Design of Hierarchical Zeolite Catalysts for the Manufacture of Polyurethane Intermediates
Design of Hierarchical Zeolite Catalysts for the Manufacture of Polyurethane Intermediates
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DOI：
10.1021/cs5017694
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发表时间：
2015-02
期刊：
影响因子：
12.9
通讯作者：
T. Keller;J. Arras;S. Wershofen;J. Pérez–Ramírez
中科院分区：
文献类型：
--
作者：
T. Keller;J. Arras;S. Wershofen;J. Pérez–Ramírez
This study undertakes the design of hierarchically structured zeolites for the synthesis of methylenedianiline (MDA) mixtures via the liquid-phase condensation of aniline with formaldehyde. Affordable acid and base treatments enabled the controlled generation of an auxiliary network of intracrystalline mesopores within commercial zeolites of different frameworks, among which the FAU topology is identified as superior. As the micropore structure of the zeolite can be preserved, the unique shape selectivity is retained while improved mass transport in the hierarchical crystals leads to a 7-fold increased activity and a 3-fold prolonged lifetime before thermal regeneration is necessary. The linear correlation between the MDA yield and the product of the Bronsted acidity and the external surface area emphasizes the need to balance acid site and pore quality in the design of an optimal catalyst. Hierarchical USY zeolites outperform the state-of-the-art delaminated zeolites and mesoporous aluminosilicates. Thes...
