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Published in 2024 at "Applied Organometallic Chemistry"
DOI: 10.1002/aoc.7608
Abstract: In an effort to better probe the structure–function relationship on the biological [Fe4S4] cluster of [FeFe]‐hydrogenases, a new library of tertiary phosphine‐supported diiron dithiolate complexes [Fe2(μ‐adtNR)(CO)5{P(C6H4X)3}] (1–3) with various substituents (X = F vs. H vs. Me),…
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Keywords:
phosphine supported;
tertiary phosphine;
fefe hydrogenases;
diiron model ... See more keywords
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Published in 2020 at "International Journal of Hydrogen Energy"
DOI: 10.1016/j.ijhydene.2019.11.206
Abstract: Abstract [FeFe]-hydrogenases efficiently catalyze the hydrogen evolution reactions (HERs) at rates of up to 104 s−1 with low overpotentials in aqueous media. Although the small-molecule diiron mimetics of the active site of [FeFe]-hydrogenases have been…
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Keywords:
fefe hydrogenases;
systems inspired;
water soluble;
soluble systems ... See more keywords
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Published in 2024 at "Accounts of Chemical Research"
DOI: 10.1021/acs.accounts.4c00231
Abstract: Conspectus Nature’s prototypical hydrogen-forming catalysts—hydrogenases—have attracted much attention because they catalyze hydrogen evolution at near zero overpotential and ambient conditions. Beyond any possible applications in the energy sphere, the hydrogenases feature complicated active sites, which…
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Keywords:
fefe hydrogenases;
cluster;
biosynthesis;
synthesis ... See more keywords
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Published in 2025 at "Inorganic chemistry"
DOI: 10.1021/acs.inorgchem.5c03496
Abstract: This paper discusses diiron complexes implicated as intermediates in the biosynthesis of the [2Fe]H site of the [FeFe]-hydrogenases. These complexes include [Fe2(μ-SH)(μ-SR)(CN)2(CO)4]2- (R = H, CH2NH2 [2H,R]2-), which are available from the new precursor [Fe2(μ-S2)(CN)2(CO)4]2-…
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Keywords:
fe2;
fe2 fe2;
fefe hydrogenases;
2fe site ... See more keywords
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Published in 2024 at "Journal of the American Chemical Society"
DOI: 10.1021/jacs.4c01635
Abstract: The active site cofactor of [FeFe]-hydrogenases consists of a cubane [4Fe-4S]-cluster and a unique [2Fe-2S]-cluster, harboring unusual CO- and CN--ligands. The biosynthesis of the [2Fe-2S]-cluster requires three dedicated maturation enzymes called HydG, HydE and HydF.…
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Keywords:
fefe hydrogenases;
cluster;
2fe precursor;
site ... See more keywords
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Published in 2019 at "Journal of the American Chemical Society"
DOI: 10.1021/jacs.8b13084
Abstract: After remaining elusive for many years, terminal hydride states have now been identified in several native and mutant [FeFe]-hydrogenases. In this Perspective, hydride states of [FeFe]-hydrogenases are considered on the basis of hydricity, a thermodynamic…
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Keywords:
hydride;
fefe hydrogenases;
hydricity;
thermodynamic hydricity ... See more keywords
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Published in 2020 at "Journal of the American Chemical Society"
DOI: 10.1021/jacs.9b13075
Abstract: [FeFe] hydrogenases are highly efficient catalysts for reversible dihydrogen evolution. H2 turnover involves different catalytic intermediates including a recently characterized hydride state of the active site (H-cluster). Applying cryogenic infrared and electron paramagnetic resonance spectroscopy…
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Keywords:
electron dynamics;
fefe hydrogenases;
electron;
proton electron ... See more keywords
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1
Published in 2017 at "Nature Communications"
DOI: 10.1038/ncomms16115
Abstract: H2 turnover at the [FeFe]-hydrogenase cofactor (H-cluster) is assumed to follow a reversible heterolytic mechanism, first yielding a proton and a hydrido-species which again is double-oxidized to release another proton. Three of the four presumed…
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Keywords:
state;
fefe hydrogenases;
hydride state;
state catalytic ... See more keywords
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Published in 2018 at "Nature Catalysis"
DOI: 10.1038/s41929-018-0137-y
Abstract: Hydrogenases are appealing catalysts for fuel cells, as these highly efficient H2-oxidation enzymes do not contain expensive precious metals and operate under very mild and safe conditions. Unfortunately, [FeFe] hydrogenases — the most active class…
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Keywords:
fuel cells;
coordination;
fefe hydrogenases;
air ... See more keywords
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Published in 2023 at "Chemical Science"
DOI: 10.1039/d2sc06098a
Abstract: [FeFe] hydrogenases are highly efficient metalloenyzmes for hydrogen conversion. Their active site cofactor (the H-cluster) is composed of a canonical [4Fe-4S] cluster ([4Fe-4S]H) linked to a unique organometallic di-iron subcluster ([2Fe]H). In [2Fe]H the two…
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Keywords:
new active;
binding exogenous;
site states;
active site ... See more keywords
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Published in 2018 at "Nature Communications"
DOI: 10.2210/pdb6gm1/pdb
Abstract: The unmatched catalytic turnover rates of [FeFe]-hydrogenases require an exceptionally efficient proton-transfer (PT) pathway to shuttle protons as substrates or products between bulk water and catalytic center. For clostridial [FeFe]-hydrogenase CpI such a pathway has…
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Keywords:
fefe hydrogenases;
proton;
proton transfer;
transfer pathway ... See more keywords