spectroscopically and crystallographically. The electrochemical behavior of the complexes and was unique as they showed catalytic proton reduction with a low reduction potential at -1.13 and -1.09 V vs Fc/Fc+, respectively, in the presence of HClO4.
Jiang
Shi
S
State Key Laboratory of Fine Chemicals, DUT-KTH Joint Education and Research Center on Molecular Devices, Dalian University of Technology (DUT), Zhongshan Road 158-40, Dalian, 116012, P. R. China.
Liu
Jianhui
J
Shi
Yu
Y
Wang
Zhen
Z
Akermark
Björn
B
Sun
Licheng
L
D001665:Binding Sites; D004563:Electrochemistry; D005296:Ferrous Compounds / Q000138:chemical synthesis / Q000737:chemistry*; D006864:Hydrogenase / Q000737:chemistry*; D007506:Iron-Sulfur Proteins / Q000737:chemistry*; D008958:Models, Molecular; D015394:Molecular Structure; D010084:Oxidation-Reduction; D011522:Protons
D005296:Ferrous Compounds; D007506:Iron-Sulfur Proteins; D011522:Protons; C118830:iron hydrogenase; D006864:Hydrogenase