Aqueous-Phase Destruction of Nerve-Agent Simulants at Copper Single Atoms in UiO-66.
Inorg Chem
; 61(22): 8585-8591, 2022 Jun 06.
Article
in En
| MEDLINE
| ID: mdl-35613459
ABSTRACT
Metal-organic frameworks (MOFs) have shown great success in aqueous-phase hydrolysis of nerve agents, with some even showing promise in the gas phase. However, both aqueous-phase reactivity and gas-phase reactivity are hindered because of the binding of the hydrolyzed products to the MOF nodes in a stable, bridging configuration, which limits turnover. Single transition-metal atoms in MOFs have been a growing field of interest for catalytic applications, and single atoms have been proposed to prevent the unwanted bridged conformation and increase catalytic turnover. To date, there has been little experimental evidence to support the hypothesis. Herein, we report two copper single atom-modified UiO-66 MOFs for nerve-agent simulant degradation. Despite the capping of highly active Zr4+ nodes with fewer Lewis acidic Cun+ atoms, the reactivity of both CuMOFs approaches that of native UiO-66 under aqueous conditions. Computational studies reveal that the Cu coordination environment impairs product inhibition with respect to the native MOF.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Main subject:
Organometallic Compounds
/
Nerve Agents
/
Metal-Organic Frameworks
Language:
En
Journal:
Inorg Chem
Year:
2022
Document type:
Article
Affiliation country:
United States