Hydroxy-bridged resting states of a [NiFe]-hydrogenase unraveled by cryogenic vibrational spectroscopy and DFT computations
نویسندگان
چکیده
منابع مشابه
Hydride bridge in [NiFe]-hydrogenase observed by nuclear resonance vibrational spectroscopy
The metabolism of many anaerobes relies on [NiFe]-hydrogenases, whose characterization when bound to substrates has proven non-trivial. Presented here is direct evidence for a hydride bridge in the active site of the (57)Fe-labelled fully reduced Ni-R form of Desulfovibrio vulgaris Miyazaki F [NiFe]-hydrogenase. A unique 'wagging' mode involving H(-) motion perpendicular to the Ni(μ-H)(57)Fe pl...
متن کاملSynthesis and vibrational spectroscopy of 57Fe-labeled models of [NiFe] hydrogenase: first direct observation of a nickeliron interaction
Despite our extremely low atmospheric concentration of dihydrogen (B1 ppm), this substrate is a key metabolite of many anaerobic bacteria. In such living systems can be found the most prevalent enzymes for hydrogen processing, the nickel–iron hydrogenases ([NiFe]–H2ases). 1,2 These electrocatalysts specifically mediate the redox reaction H2 " 2H + + 2e at several hundred turnovers per second. T...
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We have applied nuclear inelastic scattering (NIS) and computational predictions based on density functional theory (DFT) to explore the vibrational dynamics of Fe in a trinuclear oxo-bridged iron(III) complex. Quantitative comparison of the experimentally measured vibrational dynamics of the Mössbauer nuclei Fe, with normal mode analysis, calculated via quantum chemical calculation based on DF...
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Hidroxo-sais lamelares de composição Cu 2 (OH) 3 X (X = NO 3 , CH 3 COO e ClO 4 ) foram sintetizados através da coprecipitação (sais básicos de nitrato e acetato) e da troca iônica (sal básico de perclorato). Os sólidos cristalinos foram caracterizados por difratometria de raios X, análise termogravimétrica e espectroscopia vibracional. Bandas fracas em 336 e 345 cm (espectro Raman) dos sais de...
متن کاملThiolate-bridged dinuclear iron(tris-carbonyl)-nickel complexes relevant to the active site of [NiFe] hydrogenase.
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 clus...
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ژورنال
عنوان ژورنال: Chemical Science
سال: 2021
ISSN: 2041-6520,2041-6539
DOI: 10.1039/d0sc05022a