ArticleJournal of the American Chemical Society2013
Hydrogen activation by biomimetic [NiFe]-hydrogenase model containing protected cyanide cofactors.
Article in Journal of the American Chemical Society, 2013. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 15 papers.
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Who cites it
15 citing papers in PubMed.
- Second and Outer Coordination Sphere Effects in Nitrogenase, Hydrogenase, Formate Dehydrogenase, and CO Dehydrogenase.Chemical reviews · 2022Review
- Geometrical influence on the non-biomimetic heterolytic splitting of HChemical science · 2022Article
- Lewis acid protection turns cyanide containing [FeFe]-hydrogenase mimics into proton reduction catalysts.Dalton transactions (Cambridge, England : 2003) · 2022Article
- [NiFe], [FeFe], and [Fe] hydrogenase models from isomers.Science advances · 2020Article
- Crystal structure of NiFe(CO)Acta crystallographica. Section E, Crystallographic communications · 2019Article
- Anion control of tautomeric equilibria: Fe-HChemical science · 2019Article
- Bimetallic nickel-cobalt hydrides in HChemical science · 2019Article
- Frustration across the periodic table: heterolytic cleavage of dihydrogen by metal complexes.Philosophical transactions. Series A, Mathematical, physical, and engineering sciences · 2017Review
- Synthetic Models for Nickel-Iron Hydrogenase Featuring Redox-Active Ligands.Australian journal of chemistry · 2017Article
- Hydrogenase Enzymes and Their Synthetic Models: The Role of Metal Hydrides.Chemical reviews · 2016Review
- Mechanism of H2 Production by Models for the [NiFe]-Hydrogenases: Role of Reduced Hydrides.Journal of the American Chemical Society · 2016Article
- Cyanide-bridged iron complexes as biomimetics of tri-iron arrangements in maturases of the H cluster of the di-iron hydrogenase.Chemical science · 2016Article
- Proteins as templates for complex synthetic metalloclusters: towards biologically programmed heterogeneous catalysis.Proceedings. Mathematical, physical, and engineering sciences · 2016Review
- Models of the Ni-L and Ni-SIa States of the [NiFe]-Hydrogenase Active Site.Inorganic chemistry · 2016Article
- Borane-protected cyanides as surrogates of H-bonded cyanides in [FeFe]-hydrogenase active site models.Inorganic chemistry · 2014Article
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2 authors.
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Abstract
Described are experiments demonstrating incorporation of cyanide cofactors and hydride substrate into [NiFe]-hydrogenase (H2ase) active site models. Complexes of the type (CO)2(CN)2Fe(pdt)Ni(dxpe) (dxpe = dppe, 1; dxpe = dcpe, 2) bind the Lewis acid B(C6F5)3 (BAr(F)3) to give the adducts (CO)2(CNBAr(F)3)2Fe(pdt)Ni(dxpe), (1(BAr(F)3)2, 2(BAr(F)3)2). Upon decarbonylation using amine oxides, these adducts react with H2 to give hydrido derivatives [(CO)(CNBAr(F)3)2Fe(H)(pdt)Ni(dxpe)](-) (dxpe = dppe, [H3(BAr(F)3)2](-); dxpe = dcpe, [H4(BAr(F)3)2](-)). Crystallographic analysis shows that Et4N[H3(BAr(F)3)2] generally resembles the active site of the enzyme in the reduced, hydride-containing states (Ni-C/R). The Fe-H···Ni center is unsymmetrical with r(Fe-H) = 1.51(3) Å and r(Ni-H) = 1.71(3) Å. Both crystallographic and (19)F NMR analyses show that the CNBAr(F)3(-) ligands occupy basal and apical sites. Unlike cationic Ni-Fe hydrides, [H3(BAr(F)3)2](-) and [H4(BAr(F)3)2](-) oxidize at mild potentials, near the Fc(+/0) couple. Electrochemical measurements indicate that in the presence of base, [H3(BAr(F)3)2](-) catalyzes the oxidation of H2. NMR evidence indicates dihydrogen bonding between these anionic hydrides and R3NH(+) salts, which is relevant to the mechanism of hydrogenogenesis. In the case of Et4N[H3(BAr(F)3)2], strong acids such as HCl induce H2 release to give the chloride Et4N[(CO)(CNBAr(F)3)2Fe(Cl)(pdt)Ni(dppe)].
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