通过内在修饰实现二氧化碳和双环氧化物环化反应的庚嗪基材料

IF 3 4区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY ChemPlusChem Pub Date : 2024-04-10 DOI:10.1002/cplu.202400154
Dr. Hongguang Liang, Dr. Xiaoyun Li, Prof. Junwei Wang, Prof. Qifeng Li, Assoc. Prof. Yuelan Feng, Prof. Maoqing Kang, Yingan Zhang
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引用次数: 0

摘要

为了将二氧化碳有效地转化为有价值的产品,人们对具有吸引力的氮化碳催化剂进行了广泛的研究。在这项工作中,我们采用内在改性策略设计了具有不同聚合度的庚嗪相关材料,并将其用于二氧化碳与双环氧化物 1,4-丁二醇二缩水甘油醚(BDODGE)的环化反应。我们初步发现,450°C 下制备的样品含有更多的水合烯丙基酚,表现出最佳性能。在不使用任何助催化剂和溶剂的情况下,140°C 20 小时的环氧化物转化率和相应的环碳酸盐选择性分别达到 93.1% 和 99.3%。催化测试结果表明,高催化活性取决于大尺寸多孔结构以及活性氨基和 -OH 基团的协同作用。水在维持特定结构和提供活性位点方面的作用已得到证实。此外,CN-450-W 催化剂还具有出色的回收稳定性。最后,还提出了一种合理的反应机理。
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The Heptazine-Based Materials through Intrinsically Modification for the Cycloaddition of CO2 and Bisepoxides

For the efficient utilization of CO2 into valuable product, the attractive carbon nitride catalysts have been widely studied. In this work, heptazine-related materials with varying degree of polymerization were designed by an intrinsically modification strategy and employed in the cycloaddition of CO2 with the bisepoxide 1, 4-butanediol diglycidyl ether (BDODGE). We initially figured out that the sample prepared at 450 °C contained more melem hydrate, exhibiting the best performance. The epoxides conversion and corresponding cyclic carbonates selectivity could achieve 93.1 % and 99.3 % at 140 °C for 20 h without any cocatalyst and solvent, respectively. Results of the catalytic tests suggested that the high catalytic activity was dependent on big size porous structure and the synergetic effect of active amino groups and −OH groups. The role of water in maintaining the specific structure and providing active site has been proved. Moreover, the CN-450-W catalyst exhibited outstanding recycling stability. And finally, a plausible reaction mechanism was proposed.

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来源期刊
ChemPlusChem
ChemPlusChem CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
5.90
自引率
0.00%
发文量
200
审稿时长
1 months
期刊介绍: ChemPlusChem is a peer-reviewed, general chemistry journal that brings readers the very best in multidisciplinary research centering on chemistry. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies. Fully comprehensive in its scope, ChemPlusChem publishes articles covering new results from at least two different aspects (subfields) of chemistry or one of chemistry and one of another scientific discipline (one chemistry topic plus another one, hence the title ChemPlusChem). All suitable submissions undergo balanced peer review by experts in the field to ensure the highest quality, originality, relevance, significance, and validity.
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