Phenanthroline-functionalized graphene as a ligand platform for single-atom catalysis

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61989592%3A15640%2F25%3A73631922" target="_blank" >RIV/61989592:15640/25:73631922 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989100:27740/25:10258743 RIV/61989100:27640/25:10258743

Výsledek na webu

<a href="https://www.sciencedirect.com/science/article/pii/S0920586125003116?via%3Dihub" target="_blank" >https://www.sciencedirect.com/science/article/pii/S0920586125003116?via%3Dihub</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1016/j.cattod.2025.115493" target="_blank" >10.1016/j.cattod.2025.115493</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Phenanthroline-functionalized graphene as a ligand platform for single-atom catalysis

Popis výsledku v původním jazyce

The precise anchoring of single metal atoms on solid supports remains a key challenge in the design of singleatom catalysts (SACs), particularly for carbon-based materials where metal coordination environments are often poorly defined. We report a graphene-based support covalently functionalized with 1,10-phenanthroline-5amine groups via nucleophilic substitution on fluorographene in DMSO. This approach introduces well-defined chelating sites that enable the rational and selective immobilization of transition metals. A copper-based SAC was synthesized by impregnating the functionalized graphene with a CuCl2 solution. Spectroscopic and microscopic analyses confirmed the formation of atomically dispersed Cu(I) species coordinated by phenanthroline ligands, with no detectable nanoparticle formation. The resulting catalyst exhibited high activity in the Chan-Lam coupling of 1H-imidazole with phenylboronic acid, achieving a turnover frequency of 3.8 h- 1, and outperformed heterogeneous benchmark systems, including commercial CuO nanoparticles. However, recyclability tests revealed a decline in catalytic activity after four cycles, primarily due to the leaching of Cu-phenanthroline complexes. These findings demonstrate the potential of functionalized graphene as a platform for developing SACs with well-defined coordination environments. Nevertheless, enhancing catalyst stability, e.g., through secondary anchoring strategies, optimized metalation protocols, or post-synthetic stabilization, is needed for future industrial applications.

Název v anglickém jazyce

Phenanthroline-functionalized graphene as a ligand platform for single-atom catalysis

Popis výsledku anglicky

The precise anchoring of single metal atoms on solid supports remains a key challenge in the design of singleatom catalysts (SACs), particularly for carbon-based materials where metal coordination environments are often poorly defined. We report a graphene-based support covalently functionalized with 1,10-phenanthroline-5amine groups via nucleophilic substitution on fluorographene in DMSO. This approach introduces well-defined chelating sites that enable the rational and selective immobilization of transition metals. A copper-based SAC was synthesized by impregnating the functionalized graphene with a CuCl2 solution. Spectroscopic and microscopic analyses confirmed the formation of atomically dispersed Cu(I) species coordinated by phenanthroline ligands, with no detectable nanoparticle formation. The resulting catalyst exhibited high activity in the Chan-Lam coupling of 1H-imidazole with phenylboronic acid, achieving a turnover frequency of 3.8 h- 1, and outperformed heterogeneous benchmark systems, including commercial CuO nanoparticles. However, recyclability tests revealed a decline in catalytic activity after four cycles, primarily due to the leaching of Cu-phenanthroline complexes. These findings demonstrate the potential of functionalized graphene as a platform for developing SACs with well-defined coordination environments. Nevertheless, enhancing catalyst stability, e.g., through secondary anchoring strategies, optimized metalation protocols, or post-synthetic stabilization, is needed for future industrial applications.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

21001 - Nano-materials (production and properties)

Projekt

<a href="/cs/project/EH22_008%2F0004587" target="_blank" >EH22_008/0004587: Technologie za hranicí nanosvěta</a><br>

Návaznosti

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

Rok uplatnění

2025

Kód důvěrnosti údajů

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

Název periodika

CATALYSIS TODAY

ISSN

0920-5861

e-ISSN

1873-4308

Svazek periodika

460

Číslo periodika v rámci svazku

December

Stát vydavatele periodika

NL - Nizozemsko

Počet stran výsledku

9

Strana od-do

nestránkováno

Kód UT WoS článku

001578796700001

EID výsledku v databázi Scopus

2-s2.0-105012601155