Two Sustainable Pathways of MOF-Catalyzed Room Temperature\nChemical Fixation of CO<sub>2</sub> inside Alkynes under Atmospheric\nPressure

The\nrising atmospheric CO<sub>2</sub> levels necessitate the development\nof effective materials for its mitigation. Utilization of adsorbent\nmaterials for the reversible physisorption of CO<sub>2</sub> has a\nsignificantly less impact. Recognizing this need, herein, we present\na nitrogen-rich, aqua-stable, Ag(0)-nanoparticle-doped metal–organic\nframework (MOF) designed for the irreversible chemical conversion\nof CO<sub>2</sub> into valuable fine chemicals. We demonstrate two\nsustainable pathways for CO<sub>2</sub> fixation, utilizing the catalyst, <b>1′</b>@Ag NPs. The designed catalyst facilitates the cyclization\nof propargylic amines and alcohols under ambient temperature and pressure\nconditions. Remarkably, this is the first MOF-based catalyst that\nallows for quantitative conversion of propargylic amines into 2-oxazolidinones\nat room temperature with atmospheric CO<sub>2</sub> pressure. The\nprocess successfully transforms various propargylic amines and alcohols\ninto 2-oxazolidinones and α-alkylidene cyclic carbonates under\nthe CO<sub>2</sub> atmosphere. Additionally, the catalyst shows excellent\nrecyclability, maintaining its activity and structural integrity across\nmultiple reuse cycles. Control experiments revealed that the catalytic\nefficiency of <b>1′</b>@Ag NPs is attributed to the highly\nexposed alkynophilic Ag(0) sites on its pore walls. Computational\nstudies further elucidate the mechanistic pathway for CO<sub>2</sub> fixation. This work highlights the potential of <b>1′</b>@Ag NPs to enhance environmental sustainability by converting CO<sub>2</sub> into valuable bioactive chemicals under mild conditions.

Publication Details

Journal
Figshare
Published
2024-10-31
DOI
https://doi.org/10.1021/acs.inorgchem.4c03431.s001
Primary Topic
Mycorrhizal Fungi and Plant Interactions
Type
article
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Two Sustainable Pathways of MOF-Catalyzed Room Temperature\nChemical Fixation of CO2 inside Alkynes under Atmospheric\nPressure

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Mycorrhizal Fungi and Plant Interactions
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Two Sustainable Pathways of MOF-Catalyzed Room Temperature\nChemical Fixation of CO2 inside Alkynes under Atmospheric\nPressure

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Abstract

The\nrising atmospheric CO<sub>2</sub> levels necessitate the development\nof effective materials for its mitigation. Utilization of adsorbent\nmaterials for the reversible physisorption of CO<sub>2</sub> has a\nsignificantly less impact. Recognizing this need, herein, we present\na nitrogen-rich, aqua-stable, Ag(0)-nanoparticle-doped metal–organic\nframework (MOF) designed for the irreversible chemical conversion\nof CO<sub>2</sub> into valuable fine chemicals. We demonstrate two\nsustainable pathways for CO<sub>2</sub> fixation, utilizing the catalyst, <b>1′</b>@Ag NPs. The designed catalyst facilitates the cyclization\nof propargylic amines and alcohols under ambient temperature and pressure\nconditions. Remarkably, this is the first MOF-based catalyst that\nallows for quantitative conversion of propargylic amines into 2-oxazolidinones\nat room temperature with atmospheric CO<sub>2</sub> pressure. The\nprocess successfully transforms various propargylic amines and alcohols\ninto 2-oxazolidinones and α-alkylidene cyclic carbonates under\nthe CO<sub>2</sub> atmosphere. Additionally, the catalyst shows excellent\nrecyclability, maintaining its activity and structural integrity across\nmultiple reuse cycles. Control experiments revealed that the catalytic\nefficiency of <b>1′</b>@Ag NPs is attributed to the highly\nexposed alkynophilic Ag(0) sites on its pore walls. Computational\nstudies further elucidate the mechanistic pathway for CO<sub>2</sub> fixation. This work highlights the potential of <b>1′</b>@Ag NPs to enhance environmental sustainability by converting CO<sub>2</sub> into valuable bioactive chemicals under mild conditions.

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Two Sustainable Pathways of MOF-Catalyzed Room Temperature\nChemical Fixation of CO<sub>2</sub> inside Alkynes under Atmospheric\nPressure · Figshare (2024) | TGRS Research Map | TGRS