The rapid increase in the concentration of atmospheric carbon dioxide (CO₂) has resulted in undesirable environmental issues. Hence, selective CO₂ capture and utilization as C1 feedstock for the preparation of high-value chemicals and fuels has been considered as a promising step toward mitigating the growing concentration of atmospheric CO₂. In this direction, herein we report rational construction of a Ag(I)-anchored sulfonate-functionalized UiO-66 MOF named as MOF-SO₃Ag composed of CO₂-philic sulfonate functionality and catalytically active alkynophilic Ag(I) sites for chemical fixation of carbon dioxide. The MOF-SO₃Ag exhibits selective as well as recyclable adsorption of CO₂ with a high heat of adsorption energy (Q_st) of 37.8 kJ/mol. On the other hand, the analogous MOF, UiO-66 doped with Ag(I), showed a lower Q_st value of 30 kJ/mol, highlighting the importance of the sulfonate group for stronger interaction with CO₂. Furthermore, the MOF-SO₃Ag acts as an efficient heterogeneous catalyst for cyclic carboxylation of propargylic alcohols to generate α-alkylidene cyclic carbonates in >99% yield at mild conditions of RT and 1 bar CO₂. More importantly, one-pot synthesis of oxazolidinones by a three-component reaction between CO₂, propargylic alcohol, and primary amine has also been achieved using MOF-SO₃Ag catalyst under the mild conditions. The MOF is highly recyclable and retains its superior catalytic activity even after several cycles. To the best of our knowledge, MOF-SO₃Ag is the first example of MOF reported for RT chemical fixation of CO₂ to oxazolidinones by aminolysis of α-alkylidene cyclic carbonates under the environment-friendly mild conditions.

中文翻译：

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在室温和大气压条件下高效固定二氧化碳：极性功能对选择性捕获和转化二氧化碳的影响。

大气中二氧化碳（CO ₂）浓度的迅速增加导致了不良的环境问题。因此，选择性的CO ₂捕集和用作制备高价值化学品和燃料的C1原料已被认为是缓解大气中CO ₂浓度不断增加的有希望的步骤。在这个方向上，我们在此报告了由Ag（I）固定的磺酸盐官能化的UiO-66 MOF的合理结构，该MOF被命名为MOF-SO ₃ Ag，由化学性质为CO _2的磺酸盐和具有催化活性的嗜碱性Ag（I）组成。固定二氧化碳。MOF-SO ₃ Ag表现出对CO的选择性吸附和可回收吸附₂具有37.8kJ / mol的高吸附能热（Q _st）。另一方面，类似的MOF，掺有Ag（I）的UiO-66，显示出较低的Q _st值，为30 kJ / mol，突显了磺酸根基团与CO ₂更强相互作用的重要性。此外，MOF-SO ₃ Ag用作高效的非均相催化剂，用于炔丙醇的环羧化反应，在温和的RT和1 bar CO ₂条件下以> 99％的产率生成α-亚烷基环状碳酸酯。更重要的是，使用MOF-SO ₃还可以通过CO ₂，炔丙醇和伯胺之间的三组分反应一锅合成恶唑烷酮Ag催化剂在温和的条件下。MOF具有高度可回收性，即使经过数次循环后仍保持其优异的催化活性。据我们所知，MOF-SO ₃ Ag是在环境友好的温和条件下通过α-亚烷基环状碳酸酯的氨解将CO ₂ RT化学固定到恶唑烷酮的MOF的第一个实例。