{"title":"新型可重复使用的磁性 MOF 纳米复合材料耦合离子液体促进二氧化碳高效化学固定为 α-亚烷基环碳酸盐","authors":"Yu Lin Hu, Yan Hui Lei, Yu Tao Zhang","doi":"10.1016/j.jscs.2024.101950","DOIUrl":null,"url":null,"abstract":"<div><div>Carbon dioxide as a C1 building block to synthesize α-alkylidene cyclic carbonates is an environmental and sustainable approach. In this work, we designed and synthesized a type of multifunctional magnetic MOF nanocomposite catalysts, which could realize the carboxylic cyclization of CO<sub>2</sub> and propargylic alcohols into α-alkylidene cyclic carbonates under solvent-free conditions. Among all the prepared nanocomposites, the MnFe<sub>2</sub>O<sub>4</sub>@SiO<sub>2</sub>@Cu-MOF nanocomposite is the best in catalytic activity combined with the tetrabutylphosphonium acetate ([Bu<sub>4</sub>P]OAc) ionic liquid cocatalyst. The catalytic system MnFe<sub>2</sub>O<sub>4</sub>@SiO<sub>2</sub>@Cu-MOF/[Bu<sub>4</sub>P]OAc displayed excellent performance in catalyzing the carboxylic cyclization of CO<sub>2</sub> and different propargylic alcohols, and a series of α-alkylidene cyclic carbonates were obtained in high to excellent yields (88 ∼ 98 %) under mild reaction conditions (0.2 MPa, 35 °C). In addition, the two-component catalytic system had high stability and reusability, and can be easily separated and reused up to six consecutive cycles without considerable decrease in catalytic activity. Moreover, using the ionic liquid [Bu<sub>4</sub>P]OAc as the cocatalyst, the nanocomposite had good substrate adaptability for the catalytic carboxylic cyclization, which opens interesting prospects for the development of new magnetic MOF nanocomposites as efficient heterogeneous catalysts for the chemical transformation of CO<sub>2</sub> into value-added chemicals.</div></div>","PeriodicalId":16974,"journal":{"name":"Journal of Saudi Chemical Society","volume":"28 6","pages":"Article 101950"},"PeriodicalIF":5.8000,"publicationDate":"2024-10-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Novel and reusable magnetic MOF nanocomposite coupled ionic liquid-promoted efficient chemical fixation of CO2 into α-alkylidene cyclic carbonates\",\"authors\":\"Yu Lin Hu, Yan Hui Lei, Yu Tao Zhang\",\"doi\":\"10.1016/j.jscs.2024.101950\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Carbon dioxide as a C1 building block to synthesize α-alkylidene cyclic carbonates is an environmental and sustainable approach. In this work, we designed and synthesized a type of multifunctional magnetic MOF nanocomposite catalysts, which could realize the carboxylic cyclization of CO<sub>2</sub> and propargylic alcohols into α-alkylidene cyclic carbonates under solvent-free conditions. Among all the prepared nanocomposites, the MnFe<sub>2</sub>O<sub>4</sub>@SiO<sub>2</sub>@Cu-MOF nanocomposite is the best in catalytic activity combined with the tetrabutylphosphonium acetate ([Bu<sub>4</sub>P]OAc) ionic liquid cocatalyst. The catalytic system MnFe<sub>2</sub>O<sub>4</sub>@SiO<sub>2</sub>@Cu-MOF/[Bu<sub>4</sub>P]OAc displayed excellent performance in catalyzing the carboxylic cyclization of CO<sub>2</sub> and different propargylic alcohols, and a series of α-alkylidene cyclic carbonates were obtained in high to excellent yields (88 ∼ 98 %) under mild reaction conditions (0.2 MPa, 35 °C). In addition, the two-component catalytic system had high stability and reusability, and can be easily separated and reused up to six consecutive cycles without considerable decrease in catalytic activity. Moreover, using the ionic liquid [Bu<sub>4</sub>P]OAc as the cocatalyst, the nanocomposite had good substrate adaptability for the catalytic carboxylic cyclization, which opens interesting prospects for the development of new magnetic MOF nanocomposites as efficient heterogeneous catalysts for the chemical transformation of CO<sub>2</sub> into value-added chemicals.