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J Am Chem Soc. 2019 Mar 6;141(9):3772-3776. doi: 10.1021/jacs.8b11734. Epub 2019 Feb 25.

Amino Acid-Assisted Construction of Single-Crystalline Hierarchical Nanozeolites via Oriented-Aggregation and Intraparticle Ripening.

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State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry , Jilin University , 2699 Qianjin Street , Changchun 130012 , P. R. China.
School of Physical Science and Technology , ShanghaiTech University , Shanghai 201210 , P. R. China.
Shanghai Key Laboratory of Green Chemistry and Chemical Process, School of Chemistry and Molecular Engineering , East China Normal University , North Zhongshan Road 3663 , Shanghai 200062 , P. R. China.
International Center of Future Science, Jilin University , 2699 Qianjin Street , Changchun 130012 , P. R. China.


Hierarchical nanozeolites are highly desired for heavy oil conversion because of their fast mass transfer, good site accessibility, and short diffusion length compared with their conventional counterparts. Here, we provide a facile amino acid-assisted strategy to synthesize hierarchical ZSM-5 (MFI) zeolite nanocrystals by two-step crystallization in a concentrated gel system. Strikingly, each virus-like zeolite nanoparticle with abundant interconnected intracrystalline mesopores is a high-quality single crystal that is defect-free as confirmed by electron diffraction and NMR analysis. By utilizing advanced electron microscopy techniques, we have studied the evolution process of single-crystalline hierarchical ZSM-5 nanocrystals that involves oriented aggregation of protozeolitic nanoparticles formed at low temperature followed by intraparticle ripening at high temperature. The as-prepared hierarchical Ni@ZSM-5 catalysts exhibit superior catalytic performance in hydrodeoxygenation of stearic acid and palm oil.


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