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 Access content directly
Journal Articles Chemical Science Year : 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
  • Function : Author
Joe Gellett
  • Function : Author
Moritz Senger
  • Function : Author
Zehui Duan
  • Function : Author
Patricia Rodriguez-Macia
  • Function : Correspondent author
  • PersonId : 1240092

Connectez-vous pour contacter l'auteur
Gustav Berggren
Connectez-vous pour contacter l'auteur

Abstract

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.
Fichier principal
Vignette du fichier
d2sc02271k.pdf (1.11 Mo) Télécharger le fichier
Origin Publisher files allowed on an open archive

Dates and versions

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

Identifiers

Cite

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⟩
18 View
20 Download

Altmetric

Share

Gmail Mastodon Facebook X LinkedIn More