Heteroatom‐Containing Zeolites as Solid Lewis Acid Catalysts for the Cycloaddition of CO2 to Epoxides

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL ChemCatChem Pub Date : 2024-09-09 DOI:10.1002/cctc.202401385
Bohai Gao, Weijie Li, Yuchao Chai, Guangjun Wu, Landong Li
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Abstract

The catalytic cycloaddition of CO2 to epoxides to produce valuable cyclic carbonates represents a simple and promising strategy for CO2 utilization, circumventing the ineffective CO2 reduction process. Despite current progresses, there remains an impending demand for highly‐active, cost‐effective and stable catalysts especially the ideal heterogeneous catalytic systems. Herein, we report the preparation of heteroatom‐containing zeolites through a two‐step process comprising of framework dealumination and subsequent heteroatom incorporation, and their catalytic applications in CO2 cycloaddition to epoxides. Characterization results reveal the successful incorporation of heteroatoms into framework to derive Lewis acidic M‐Beta zeolites (M=Ti, Zr or Hf). The as‐prepared M‐Beta Lewis acids show remarkable performance in the model reaction of CO2 cycloaddition to propylene oxide with the assistance of potassium iodide under solvent‐free conditions. The reaction parameters have been optimized employing Ti‐Beta catalyst and the substrate scope has been investigated. Finally, the impact of Lewis acidity on the cycloaddition reaction is discussed and the actual bifunctional Ti‐Beta/KI catalyst system is proposed, which is of important significance for the understanding of CO2 catalytic cycloaddition to epoxides.
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含异构体的沸石作为二氧化碳与环氧化物环化反应的固体路易斯酸催化剂
将二氧化碳催化环化加成到环氧化物中,生成有价值的环状碳酸盐,是一种简单而有前途的二氧化碳利用策略,可避免无效的二氧化碳还原过程。尽管目前取得了一些进展,但对高活性、高成本效益和稳定的催化剂,尤其是理想的异相催化体系的需求仍迫在眉睫。在此,我们报告了通过两步法制备含杂原子沸石的过程,包括框架脱铝和随后的杂原子加入,以及它们在环氧化物的 CO2 环加成中的催化应用。表征结果表明,杂原子成功地加入到框架中,从而得到了路易斯酸型 M-Beta 沸石(M=钛、锆或铪)。在无溶剂条件下,在碘化钾的帮助下,制备的 M-Beta 路易斯酸在二氧化碳与环氧丙烷的环加成模型反应中表现出了卓越的性能。利用 Ti-Beta 催化剂对反应参数进行了优化,并对底物范围进行了研究。最后,讨论了路易斯酸对环加成反应的影响,并提出了实际的双功能 Ti-Beta/KI 催化剂体系,这对理解 CO2 催化环加成环氧化物具有重要意义。
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来源期刊
ChemCatChem
ChemCatChem 化学-物理化学
CiteScore
8.10
自引率
4.40%
发文量
511
审稿时长
1.3 months
期刊介绍: With an impact factor of 4.495 (2018), ChemCatChem is one of the premier journals in the field of catalysis. The journal provides primary research papers and critical secondary information on heterogeneous, homogeneous and bio- and nanocatalysis. The journal is well placed to strengthen cross-communication within between these communities. Its authors and readers come from academia, the chemical industry, and government laboratories across the world. It is published on behalf of Chemistry Europe, an association of 16 European chemical societies, and is supported by the German Catalysis Society.
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