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Tethering Dual Hydroxyls into Mesoporous Poly(ionic liquid)s for Chemical Fixation of CO2 at Ambient Conditions: A Combined Experimental and Theoretical Study
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-08 00:00:00 , DOI: 10.1021/acscatal.7b02399 Zengjing Guo 1 , Qiuwei Jiang 1 , Yuming Shi 1 , Jing Li 1 , Xiaoning Yang 1 , Wei Hou 1 , Yu Zhou 1 , Jun Wang 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2017-09-08 00:00:00 , DOI: 10.1021/acscatal.7b02399 Zengjing Guo 1 , Qiuwei Jiang 1 , Yuming Shi 1 , Jing Li 1 , Xiaoning Yang 1 , Wei Hou 1 , Yu Zhou 1 , Jun Wang 1
Affiliation
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Vicinal dual hydroxyl functional mesoporous poly(ionic liquid)s with large surface area and high ionic liquid (IL) content were synthesized through the copolymerization of epoxy-containing IL monomers and divinylbenzene, followed by ring opening in water. They acted as recyclable heterogeneous organocatalysts in the cycloaddition of a series of epoxides with CO2 under mild conditions (down to ambient conditions). The catalyst can be lightly recovered and reused with stable activity. The remarkable performance was attributable to the abundant mesoporosity and the synergistic effect of vicinal dual hydroxyls as hydrogen-bonding donors and halogen anions as nucleophiles. Density functional theory calculation, comprising the structural optimization, the energetic profile, and the charge and energy decomposition analysis by the combination of the extended transition state energy decomposition scheme with the natural orbitals for chemical valence approach, was performed to afford insight, indicating that the vicinal dual hydroxyls accelerated the reaction by providing a strong hydrogen-bonding effect and enhancing the leaving ability of the halogen anions.
中文翻译：
将双羟基化合物束缚到介孔聚离子液体中以在环境条件下化学固定CO 2：组合的实验和理论研究
通过含环氧基的IL单体与二乙烯基苯的共聚反应，然后在水中开环，合成了具有大表面积和高离子液体（IL）含量的双羟基官能介孔聚离子液体。在一系列环氧化物与CO 2的环加成反应中，它们充当了可回收的异质有机催化剂。在温和的条件下（降至环境条件）。该催化剂可以轻度回收并以稳定的活性进行再利用。出色的性能归因于丰富的介孔性以及邻位双羟基作为氢键供体和卤素阴离子作为亲核试剂的协同作用。进行了密度泛函理论计算，包括结构优化，能级分布以及结合扩展的过渡态能量分解方案与化学价态的自然轨道进行的电荷和能量分解分析，以提供洞察力，表明邻位双羟基通过提供强大的氢键作用并增强卤素阴离子的离去能力，从而加速了反应。
更新日期：2017-09-08
中文翻译：
将双羟基化合物束缚到介孔聚离子液体中以在环境条件下化学固定CO 2：组合的实验和理论研究
通过含环氧基的IL单体与二乙烯基苯的共聚反应，然后在水中开环，合成了具有大表面积和高离子液体（IL）含量的双羟基官能介孔聚离子液体。在一系列环氧化物与CO 2的环加成反应中，它们充当了可回收的异质有机催化剂。在温和的条件下（降至环境条件）。该催化剂可以轻度回收并以稳定的活性进行再利用。出色的性能归因于丰富的介孔性以及邻位双羟基作为氢键供体和卤素阴离子作为亲核试剂的协同作用。进行了密度泛函理论计算，包括结构优化，能级分布以及结合扩展的过渡态能量分解方案与化学价态的自然轨道进行的电荷和能量分解分析，以提供洞察力，表明邻位双羟基通过提供强大的氢键作用并增强卤素阴离子的离去能力，从而加速了反应。
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