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Creation of Al‐Enriched Mesoporous ZSM‐5 Nanoboxes with High Catalytic Activity: Converting Tetrahedral Extra‐Framework Al into Framework Sites by Post Treatment
Angewandte Chemie International Edition ( IF 16.6 ) Pub Date : 2020-03-11 , DOI: 10.1002/anie.202002416
Yilai Jiao 1 , Luke Forster 2 , Shaojun Xu 2 , Huanhao Chen 2 , Jingfeng Han 3 , Xuqing Liu 4 , Yangtao Zhou 1 , Jinming Liu 1 , Jinsong Zhang 1 , Jihong Yu 5 , Carmine D’Agostino 6 , Xiaolei Fan 7
Affiliation  

ZSM‐5 zeolite nanoboxes with accessible meso‐micro‐pore architecture and strong acid sites are important in relevant heterogeneous catalysis suffering from mass transfer limitations and weak acidities. Rational design of parent zeolites with concentrated and non‐protective coordination of Al species can facilitate post‐synthetic treatment to produce mesoporous ZSM‐5 nanoboxes. In this work, a simple and effective method was developed to convert parent MFI zeolites with tetrahedral extra‐framework Al into Al‐enriched mesoporous ZSM‐5 nanoboxes with low silicon‐to‐aluminium ratios of ≈16. The parent MFI zeolite was prepared by rapid ageing of the zeolite sol gel synthesis mixture. The accessibility to the meso‐micro‐porous intra‐crystalline network was probed systematically by comparative pulsed field gradient nuclear magnetic resonance diffusion measurements, which, together with the strong acidity of nanoboxes, provided superb catalytic activity and longevity in hydrocarbon cracking for propylene production.

中文翻译:

具有高催化活性的富铝介孔ZSM-5纳米盒的创建:通过后处理将四面体骨架外铝转化为骨架位点

ZSM-5分子筛nanoboxes配有无障碍-微孔隙结构和强酸位在传质限制和弱酸度有关多相催化痛苦重要。合理设计具有高浓度和非保护性配位的Al物种的母体沸石可以促进合成后处理,以产生中孔ZSM-5纳米盒。在这项工作中,开发了一种简单有效的方法,将具有四面体骨架Al的母体MFI沸石转化为硅铝比低至≈16的富含Al的介孔ZSM-5纳米盒。通过快速老化沸石溶胶凝胶合成混合物来制备母体MFI沸石。中的可及性通过比较脉冲场梯度核磁共振扩散测量系统地探测了微孔晶体内部网络,该网络与纳米盒的强酸性一起,为丙烯生产的烃裂化提供了极好的催化活性和寿命。
更新日期:2020-03-11
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