ArticleProceedings of the National Academy of Sciences of the United States of America2008
Thiolate-bridged dinuclear iron(tris-carbonyl)-nickel complexes relevant to the active site of [NiFe] hydrogenase.
Article in Proceedings of the National Academy of Sciences of the United States of America, 2008. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 10 papers.
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10 citing papers in PubMed, 69 citations in OpenAlex.
- Crystal structure of bis-(tetra-methyl-thio-urea-κActa crystallographica. Section E, Crystallographic communications · 2020Article
- Influence of Benzannulation on Metal Coordination Geometries: Synthesis and Structural Characterization ofJournal of molecular structure · 2015Article
- Ferrous Carbonyl Dithiolates as Precursors to FeFe, FeCo, and FeMn Carbonyl Dithiolates.Organometallics · 2014Article
- Hydride-containing models for the active site of the nickel-iron hydrogenases.Journal of the American Chemical Society · 2010Article
- Artificial hydrogenases.Current opinion in biotechnology · 2010Article
- A model for the CO-inhibited form of [NiFe] hydrogenase: synthesis of CO3Fe(micro-StBu)3Ni{SC6H3-2,6-(mesityl)2} and reversible CO addition at the Ni site.Proceedings of the National Academy of Sciences of the United States of America · 2010Article
- Nickel-iron dithiolato hydrides relevant to the [NiFe]-hydrogenase active site.Journal of the American Chemical Society · 2009Article
- Coordination chemistry of [HFe(CN)(2)(CO)(3)](-) and its derivatives: toward a model for the iron subsite of the [NiFe]-hydrogenases.Inorganic chemistry · 2009Article
- Biomimetic chemistry of iron, nickel, molybdenum, and tungsten in sulfur-ligated protein sites.Biochemistry · 2009Article
- Small molecule mimics of hydrogenases: hydrides and redox.Chemical Society reviews · 2009Review
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7 authors at 1 institution in 1 country.
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Abstract
The reaction of NiBr(2)(EtOH)(4) with a 1:2-3 mixture of FeBr(2)(CO)(4) and Na(SPh) generated a linear trinuclear Fe-Ni-Fe cluster (CO)(3)Fe(mu-SPh)(3)Ni(mu-SPh)(3)Fe(CO)(3), 1, whereas the analogous reaction system FeBr(2)(CO)(4)/Na(S(t)Bu)/NiBr(2)(EtOH)(4) (1:2-3:1) gave rise to a linear tetranuclear Fe-Ni-Ni-Fe cluster [(CO)(3)Fe(mu-S(t)Bu)(3)Ni(mu-Br)](2), 2. By using this tetranuclear cluster 2 as the precursor, we have developed a new synthetic route to a series of thiolate-bridged dinuclear Fe(CO)(3)-Ni complexes, the structures of which mimic [NiFe] hydrogenase active sites. The reactions of 2 with SC(NMe(2))(2) (tmtu), Na{S(CH(2))(2)SMe} and ortho-NaS(C(6)H(4))SR (R = Me, (t)Bu) led to isolation of (CO)(3)Fe(mu-S(t)Bu)(3)NiBr(tmtu), 3, (CO)(3)Fe(S(t)Bu)(mu-S(t)Bu)(2)Ni{S(CH(2))(2)SMe}, 4, and (CO)(3)Fe(S(t)Bu)(mu-S(t)Bu)(2)Ni{S(C(6)H(4))SR}, 5a (R = Me) and 5b (R = (t)Bu), respectively. On the other hand, treatment of 2 with 2-methylthio-phenolate (ortho-O(C(6)H(4))SMe) in methanol resulted in (CO)(3)Fe(mu-S(t)Bu)(3)Ni(MeOH){O(C(6)H(4))SMe}, 6a. The methanol molecule bound to Ni is labile and is readily released under reduced pressure to afford (CO)(3)Fe(S(t)Bu)(mu-S(t)Bu)(2)Ni{O(C(6)H(4))SMe}, 6b, and the coordination geometry of nickel changes from octahedral to square planar. Likewise, the reaction of 2 with NaOAc in methanol followed by crystallization from THF gave (CO)(3)Fe(mu-S(t)Bu)(3)Ni(THF)(OAc), 7. The dinuclear complexes, 3-7, are thermally unstable, and a key to their successful isolation is to carry out the reactions and manipulations at -40 degrees C.
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