期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 22, 期 23, 页码 7895-7905出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201504813
关键词
mesoporous materials; penetrating mesopores; scalable synthesis; single crystalline; zeolites
资金
- National Basic Research Program of China [2013CB933200]
- China National Funds for Distinguished Young Scientists [51225202]
- Natural Science Foundation of China [U1510107]
- State Key Laboratory of Heavy Oil Processing [SKLOP201402003]
Hierarchically structured zeolites (HSZs) have gained much academic and industrial interest owing to their multiscale pore structures and consequent excellent performances in varied chemical processes. Although a number of synthetic strategies have been developed in recent years, the scalable production of HSZs single crystals with penetrating and three-dimensionally (3-D) interconnected mesopore systems but without using a mesoscale template is still a great challenge. Herein, based on a steam-assisted crystallization (SAC) method, we report a facile and scalable strategy for the synthesis of single-crystalline ZSM-5 HSZs by using only a small amount of micropore-structure-directing agents (i.e., tetrapropylammonium hydroxide). The synthesized materials exhibited high crystallinity, a large specific surface area of 468 m(2) g(-1), and a pore volume of 0.43 cm(3) g(-1) without sacrificing the microporosity (approximate to 0.11 cm(3) g(-1)) in a product batch up to 11.7 g. Further, a kinetically controlled nucleation-growth mechanism is proposed for the successful synthesis of single-crystalline ZSM-5 HSZs with this novel process. As expected, compared with the conventional microporous ZSM-5 and amorphous mesoporous Al-MCM-41 counterparts, the synthesized HSZs exhibited significantly enhanced activity and stability and prolonged lifetime in model reactions, especially when bulky molecules were involved.
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