</div></div>\",\"PeriodicalId\":16974,\"journal\":{\"name\":\"Journal of Saudi Chemical Society\",\"volume\":\"28 6\",\"pages\":\"Article 101950\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-10-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Saudi Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1319610324001455\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Saudi Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1319610324001455","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
以二氧化碳为C1构筑基块合成α-亚烷基环碳酸盐是一种环保且可持续的方法。本研究设计并合成了一种多功能磁性 MOF 纳米复合催化剂,可在无溶剂条件下实现二氧化碳与丙炔醇的羧基环化反应生成α-亚烷基环碳酸盐。在所有制备的纳米复合材料中,MnFe2O4@SiO2@Cu-MOF 纳米复合材料与四丁基醋酸鏻([Bu4P]OAc)离子液体催化剂结合的催化活性最好。MnFe2O4@SiO2@Cu-MOF/[Bu4P]OAc 催化体系在催化 CO2 和不同丙炔醇的羧基环化反应中表现出优异的性能,在温和的反应条件(0.2 兆帕,35 °C)下,以高至优异的收率(88 ∼ 98 %)获得了一系列α-亚烷基环碳酸盐。此外,该双组分催化体系具有很高的稳定性和重复使用性,可轻松分离并重复使用长达六个连续循环,而不会显著降低催化活性。此外,以离子液体[Bu4P]OAc 为助催化剂,该纳米复合材料对催化羧基环化具有良好的底物适应性,这为开发新型磁性 MOF 纳米复合材料作为将 CO2 化学转化为高附加值化学品的高效异相催化剂开辟了有趣的前景。
Novel and reusable magnetic MOF nanocomposite coupled ionic liquid-promoted efficient chemical fixation of CO2 into α-alkylidene cyclic carbonates
Carbon dioxide as a C1 building block to synthesize α-alkylidene cyclic carbonates is an environmental and sustainable approach. In this work, we designed and synthesized a type of multifunctional magnetic MOF nanocomposite catalysts, which could realize the carboxylic cyclization of CO2 and propargylic alcohols into α-alkylidene cyclic carbonates under solvent-free conditions. Among all the prepared nanocomposites, the MnFe2O4@SiO2@Cu-MOF nanocomposite is the best in catalytic activity combined with the tetrabutylphosphonium acetate ([Bu4P]OAc) ionic liquid cocatalyst. The catalytic system MnFe2O4@SiO2@Cu-MOF/[Bu4P]OAc displayed excellent performance in catalyzing the carboxylic cyclization of CO2 and different propargylic alcohols, and a series of α-alkylidene cyclic carbonates were obtained in high to excellent yields (88 ∼ 98 %) under mild reaction conditions (0.2 MPa, 35 °C). In addition, the two-component catalytic system had high stability and reusability, and can be easily separated and reused up to six consecutive cycles without considerable decrease in catalytic activity. Moreover, using the ionic liquid [Bu4P]OAc as the cocatalyst, the nanocomposite had good substrate adaptability for the catalytic carboxylic cyclization, which opens interesting prospects for the development of new magnetic MOF nanocomposites as efficient heterogeneous catalysts for the chemical transformation of CO2 into value-added chemicals.
期刊介绍:
Journal of Saudi Chemical Society is an English language, peer-reviewed scholarly publication in the area of chemistry. Journal of Saudi Chemical Society publishes original papers, reviews and short reports on, but not limited to:
•Inorganic chemistry
•Physical chemistry
•Organic chemistry
•Analytical chemistry
Journal of Saudi Chemical Society is the official publication of the Saudi Chemical Society and is published by King Saud University in collaboration with Elsevier and is edited by an international group of eminent researchers.