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Synthesis, characterization, and crystal structures of N-functionalized diiron azadithiolate complexes related to the active site of [FeFe]-hydrogenases
Ist Teil von
Journal of coordination chemistry, 2011-03, Vol.64 (6), p.1023-1031
Ort / Verlag
Abingdon: Taylor & Francis Group
Erscheinungsjahr
2011
Quelle
Taylor & Francis
Beschreibungen/Notizen
A series of N-functionalized diiron azadithiolate complexes, [(µ-SCH
2
)
2
NCH
2
CO
2
Me]Fe
2
(CO)
5
L [L = CO (1); PPh
3
(2); Ph
2
PCH
2
PPh
2
(3)], as active site models of [FeFe]-hydrogenases has been prepared and characterized. While 1 was prepared by a sequential reaction of (µ-HS)
2
Fe
2
(CO)
6
with two equiv. of aqueous HCHO, followed by treatment of (µ-HOCH
2
S)
2
Fe
2
(CO)
6
with one equiv. of H
2
NCH
2
CO
2
Me in 46% yield; 2 and 3 were prepared by a carbonyl substitution reaction of 1 with PPh
3
or Ph
2
PCH
2
PPh
2
in the presence of Me
3
NO · 2H
2
O in 90% and 85% yields, respectively. The crystal structures of 1 and 2 revealed that the substituent attached to the bridgehead nitrogen occupies an equatorial position and the PPh
3
ligand resides in an axial position of the square pyramid of Fe2.