Confinement of atomically dispersed Ce in dealuminated beta zeolite for selective C–C coupling and deoxygenation

IF 10.7 Q1 CHEMISTRY, PHYSICAL

Chem Catalysis Pub Date : 2026-02-24 DOI:10.1016/j.checat.2025.101628

Vannessa Caballero, Wenda Hu, Hao Xu, Houqian Li, Huamin Wang, Jinshu Tian, Mingwu Tan, Konstantin Khivantsev, Yong Wang

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Abstract

The acetone-to-isobutene reaction is a key step in the ethanol cascade process toward high-value chemicals. However, the effects of spatial confinement and the role of cerium (Ce) species remain poorly understood. Here, we reveal that Ce-incorporated dealuminated beta zeolite (CedeAlBEA) exhibits exceptional isobutene selectivity when Ce species are atomically dispersed within the BEA framework. Spectroscopy analyses show that isolated Ce atoms provide optimal Lewis acidity for facilitating selective isobutene formation. In contrast, increasing Ce loading leads to the formation of CeO₂ nanoparticles, promoting mesityl oxide (MSO) as a byproduct. The Ce species in CedeAlBEA enhance C–C coupling and deoxygenation selectivity, whereas mesoporous and non-porous supports favor MSO formation because of the weaker confinement effects. Kinetic experiments reveal that oxygen elimination is the rate-limiting step. This study highlights the critical role of confined, atomically dispersed Ce cations in the BEA framework in directing acetone throughout diacetone alcohol decomposition to isobutene.

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原子分散的铈在脱铝沸石中的约束选择性碳-碳偶联和脱氧

丙酮-异丁烯反应是乙醇级联生产高价值化学品的关键步骤。然而，空间限制的影响和铈（Ce）物种的作用仍然知之甚少。在这里，我们发现Ce掺杂的脱铝β沸石（CedeAlBEA）表现出特殊的异丁烯选择性，当Ce原子分散在BEA框架内时。光谱分析表明，分离的Ce原子为促进选择性异丁烯形成提供了最佳的刘易斯酸度。相反，增加Ce负载导致CeO2纳米颗粒的形成，促进二甲氧基氧化物（MSO）作为副产物。CedeAlBEA中的Ce物种增强了C-C偶联和脱氧选择性，而介孔和无孔载体由于约束效应较弱而有利于MSO的形成。动力学实验表明，氧消除是反应的限速步骤。这项研究强调了在BEA框架中受限制的、原子分散的Ce阳离子在整个二丙酮醇分解过程中指导丙酮生成异丁烯的关键作用。

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来源期刊

Chem Catalysis

CiteScore

10.50

自引率

6.40%

发文量

期刊介绍： Chem Catalysis is a monthly journal that publishes innovative research on fundamental and applied catalysis, providing a platform for researchers across chemistry, chemical engineering, and related fields. It serves as a premier resource for scientists and engineers in academia and industry, covering heterogeneous, homogeneous, and biocatalysis. Emphasizing transformative methods and technologies, the journal aims to advance understanding, introduce novel catalysts, and connect fundamental insights to real-world applications for societal benefit.