期刊
ACS NANO
卷 9, 期 4, 页码 4006-4016出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.5b01308
关键词
zeolite; MFI; core-shell; epitaxy; passivation; heterogeneous catalysis
类别
资金
- American Chemical Society [PRF 52422-DNI5]
- National Science Foundation [CAREER 1151098]
- Welch Foundation [E-1794]
- NIFA-USDA BRDI [2012-10008-20271]
- Department of Energy [DE-EE0006287]
- DOE Early Career Research Program [DE-SC0011983]
- Directorate For Engineering
- Div Of Chem, Bioeng, Env, & Transp Sys [1151098] Funding Source: National Science Foundation
- U.S. Department of Energy (DOE) [DE-SC0011983] Funding Source: U.S. Department of Energy (DOE)
The design of materials with spatially controlled chemical composition has potential advantages for wide-reaching applications that span energy to medicine. Here, we present a method for preparing a core shell aluminosilicate zeolite with continuous translational symmetry of nanopores and an epitaxial shell of tunable thickness that passivates Brasted acid sites associated with framework Al on exterior surfaces. For this study, we selected the commercially relevant MFI framework type and prepared core shell particles consisting of an aluminosilicate core (ZSM-5) and a siliceous shell (silicalite-1). Transmission electron microscopy and gas adsorption studies confirmed that silicalite-1 forms an epitaxial layer on ZSM-5 crystals without blocking pore openings. Scanning electron microscopy and dynamic light scattering were used in combination to confirm that the shell thickness can be tailored with nanometer resolution (e.g., 5-20 nm). X-ray photoelectron spectroscopy and temperature-programmed desorption measurements revealed the presence of a siliceous shell, while probe reactions using molecules that were either too large or adequately sized to access MFI pores confirmed the uniform shell coverage. The synthesis of ZSM-5@silicalite-1 offers a pathway for tailoring the physicochemical properties of MFI-type materials, notably in the area of catalysis, where surface passivation can enhance product selectivity without sacrificing catalyst activity. The method described herein may prove to be a general platform for zeolite core shell design with potentially broader applicability to other porous materials.
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