Mixed-Valence Single-Atom Catalyst Derived from Functionalized Graphene

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15310%2F19%3A73594904" target="_blank" >RIV/61989592:15310/19:73594904 - isvavai.cz</a>

Výsledek na webu

<a href="https://onlinelibrary.wiley.com/doi/full/10.1002/adma.201900323" target="_blank" >https://onlinelibrary.wiley.com/doi/full/10.1002/adma.201900323</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/adma.201900323" target="_blank" >10.1002/adma.201900323</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Mixed-Valence Single-Atom Catalyst Derived from Functionalized Graphene

Popis výsledku v původním jazyce

Single-atom catalysts (SACs) aim at bridging the gap between homogeneous and heterogeneous catalysis. The challenge is the development of materials with ligands enabling coordination of metal atoms in different valence states, and preventing leaching or nanoparticle formation. Graphene functionalized with nitrile groups (cyanographene) is herein employed for the robust coordination of Cu(II) ions, which are partially reduced to Cu(I) due to graphene-induced charge transfer. Inspired by nature&apos;s selection of Cu(I) in enzymes for oxygen activation, this 2D mixed-valence SAC performs flawlessly in two O-2-mediated reactions: the oxidative coupling of amines and the oxidation of benzylic C-H bonds toward high-value pharmaceutical synthons. High conversions (up to 98%), selectivities (up to 99%), and recyclability are attained with very low metal loadings in the reaction. The synergistic effect of Cu(II) and Cu(I) is the essential part in the reaction mechanism. The developed strategy opens the door to a broad portfolio of other SACs via their coordination to various functional groups of graphene, as demonstrated by successful entrapment of Fe-III/Fe-II single atoms to carboxy-graphene.

Název v anglickém jazyce

Mixed-Valence Single-Atom Catalyst Derived from Functionalized Graphene

Popis výsledku anglicky

Single-atom catalysts (SACs) aim at bridging the gap between homogeneous and heterogeneous catalysis. The challenge is the development of materials with ligands enabling coordination of metal atoms in different valence states, and preventing leaching or nanoparticle formation. Graphene functionalized with nitrile groups (cyanographene) is herein employed for the robust coordination of Cu(II) ions, which are partially reduced to Cu(I) due to graphene-induced charge transfer. Inspired by nature&apos;s selection of Cu(I) in enzymes for oxygen activation, this 2D mixed-valence SAC performs flawlessly in two O-2-mediated reactions: the oxidative coupling of amines and the oxidation of benzylic C-H bonds toward high-value pharmaceutical synthons. High conversions (up to 98%), selectivities (up to 99%), and recyclability are attained with very low metal loadings in the reaction. The synergistic effect of Cu(II) and Cu(I) is the essential part in the reaction mechanism. The developed strategy opens the door to a broad portfolio of other SACs via their coordination to various functional groups of graphene, as demonstrated by successful entrapment of Fe-III/Fe-II single atoms to carboxy-graphene.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10403 - Physical chemistry

Projekt

Výsledek vznikl pri realizaci vícero projektů. Více informací v záložce Projekty.

Návaznosti

P - Projekt vyzkumu a vyvoje financovany z verejnych zdroju (s odkazem do CEP)

Rok uplatnění

2019

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Advanced Materials

ISSN

0935-9648

e-ISSN

—

Svazek periodika

31

Číslo periodika v rámci svazku

17

Stát vydavatele periodika

DE - Spolková republika Německo

Počet stran výsledku

9

Strana od-do

"1900323-1"-"1900323-9"

Kód UT WoS článku

000465600000025

EID výsledku v databázi Scopus

2-s2.0-85062321283