ArticleJournal of the American Chemical Society2009
Nickel-iron dithiolato hydrides relevant to the [NiFe]-hydrogenase active site.
Article in Journal of the American Chemical Society, 2009. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Cited by 34 papers.
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Who cites it
34 citing papers in PubMed.
- NRVS of FeS cluster proteins & models - A bestiary of nifty normal modes.Journal of inorganic biochemistry · 2025Review
- How Geometric Constraints Control the Hydride Position and Activity in [NiFe]-Hydrogenases and Their Biomimetic Complexes.Inorganic chemistry · 2025Article
- Artificial Small Molecules as Cofactors and Biomacromolecular Building Blocks in Synthetic Biology: Design, Synthesis, Applications, and Challenges.Molecules (Basel, Switzerland) · 2023Review
- The Fully Oxidized State of the Glutamate Coordinated OJournal of the American Chemical Society · 2023Article
- Transition Metal Pyrithione Complexes (Ni, Mn, Fe, and Co) as Electrocatalysts for Proton Reduction of Acetic Acid.ACS omega · 2023Article
- Characterization of paramagnetic states in an organometallic nickel hydrogen evolution electrocatalyst.Nature communications · 2023Article
- Size-dependent H and HPhysical chemistry chemical physics : PCCP · 2022Article
- [CrMolecules (Basel, Switzerland) · 2021Article
- Electronic spectroscopy and nanocalorimetry of hydrated magnesium ions [Mg(HFaraday discussions · 2019Article
- Crystal structure of NiFe(CO)Acta crystallographica. Section E, Crystallographic communications · 2019Article
- Electro- and Solar-Driven Fuel Synthesis with First Row Transition Metal Complexes.Chemical reviews · 2019Article
- Synthetic Designs and Structural Investigations of Biomimetic Ni-Fe Thiolates.Inorganic chemistry · 2019Article
- Photochemistry and spectroscopy of small hydrated magnesium clusters MgThe Journal of chemical physics · 2018Article
- In situ formation of molecular Ni-Fe active sites on heteroatom-doped graphene as a heterogeneous electrocatalyst toward oxygen evolution.Science advances · 2018Article
- Interplay of hemilability and redox activity in models of hydrogenase active sites.Proceedings of the National Academy of Sciences of the United States of America · 2017Article
- Synthetic Models for Nickel-Iron Hydrogenase Featuring Redox-Active Ligands.Australian journal of chemistry · 2017Article
- Nickel-centred proton reduction catalysis in a model of [NiFe] hydrogenase.Nature chemistry · 2016Article
- 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
- A strenuous experimental journey searching for spectroscopic evidence of a bridging nickel-iron-hydride in [NiFe] hydrogenase.Journal of synchrotron radiation · 2015Article
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Abstract
The ferrous dithiolato carbonyl Fe(S(2)C(3)H(6))(CO)(2)(dppe) (1) condenses with NiCl(2)(dppe) to give [FeNi(pdt)(mu-Cl)(CO)(dppe)(2)]BF(4) ([2Cl](+)). The corresponding reaction of the ditosylate Ni(OTs)(2)(dppe) gave the dication [(CO)(2)(dppe)Fe(pdt)Ni(dppe)](OTs)(2) ([2(CO)](OTs)(2)) (pdt = 1,3-propanedithiolate; dppe = 1,2-C(2)H(4)(PPh(2))(2); OTs(-) = CH(3)C(6)H(4)-4-SO(3)(-)). Reduction of the bimetallic dicarbonyl with borohydride salts afforded impure, thermally stable hydride, [(CO)(dppe)Fe(pdt)(mu-H)Ni(dppe)](+) ([2H](+)). A reliable route to NiFe(SR)(2)H species entailed protonation of (CO)(3)Fe(pdt)Ni(dppe) to give [(CO)(3)Fe(pdt)(mu-H)Ni(dppe)](+) ([3H](+)). The iron-nickel dithiolato hydride, [3H]BF(4), was characterized crystallographically: as anticipated by biophysical studies, the hydride ligand is bridging, the Fe center is octahedral, and the Ni center is pentacoordinate. Solutions of [3H]BF(4) undergo substitution by dppe to give [2H](+). The hydride undergoes rapid deprotonation and is an electrocatalyst for hydrogen evolution from trifluoroacetic acid. Oxidation of 3 gives a mixed valence species [3](+), a potential model for the Ni-L state.
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