Organic-Free Synthesis of High-Silica Zeolite Y with Aluminophosphate as the Aluminum Carrier

Qingdi Zhao, Jiejie Ling, Dr. Jilong Wang, Yan Gao, Hailang Liu, Zhenghan Zhang, Dr. Jingang Jiang, Prof. Akira Nakayama, Prof. Jian Li, Prof. Koki Muraoka, Prof. Peng Wu, Prof. Le Xu
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Abstract

The wide application of zeolite Y in petrochemical industry is well-known as one of the milestones in zeolite chemistry and heterogeneous catalysis. However, the traditional organic-free synthesis typically produces (hydro)thermally unstable zeolite Y with Si/Al atomic ratio (SAR) less than 2.5. Inspired by drug delivery process in which active components are kinetically controlled released, we develop a unique approach based on the pre-synthesized aluminum carrier to prepare one of the most siliceous zeolite Y with SAR up to 3.44 without using organics. The crystalline or amorphous aluminophosphates serve as the ideal carrier for the controlled incorporation of Al into zeolite framework during zeolite Y crystallization. Experimental and theoretical results reveal that the partial introduction of aluminophosphate as Al source would rationally regulate the crystallization kinetics, facilitating the formation of high-silica zeolite Y with random Al distribution. This approach enhances the hydrothermal stability and catalytic performance of zeolite Y in benchmark reaction.

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以磷酸铝为载体无有机合成高硅Y型沸石
Y型沸石在石油化工领域的广泛应用被认为是沸石化学和多相催化的里程碑之一。然而,传统的无有机合成通常产生(水)热不稳定的Y沸石,Si/Al原子比(SAR)小于2.5。受药物释放过程中活性成分被动力学控制释放的启发,我们开发了一种独特的方法,基于预合成的铝载体,制备了一种硅质含量最高的Y型分子筛,其SAR高达3.44,而不使用有机物。在Y型沸石结晶过程中,结晶或无定形的磷酸铝作为理想的载体,将Al控制在沸石骨架中。实验和理论结果表明,部分引入磷酸铝作为Al源可以合理调节结晶动力学,有利于形成Al随机分布的高硅Y型沸石。该方法提高了Y沸石在基准反应中的水热稳定性和催化性能。
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来源期刊
Angewandte Chemie
Angewandte Chemie 化学科学, 有机化学, 有机合成
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