Carbocation chemistry confined in zeolites: spectroscopic and theoretical characterizations,Chemical Society Reviews

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Carbocation chemistry confined in zeolites: spectroscopic and theoretical characterizations
Chemical Society Reviews ( IF 40.4 ) Pub Date : 2022-05-10 , DOI: 10.1039/d1cs00966d
Wei Chen ₁ , Xianfeng Yi ₁ , Zhiqiang Liu ₁ , Xiaomin Tang ₁ , Anmin Zheng _{1,

2}

Affiliation

Acid-catalyzed reactions inside zeolites are one type of broadly applied industrial reactions, where carbocations are the most common intermediates of these reaction processes, including methanol to olefins, alkene/aromatic alkylation, and hydrocarbon cracking/isomerization. The fundamental research on these acid-catalyzed reactions is focused on the stability, evolution, and lifetime of carbocations under the zeolite confinement effect, which greatly affects the efficiency, selectivity and deactivation of zeolite catalysts. Therefore, a profound understanding of the carbocations confined in zeolites is not only beneficial to explain the reaction mechanism but also drive the design of new zeolite catalysts with ideal acidity and cages/channels. In this review, we provide both an in-depth understanding of the stabilization of carbocations by the pore confinement effect and summary of the advanced characterization methods to capture carbocations in zeolites, including UV-vis spectroscopy, solid-state NMR, fluorescence microscopy, IR spectroscopy and Raman spectroscopy. Also, we clarify the relationship between the activity and stability of carbocations in zeolite-catalyzed reactions, and further highlight the role of carbocations in various hydrocarbon conversion reactions inside zeolites with diverse frameworks and varying acidic properties.

中文翻译：

限制在沸石中的碳阳离子化学：光谱和理论表征

沸石内的酸催化反应是一种广泛应用的工业反应，其中碳阳离子是这些反应过程中最常见的中间体，包括甲醇制烯烃、烯烃/芳烃烷基化和烃裂化/异构化。这些酸催化反应的基础研究集中在沸石限制效应下碳阳离子的稳定性、演化和寿命，这极大地影响了沸石催化剂的效率、选择性和失活。因此，深入了解限制在沸石中的碳阳离子不仅有助于解释反应机理，而且有助于设计具有理想酸度和笼/通道的新型沸石催化剂。在本次审查中，我们提供了对通过孔限制效应稳定碳阳离子的深入理解，并总结了在沸石中捕获碳阳离子的先进表征方法，包括紫外可见光谱、固态核磁共振、荧光显微镜、红外光谱和拉曼光谱. 此外，我们阐明了碳阳离子在沸石催化反应中的活性和稳定性之间的关系，并进一步强调了碳阳离子在具有不同骨架和不同酸性性质的沸石内部的各种烃转化反应中的作用。

更新日期：2022-05-10

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