高活性苯并三唑离子液体修饰的周期性介孔有机硅负载的钐/镧纳米颗粒用于二氧化碳到环状碳酸盐的可持续转化

Hung Yu Lin, B. Xiao, Yang Liu
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引用次数: 1

摘要

摘要本文提出了一种新型的多功能纳米催化剂La-/Sm-PMO-ILCl,该催化剂是基于苯并三唑离子液体的固定化和在周期性介孔有机硅上进一步掺入乙酸钐或乙酸镧,用于CO2和环氧化物的环加成反应,从而制备环状碳酸盐。由于周期性介孔有机硅的钐位与离子液体均匀分散的碱位之间的分子内协同作用,强力催化剂Sm-PMO-ILCl在不添加任何溶剂和助催化剂的情况下,在环加成反应中具有超高收率和选择性的优异催化性能。此外,催化剂Sm-PMO-ILCl可以很容易地通过过滤回收,并且可以重复使用至少5次,而不会显著降低其催化活性。Resumen。在有机硅介孔条件下,通过苯并三唑液相催化制备了新型纳米催化剂La-(Sm-PMO-ILC1)。利用环氧化合物对二氧化碳的催化活性进行了评价。本文研究了分子内分子中心失稳的影响,通过失稳的碱基和离子的均质分布诱导了分子内活性催化剂Sm-PMO-ILC1的失稳。同时,合成催化剂采用选择性催化法,在聚合溶剂和共催化剂的催化作用下,实现了催化剂的选择性转化。结果表明,该催化剂Sm-PMO-ILC1对催化活性较低的5种催化剂具有显著的催化活性。
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Highly Active Benzotriazolium Ionic Liquid-modified Periodic Mesoporous Organosilica Supported Samarium/Lanthanum Nanoparticles for Sustainable Transformation of Carbon Dioxide to Cyclic Carbonates
Abstract. A novel type of multifunctional nanocatalysts (La-/Sm-PMO-ILCl) based on the immobilization of benzotriazolium ionic liquid and further incorporation of samarium acetate or lanthanum acetate onto periodic mesoporous organosilica were afforded for the cycloaddition of CO2 and epoxides to produce cyclic carbonates. In consequence of the intramolecular synergistic effect between samarium sites of periodic mesoporous organosilica and homogeneously dispersed basic sites of ionic liquid, the powerful catalyst Sm-PMO-ILCl offered superior catalytic performance with ultra high yields and selectivities in the cycloaddition reaction without the addition of any solvent and cocatalyst. Moreover, the catalyst Sm-PMO-ILCl could be easily recovered by filtration and reused for at least five runs without any significant loss of its catalytic activity. Resumen. Se prepararon nuevos nano catalizadores (La-(Sm-PMO-ILC1) por la via de inmovilizacion del liquido ionico benzotriazolium y adicion se acetato de samario o acetato de lantano en organosilice mesoporosa. Los catalizadores se evaluaron en la ciclo adicion de CO2 y epoxidos para producir carbonatos ciclicos. El efecto sinergico intramolecular entre los sitios de samario de la organosilice y los sitios basicos del liquido ionico homogeneamente distribuidos inducen una alta actividad catalitica en el catalizador Sm-PMO-ILC1. Asi, con este catalizador se obtuvo alta conversion y selectividad en la reaccion de ciclo adicion, sin agregar solvente ni co-catalizador. Ademas, el catalizador Sm-PMO-ILC1 podria recuperarse facilmente por filtracion y reusado por al menos 5 corridas sin perdida significativa de su actividad catalitica.
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