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Pyrene-Based Nanoporous Covalent Organic Framework for Carboxylation of C-H Bonds with CO 2 and Value-Added 2-Oxazolidinones Synthesis under Ambient Conditions.
- Source :
-
ACS applied materials & interfaces [ACS Appl Mater Interfaces] 2024 Feb 07; Vol. 16 (5), pp. 5857-5868. Date of Electronic Publication: 2024 Jan 23. - Publication Year :
- 2024
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Abstract
- The selective carbon capture and utilization (CCU) as a one-carbon (C1) feedstock offers dual advantages for mitigating the rising atmospheric CO <subscript>2</subscript> content and producing fine chemicals/fuels. In this context, herein, we report the application of a porous bipyridine-functionalized, pyrene-based covalent organic framework (Pybpy-COF) for the stable anchoring of catalytic Ag(0) nanoparticles (NPs) and its catalytic investigation for fixation of CO <subscript>2</subscript> to commodity chemicals at ambient conditions. Notably, Ag@Pybpy-COF showed excellent catalytic activity for the carboxylation of various terminal alkynes to corresponding alkynyl carboxylic acids/phenylpropiolic acids via C-H bond activation under atmospheric pressure conditions. Besides, carboxylative cyclization of various propargylic amines with CO <subscript>2</subscript> to generate 2-oxazolidinones, an important class of antibiotics, has also been achieved under mild conditions. This significant catalytic activity of Ag@Pybpy-COF with wide functional group tolerance is rendered by the presence of highly exposed, alkynophilic Ag(0) catalytic sites decorated on the pore walls of high surface area (787 m <superscript>2</superscript> g <superscript>-1</superscript> ) Pybpy-COF. Further, density functional theory calculations unveiled the detailed mechanistic path of the Ag@Pybpy-COF-catalyzed transformation of CO <subscript>2</subscript> to alkynyl carboxylic acids and 2-oxazolidinones. Moreover, the catalyst showed high recyclability for several cycles of reuse without significant loss in its catalytic activity and structural rigidity. This work demonstrates the promising application of Pybpy-COF for stable anchoring of Ag NPs for successful transformation of CO <subscript>2</subscript> to valuable commodity chemicals at ambient conditions.
Details
- Language :
- English
- ISSN :
- 1944-8252
- Volume :
- 16
- Issue :
- 5
- Database :
- MEDLINE
- Journal :
- ACS applied materials & interfaces
- Publication Type :
- Academic Journal
- Accession number :
- 38259199
- Full Text :
- https://doi.org/10.1021/acsami.3c16690