Finned zeolite catalysts

被引:169
作者
Dai, Heng [1 ]
Shen, Yufeng [1 ]
Yang, Taimin [2 ]
Lee, Choongsze [3 ]
Fu, Donglong [4 ]
Agarwal, Ankur [1 ]
Le, Thuy Thanh [1 ]
Tsapatsis, Michael [3 ,5 ]
Palmer, Jeremy C. [1 ]
Weckhuysen, Bert M. [4 ]
Dauenhauer, Paul J. [3 ]
Zou, Xiaodong [2 ]
Rimer, Jeffrey D. [1 ]
机构
[1] Univ Houston, Dept Chem & Biomol Engn, Houston, TX 77004 USA
[2] Stockholm Univ, Dept Mat & Environm Chem, Stockholm, Sweden
[3] Univ Minnesota, Dept Chem Engn & Mat Sci, 421 Washington Ave SE, Minneapolis, MN 55455 USA
[4] Univ Utrecht, Debye Inst Nanomat Sci, Inorgan Chem & Catalysis Grp, Utrecht, Netherlands
[5] Johns Hopkins Univ, Dept Chem & Biomol Engn, Baltimore, MD USA
基金
瑞典研究理事会; 美国国家科学基金会; 欧洲研究理事会;
关键词
DIFFUSION; METHANOL; SILICALITE-1; CONVERSION; NANOSHEETS; CRYSTALLIZATION; HYDROCARBONS; TEMPERATURE; SELECTIVITY; MECHANISM;
D O I
10.1038/s41563-020-0753-1
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nanosized zeolites enable better catalytic performance; however, their synthesis is non-trivial. Here, a simple treatment is presented that enables the growth of nanosized fins on zeolites that act as pseudo-nanoparticles, reducing deactivation rates for methanol-to-hydrocarbon catalysis. There is growing evidence for the advantages of synthesizing nanosized zeolites with markedly reduced internal diffusion limitations for enhanced performances in catalysis and adsorption. Producing zeolite crystals with sizes less than 100 nm, however, is non-trivial, often requires the use of complex organics and typically results in a small product yield. Here we present an alternative, facile approach to enhance the mass-transport properties of zeolites by the epitaxial growth of fin-like protrusions on seed crystals. We validate this generalizable methodology on two common zeolites and confirm that fins are in crystallographic registry with the underlying seeds, and that secondary growth does not impede access to the micropores. Molecular modelling and time-resolved titration experiments of finned zeolites probe internal diffusion and reveal substantial improvements in mass transport, consistent with catalytic tests of a model reaction, which show that these structures behave as pseudo-nanocrystals with sizes commensurate to that of the fin. This approach could be extended to the rational synthesis of other zeolite and aluminosilicate materials.
引用
收藏
页码:1074 / +
页数:9
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