Title :

Optimizing Group Transfer Catalysis by Copper Complex with Redox-Active Ligand in an Entatic State

Author(s) :

Ren, Yufeng [Auteur]
Forté, Jeremy [Auteur]
Cheaib, Khaled [Auteur]
Vanthuyne, Nicolas [Auteur]
Fensterbank, Louis [Auteur]
Vezin, Herve [Auteur]
1292|||Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 [LASIRE]
Orio, Maylis [Auteur]
Institut des Sciences Moléculaires de Marseille [ISM2]
Blanchard, Sébastien [Auteur]
Desage-El Murr, Marine [Auteur]

Journal title :

Iscience

Abbreviated title :

iScience

Volume number :

23

Pages :

100955

Publisher :

Elsevier BV

Publication date :

2020-03

ISSN :

2589-0042

English keyword(s) :

Inorganic Chemistry
Molecular Inorganic Chemistry
Catalysis

HAL domain(s) :

Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

Metalloenzymes use earth-abundant non-noble metals to perform high-fidelity transformations in the biological world. To ensure chemical efficiency, metalloenzymes have acquired evolutionary reactivity-enhancing tools. Among ...
Show more >Metalloenzymes use earth-abundant non-noble metals to perform high-fidelity transformations in the biological world. To ensure chemical efficiency, metalloenzymes have acquired evolutionary reactivity-enhancing tools. Among these, the entatic state model states that a strongly distorted geometry induced by ligands around a metal center gives rise to an energized structure called entatic state, strongly improving the reactivity. However, the original definition refers both to the transfer of electrons or chemical groups, whereas the chemical application of this concept in synthetic systems has mostly focused on electron transfer, therefore eluding chemical transformations. Here we report that a highly strained redox-active ligand enables a copper complex to perform catalytic nitrogen- and carbon-group transfer in as fast as 2 min, thus exhibiting a strong increase in reactivity compared with its unstrained analogue. This report combines two reactivity-enhancing features from metalloenzymes, entasis and redox cofactors, applied to group-transfer catalysis.Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

Administrative institution(s) :

Université de Lille
CNRS

Collections :

• Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516

Research team(s) :

Propriétés magnéto structurales des matériaux (PMSM)

Submission date :

2021-06-17T12:12:06Z
2021-06-24T09:55:11Z
2021-06-24T10:01:31Z
2023-07-11T11:56:24Z