High-Silica, Enantiomerically Enriched STW-Type Molecular Sieves

被引:0
作者
Park, Youngkyu [1 ]
Alshafei, Faisal H. [1 ,2 ]
De Moraes, Lygia Silva [3 ]
Rodriguez, Isabel Hernandez [3 ]
Deem, Michael W. [4 ,5 ]
Nelson, Hosea M. [3 ]
Davis, Mark E. [1 ]
机构
[1] CALTECH, Chem Engn, Pasadena, CA 91125 USA
[2] MIT, Dept Chem Engn, Cambridge, MA 02139 USA
[3] CALTECH, Div Chem & Chem Engn, Pasadena, CA 91125 USA
[4] SmartHealth Catalyzer Inc, Riverwoods, IL 60015 USA
[5] Certus LLC, Houston, TX 77002 USA
关键词
Catalysis; -; Enantiomers; Enantioselectivity; Microcrystals; Silicates; Synthesis; (chemical);
D O I
10.1021/acs.chemmater.4c01792
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
Enantiomerically enriched molecular sieves can provide new opportunities for enantioselective catalysis and adsorption. The potential of using these materials for practical applications relies on the preparation of stable materials that can survive the rigors of use and regeneration. Reported enantiomerically enriched STW-type molecular sieves contain large amounts of Ge that limit the structural stability. Higher Si-containing STW-type molecular sieves will have enhanced stability, which should enable practical application. To achieve high-silica framework composition within enantiomerically enriched STW-type molecular sieves, a chiral organic structure-directing agent (OSDA) is computationally designed based on predicted stabilization energy toward the STW framework that is superior to previously employed OSDAs. With enantiopure forms of the designed OSDA, the synthesis of enantiomerically enriched STW-type germanosilicate molecular sieves with the framework Si/Ge as high as 18 is achieved. This high-silica STW-type molecular sieve has a significantly higher Si framework composition from the previously reported enantiomerically enriched germanium-rich STW-type molecular sieve and exhibits stability upon thermal treatment to 800 degrees C. The absolute stereochemistry of the framework structure is characterized by the dynamical refinement of microcrystal electron diffraction data from several microcrystals. The enantioselective adsorption of 2-butanol is demonstrated over the high-silica, enantioenriched STW-type molecular sieve.
引用
收藏
页码:10552 / 10559
页数:8
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