Lewis Acid Catalyzed Amide Bond Formation in Covalent Graphene-MOF Hybrids

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F61388963%3A_____%2F23%3A00573682" target="_blank" >RIV/61388963:_____/23:00573682 - isvavai.cz</a>

Nalezeny alternativní kódy

RIV/61989592:15640/23:73620079 RIV/61989100:27640/23:10252632 RIV/61989100:27740/23:10252632

Výsledek na webu

<a href="https://doi.org/10.1021/acs.jpcc.3c01821" target="_blank" >https://doi.org/10.1021/acs.jpcc.3c01821</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1021/acs.jpcc.3c01821" target="_blank" >10.1021/acs.jpcc.3c01821</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Lewis Acid Catalyzed Amide Bond Formation in Covalent Graphene-MOF Hybrids

Popis výsledku v původním jazyce

Covalent hybrids of graphene and metal–organic frameworks (MOFs) hold immense potential in various technologies, particularly catalysis and energy applications, due to the advantageous combination of conductivity and porosity. The formation of an amide bond between carboxylate-functionalized graphene acid (GA) and amine-functionalized UiO-66-NH2 MOF (Zr6O4(OH)4(NH2-bdc)6, with NH2-bdc2– = 2-amino-1,4-benzenedicarboxylate and UiO = Universitetet i Oslo) is a highly efficient strategy for creating such covalent hybrids. Previous experimental studies have demonstrated exceptional properties of these conductive networks, including significant surface area and functionalized hierarchical pores, showing promise as a chemiresistive CO2 sensor and electrode materials for asymmetric supercapacitors. However, the molecular-level origin of the covalent linkages between pristine MOF and GA layers remains unclear. In this study, density functional theory (DFT) calculations were conducted to elucidate the mechanism of amide bond formation between GA and UiO-66-NH2. The theoretical calculations emphasize the crucial role of zirconium within UiO-66, which acts as a catalyst in the reaction cycle. Both commonly observed hexa-coordinated and less common hepta-coordinated zirconium complexes are considered as intermediates. By gaining detailed insights into the binding interactions between graphene derivatives and MOFs, strategies for tailored syntheses of such nanocomposite materials can be developed.

Název v anglickém jazyce

Lewis Acid Catalyzed Amide Bond Formation in Covalent Graphene-MOF Hybrids

Popis výsledku anglicky

Covalent hybrids of graphene and metal–organic frameworks (MOFs) hold immense potential in various technologies, particularly catalysis and energy applications, due to the advantageous combination of conductivity and porosity. The formation of an amide bond between carboxylate-functionalized graphene acid (GA) and amine-functionalized UiO-66-NH2 MOF (Zr6O4(OH)4(NH2-bdc)6, with NH2-bdc2– = 2-amino-1,4-benzenedicarboxylate and UiO = Universitetet i Oslo) is a highly efficient strategy for creating such covalent hybrids. Previous experimental studies have demonstrated exceptional properties of these conductive networks, including significant surface area and functionalized hierarchical pores, showing promise as a chemiresistive CO2 sensor and electrode materials for asymmetric supercapacitors. However, the molecular-level origin of the covalent linkages between pristine MOF and GA layers remains unclear. In this study, density functional theory (DFT) calculations were conducted to elucidate the mechanism of amide bond formation between GA and UiO-66-NH2. The theoretical calculations emphasize the crucial role of zirconium within UiO-66, which acts as a catalyst in the reaction cycle. Both commonly observed hexa-coordinated and less common hepta-coordinated zirconium complexes are considered as intermediates. By gaining detailed insights into the binding interactions between graphene derivatives and MOFs, strategies for tailored syntheses of such nanocomposite materials can be developed.

Druh

J_imp - Článek v periodiku v databázi Web of Science

CEP obor

—

OECD FORD obor

10402 - Inorganic and nuclear chemistry

Projekt

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

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2023

Kód důvěrnosti údajů

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

Název periodika

Journal of Physical Chemistry C

ISSN

1932-7447

e-ISSN

1932-7455

Svazek periodika

127

Číslo periodika v rámci svazku

31

Stát vydavatele periodika

US - Spojené státy americké

Počet stran výsledku

7

Strana od-do

15454-15460

Kód UT WoS článku

001018960800001

EID výsledku v databázi Scopus

2-s2.0-85164822895