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Träfflista för sökning "WFRF:(Greco Claudio) srt2:(2015-2019)"

Sökning: WFRF:(Greco Claudio) > (2015-2019)

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1.
  • Rovaletti, Anna, et al. (författare)
  • A thiocarbonate sink on the enzymatic energy landscape of aerobic CO oxidation? Answers from DFT and QM/MM models of Mo–Cu CO-dehydrogenases
  • 2019
  • Ingår i: Journal of Catalysis. - : Elsevier BV. - 0021-9517. ; , s. 201-205
  • Tidskriftsartikel (refereegranskat)abstract
    • We present a theoretical investigation providing key insights on a long-standing controversial issue that dominated the debate on carbon monoxide oxidation by Mo–Cu CO-dehydrogenases. Previous investigations gravitate around the possible occurrence of a thiocarbonate intermediate, that was repeatedly reported to behave as a thermodynamic sink on the catalytic energy landscape. By using a hierarchy of quantum mechanical and hybrid quantum/classical models of the enzyme, we show that no such energy sink is present on the catalytic energy profile. Consequent perspectives for the definition of a novel mechanistic proposal for the enzyme-catalyzed CO-oxidation are discussed in light of the recent literature.
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2.
  • Rovaletti, Anna, et al. (författare)
  • Theoretical insights into the aerobic hydrogenase activity of molybdenum-copper CO dehydrogenase
  • 2019
  • Ingår i: Inorganics. - : MDPI AG. - 2304-6740. ; 7:11
  • Tidskriftsartikel (refereegranskat)abstract
    • The Mo/Cu-dependent CO dehydrogenase from O. carboxidovorans is an enzyme that is able to catalyse CO oxidation to CO2; moreover, it also expresses hydrogenase activity, as it is able to oxidize H2. Here, we have studied the dihydrogen oxidation catalysis by this enzyme using QM/MM calculations. Our results indicate that the equatorial oxo ligand of Mo is the best suited base for catalysis. Moreover, extraction of the first proton from H2 by means of this basic centre leads to the formation of a Mo–OH–CuIH hydride that allows for the stabilization of the copper hydride, otherwise known to be very unstable. In light of our results, two mechanisms for the hydrogenase activity of the enzyme are proposed. The first reactive channel depends on protonation of the sulphur atom of a Cu-bound cysteine residues, which appears to favour the binding and activation of the substrate. The second reactive channel involves a frustrated Lewis pair, formed by the equatorial oxo group bound to Mo and by the copper centre. In this case, no binding of the hydrogen molecule to the Cu center is observed but once H2 enters into the active site, it can be split following a low-energy path.
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  • Resultat 1-2 av 2
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tidskriftsartikel (2)
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refereegranskat (2)
Författare/redaktör
Ryde, Ulf (2)
Bruschi, Maurizio (2)
Greco, Claudio (2)
Rovaletti, Anna (2)
Moro, Giorgio (2)
Cosentino, Ugo (2)
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Lunds universitet (2)
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Engelska (2)
Forskningsämne (UKÄ/SCB)
Naturvetenskap (2)
Teknik (1)
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2019 (2)

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