铝源种类对ZSM-5分子筛铝原子分布及丁烯裂解反应性能的影响

摘要/Abstract

摘要： 采用水热合成法分别以偏铝酸钠、拟薄水铝石、氢氧化铝和异丙醇铝为铝源制备了ZSM-5分子筛，结合理化性质表征与丁烯裂解催化性能测试，探究了铝源种类对分子筛骨架铝原子落位及丁烯裂解性能的影响。结果表明：铝源种类对分子筛晶体结构、孔道结构、表面形貌和总酸量影响较小，但对骨架铝原子分布影响显著；在合成体系中，与水解速率较慢的铝源（如拟薄水铝石和异丙醇铝）合成的分子筛相比，溶解速度较快的铝源（如偏铝酸钠）落位于直通形孔道（α位）的铝原子占比提高。丁烯催化裂解反应中，由于空间限制作用，骨架铝原子落位在α位占比高的分子筛的丙烯选择性高。进一步地，验证了ZSM-5分子筛酸中心分布与丁烯裂解催化性能的构效关系，为定向合成高性能催化剂提供了依据。

关键词: 分子筛, 酸性质, 骨架铝原子, 丙烯选择性, 水热合成法

Abstract: In this study, ZSM-5 zeolites were synthesized via the hydrothermal method using sodium metaaluminate,sodium hydroxide,pseudo-boehmite and aluminum isopropoxide as aluminum sources, respectively. Based on the characterization of physicochemical properties and the catalytic performance test of butene cracking, the effect of aluminum source types on the sitting of framework aluminum atoms and structure-activity relationship was investigated. The results showed that the type of aluminum source had little influence on the crystal structure, pore structure, surface morphology, and total acid amount of ZSM-5 zeolite. However, it exerted a significant effect on the distribution of framework aluminum atoms. In the research synthesis system, aluminum sources with higher solubility (e.g., sodium metaaluminate) compared to those with slower hydrolysis rates (e.g., pseudoboehmite and aluminum isopropoxide), the proportion of aluminum atoms located in the straight channels (α-sites) is increased. Due to spatial restriction, zeolites with a high proportion of framework aluminum atoms located at α-sites exhibit high propylene selectivity in butylene catalytic cracking reaction.This study not only verified the structure-activity relationship between the acid site distribution of ZSM-5 zeolites furtherly, and also provided a basis for the directional synthesis of high-performance catalyst for butylene catalytic cracking.

Key words: molecular sieve, acid property, framework aluminum atom, propylene selectivity, hydrothermal synthesis method

段绘州刘鑫辉吴一鹏熊小念吴韬. 铝源种类对ZSM-5分子筛铝原子分布及丁烯裂解反应性能的影响[J]. 石油炼制与化工, 2026, 57(2): 158-165.

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