Investigating the role of the strong field ligands in [FeFe] hydrogenase: spectroscopic and functional characterization of a semi-synthetic mono-cyanide active site - CEA Grenoble Accéder directement au contenu
Article Dans Une Revue Chemical Science Année : 2022

Investigating the role of the strong field ligands in [FeFe] hydrogenase: spectroscopic and functional characterization of a semi-synthetic mono-cyanide active site

Marco Lorenzi
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Joe Gellett
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Moritz Senger
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Zehui Duan
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Patricia Rodriguez-Macia
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Gustav Berggren
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Résumé

Artificial maturation of hydrogenases provides a path towards generating new semi-synthetic enzymes with novel catalytic properties. Here enzymes featuring a synthetic asymmetric mono-cyanide cofactor have been prepared using two different hydrogenase scaffolds. Their structure and reactivity was investigated in order to elucidate the design rationale behind the native di-cyanide cofactor, and by extension the second coordination sphere of the active-site pocket. Surprisingly, the choice of host enzyme was found to have a dramatic impact on reactivity. Moreover, the study shows that synthetic manipulations of the active-site can significantly increase inhibitor tolerance, as compared to native [FeFe] hydrogenase, while retaining the enzyme's native capacity for reversible catalysis.
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Dates et versions

hal-04041579 , version 1 (22-03-2023)

Identifiants

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Marco Lorenzi, Joe Gellett, Afridi Zamader, Moritz Senger, Zehui Duan, et al.. Investigating the role of the strong field ligands in [FeFe] hydrogenase: spectroscopic and functional characterization of a semi-synthetic mono-cyanide active site. Chemical Science, 2022, 13 (37), pp.11058-11064. ⟨10.1039/d2sc02271k⟩. ⟨hal-04041579⟩
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