Poly(ionic liquid)s with unique adsorption-swelling ability toward epoxides for efficient atmospheric CO2 conversion under cocatalyst-/metal-/solvent-free conditions,Green Chemistry

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Poly(ionic liquid)s with unique adsorption-swelling ability toward epoxides for efficient atmospheric CO2 conversion under cocatalyst-/metal-/solvent-free conditions
Green Chemistry ( IF 9.3 ) Pub Date : 2023-08-30 , DOI: 10.1039/d3gc02213g
Bihua Chen ₁ , Shiguo Zhang ₁ , Yan Zhang ₁

Affiliation

Developing a simple and efficient heterogeneous catalyst for the cycloaddition of epoxides with CO₂ under atmospheric pressure and cocatalyst-/metal-/solvent-free conditions remains a great challenge. Herein, poly(ionic liquid)s (P-[VRIm]Br-crosslinker-x) with unique adsorption-swelling ability toward epoxides are designed and facilely synthesized via free radical polymerization in water. The adsorption-swelling of epoxides by P-[VRIm]Br-crosslinker-x is controllable, reversible, and widespread, resulting from the strong interactions between the poly(ionic liquid)s and epoxide molecules, especially the hydrogen-bonding interaction. Superior CO₂ cycloaddition is realized in the P-[VRIm]Br-crosslinker-x catalyst through the adsorption-swelling effect. Specifically, P-[VC6Im]Br-C8-5% with 54.1 mmol g⁻¹ adsorption-swelling ability toward styrene oxide achieves 89.3% yield and >99% selectivity in the cycloaddition of styrene oxide with CO₂ to styrene carbonate under mild conditions (1 atm, 80 °C) without cocatalyst/metal/solvent consumption. Moreover, P-[VC6Im]Br-C8-5% can be easily recovered by deswelling, and shows good reusability and stability after five cycles for a total of 180 h. The adsorption-swelling property of P-[VRIm]Br-crosslinker-x to epoxides not only prompts the active centers to be fully exposed to the reactants but also induces the enrichment of epoxides during the whole catalytic process, thus accelerating the CO₂ cycloaddition reaction rate. This work furnishes new insights for improving the activity of CO₂ cycloaddition and would guide the design of efficient poly(ionic liquid) catalysts for atmospheric CO₂ conversion.

中文翻译：

聚（离子液体）对环氧化物具有独特的吸附溶胀能力，可在无助催化剂/金属/溶剂的条件下实现大气中二氧化碳的高效转化

开发一种简单且高效的多相催化剂，用于在大气压和无助催化剂/金属/溶剂的条件下环氧化物与CO ₂的环加成仍然是一个巨大的挑战。在此，设计并通过水中自由基聚合轻松合成了对环氧化物具有独特吸附溶胀能力的聚（离子液体）（P-[VRIm]Br-交联剂-x ）。P-[VRIm]Br-交联剂-x对环氧化物的吸附溶胀是可控、可逆且广泛的，这是由于聚离子液体与环氧化物分子之间的强相互作用，特别是氢键相互作用所致。P-[VRIm]Br-交联剂- 实现了卓越的 CO _{2环加成反应-}x催化剂通过吸附溶胀作用。具体而言，P-[VC6Im]Br-C8-5%对氧化苯乙烯具有54.1 mmol g ^{-1 的}吸附溶胀能力，在温和条件下，氧化苯乙烯与CO ₂环加成至碳酸苯乙烯，产率达到89.3%，选择性>99% （1 atm，80 °C），无助催化剂/金属/溶剂消耗。此外，P-[VC6Im]Br-C8-5%可以通过消溶胀轻松回收，并且在总共180小时的五个循环后表现出良好的可重复使用性和稳定性。P-[VRIm]Br-交联剂-x对环氧化物的吸附溶胀特性不仅促使活性中心充分暴露于反应物，而且在整个催化过程中诱导环氧化物的富集，从而加速CO 2 的反应_。环加成反应速率。_{这项工作为提高CO 2}环加成活性提供了新的见解，并将指导用于大气CO ₂转化的高效聚（离子液体）催化剂的设计。

更新日期：2023-08-30

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