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Controlled synthesis of ZSM-5 zeolite with an unusual Al distribution in framework from natural aluminosilicate mineral
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2020-06-07 , DOI: 10.1016/j.micromeso.2020.110357
Yanni Zhou , Haiyan Liu , Xiaorong Rao , Yuanyuan Yue , Haibo Zhu , Xiaojun Bao

Precisely tuning the location of Al atoms in zeolite framework that plays a critical role in determining the catalytic performance of zeolite based catalysts has attracted considerable attention. In this article, we present an organotemplate-free approach for the controllable synthesis of ZSM-5 zeolite with a high content of Al pairs selectively located at the channel intersections, which is achieved by using a submolten salt (SMS) depolymerized rectorite as both the Al source and heteropical crystalline seeds. The quasi in-situ characterizations tracking the zeolite crystallization process reveal that the depolymerized rectorite with abundant oligomeric aluminosilicate species and Al–O-(Si–O)1,2-Al sequences plays dual roles in the synthesis of ZSM-5 zeolite. These oligomeric aluminosilicate species like 5- and 6-membered ring structures serve as the crystalline seeds to promote the zeolite nucleation; simultaneously, the Al–O-(Si–O)1,2-Al sequences are in-situ transformed into the final zeolite framework leading to the generation of numerous Al pairs selectively located at the channel intersections. Such an unusual Al distribution endows the synthesized ZSM-5 zeolite with excellent catalytic performance in methanol to aromatics (MTA) reaction. Our strategy provides a sustainable and efficient way to design and synthesize high-performance zeolites with special framework Al distributions for catalytic applications.



中文翻译:

从天然铝硅酸盐矿物受控合成ZSM-5沸石的骨架中分布异常的Al

精确调节沸石骨架中Al原子的位置在决定沸石基催化剂的催化性能方面起着至关重要的作用,引起了人们的广泛关注。在本文中,我们提出了一种可控合成ZSM-5沸石的无有机模板方法,该沸石具有高含量的Al对,选择性地位于通道交叉处,这是通过使用亚熔融盐(SMS)解聚累托石来实现的。铝源和异型晶种。跟踪沸石结晶过程的准原位表征表明,解聚的累托石具有丰富的低聚硅铝酸盐种类和Al–O-(Si–O)1,2-A1序列在ZSM-5沸石的合成中起双重作用。这些低聚的铝硅酸盐物质,如5元和6元环结构,是促进沸石成核的晶种。同时,将Al–O–(Si–O)1,2 – Al序列原位转化为最终的沸石骨架,从而导致生成大量选择性地位于通道交叉点的Al对。这种异常的Al分布使合成的ZSM-5沸石在甲醇与芳烃(MTA)反应中具有出色的催化性能。我们的策略为设计和合成具有特殊骨架Al分布的高性能沸石提供了一种可持续,高效的方法,用于催化应用。

更新日期:2020-06-07
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