Enhanced aromatic selectivity using the core–shell synergistic effects of HZSM-5/SAPO-5 zeolites in isobutane conversion

Journal of Physics and Chemistry of Solids(2021)

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摘要
HZSM-5 molecular sieves are efficient catalysts in the aromatization of light hydrocarbons and the fabrication of HZSM-5-based core–shell composites has become an important strategy to improve their catalytic performance due to the simultaneous modification of the acidity and pore structures in the catalyst. In this paper, HZSM-5/SAPO-5 (CSZP and CSZC) were synthesized via a two-stage crystallization process using PDDA and CTAB as modifiers of HZSM-5, respectively. The structure, acidity, and the weight of carbon deposition of the resulting molecular sieves catalysts were characterized using various methods and their catalytic behavior in isobutane aromatization investigated. The results show that CSZP exhibits a perfect core–shell structure with a uniform and thin shell composed of nano-SAPO-5, while CSZC has an irregular coat configuration with HZSM-5 covered by a rough and thick shell consisting of flaky micro-SAPO-5 crystals. The introduction of SAPO-5 via an in-situ synthesis decreases the Brønsted acidity of the catalysts to different extents and provides a large number of intergranular mesopores due to the stacking of SAPO-5 on the surface of HZSM-5, which is favorable toward improving the BTEX selectivity (benzene, toluene, ethylbenzene, and xylene) and catalytic stability over CSZP and CSZC. Meanwhile, CSZP has more competitive advantages than CSZC in promoting the mass transfer efficiency due to its significantly thinner shell than CSZC, which combined with its moderate acidity and appropriate mesopore structure result in its excellent selectivity and stability during the aromatization of isobutane.
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关键词
HZSM-5/SAPO-5 core–shell molecular sieves,Surfactant-assisted synthesis,Two-stage crystallization,Isobutane aromatization
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