[HDBU]Br@P-DD 作为多孔有机聚合物负载的离子液体催化剂用于将 CO2 化学固定为环状碳酸酯,ACS Sustainable Chemistry & Engineering

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[HDBU]Br@P-DD 作为多孔有机聚合物负载的离子液体催化剂用于将 CO2 化学固定为环状碳酸酯
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2023-02-24 , DOI: 10.1021/acssuschemeng.2c07453
Huadeng Li ₁ , Ke Zheng ₂ , Jiaxiang Qiu ₁ , Ruomeng Duan ₂ , Jianling Feng ₁ , Rui Wang ₁ , Zhimeng Liu ₂ , Guanqun Xie ₁ , Xiaoxia Wang ₂

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_{CO 2}的化学固定将其转化为高附加值的环状碳酸酯在解决能源和生态问题方面具有巨大的潜力和可持续性。[HDBU]Br@P-DD-m/n，一系列多孔有机聚合物负载的离子液体 (PSILs)，通过 DMAEMA、DVB、4-溴丁酸的一锅四组分反应制备。 , 和 DBU。[HDBU]Br 的形成和 P-DD 聚合物网络的构建同时进行，同时实现了原位形成的 IL 的支持。通过 IR、ICP、BET、SEM 和 TGA 等对 PSIL 进行表征表明，所制备的催化剂具有多功能的分级孔隙率、不同的离子密度和优异的热稳定性。发现共聚物骨架的孔隙率受伴随形成的 [HDBU]Br 的影响。₂与环氧化物的反应，其中[HDBU]Br@P-DD-4/1在大气压和无溶剂/助催化剂条件下表现出最佳性能（95%的收率和99%的CO 2 与环氧氯丙烷环加成的选择性_）。通过关联催化剂的性能和结构，证明了叔胺、[HDBU]Br 和孔分布的协同作用。此外，该催化剂被发现适用于以良好至优异的收率合成一系列不同取代的碳酸酯。最后，催化剂可以很容易地回收，并且在使用 6 次后仍观察到良好的催化活性。该工作不仅为CO _{2的固定提供了一种活性、可重复使用、无金属的多相催化剂}进入环状碳酸酯，但也开发了一种简便的一步多组分策略来构建 PSIL 催化剂，这有望在催化和有机合成领域得到广泛应用。

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[HDBU]Br@P-DD as Porous Organic Polymer-Supported Ionic Liquid Catalysts for Chemical Fixation of CO2 into Cyclic Carbonates

The chemical fixation of CO₂ into high value-added cyclic carbonates is of significant potential and sustainability to address the energy and ecological issues. [HDBU]Br@P-DD-m/n, a series of porous organic polymer-supported ionic liquids (PSILs), were fabricated in this work through a one-pot four-component reaction of DMAEMA, DVB, 4-bromobutyric acid, and DBU. The formation of [HDBU]Br and construction of the P-DD polymer network proceeded concurrently with the support of the in situ-formed IL being achieved simultaneously. Characterization of the PSILs by IR, ICP, BET, SEM, and TGA etc. showed that the as-prepared catalysts possessed versatile hierarchical porosity with varying ionic densities and excellent thermostability. The porosity of the copolymer skeleton was found to be affected by the accompanying formation of [HDBU]Br. The PSILs were then evaluated as catalysts for the cycloaddition reaction of CO₂ with epoxides, among which [HDBU]Br@P-DD-4/1 showed the optimal performance under atmospheric pressure and solvent-/cocatalyst-free conditions (95% yield and 99% selectivity for CO₂ cycloaddition with epichlorohydrin). By correlating the performance and structures of the catalysts, the synergistic effect of the tertiary amine, [HDBU]Br, and pore distribution was demonstrated. In addition, the catalyst was found to be applicable in synthesizing a range of differently substituted carbonates in good to excellent yields. Finally, the catalyst could be recovered readily and good catalytic activity was still observed after use for 6 runs. The work not only provided an active, reusable, and metal-free heterogeneous catalyst for the fixation of CO₂ into cyclic carbonates but also developed a facile one-step multicomponent strategy for constructing PSIL catalysts, which would be promising to find wide applications in catalysis and organic synthesis field.

更新日期：2023-02-24

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