Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA

Boal, Ben W.; Schmidt, Joel E.; Deimund, Mark A.; Deem, Michael W.; Henling, Lawrence M.; Brand, Stephen K.; Zones, Stacey I.; Davis, Mark E.

doi:10.1021/acs.chemmater.5b03579

Cited by 82 publications

(93 citation statements)

References 23 publications

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“…In addition to STW, numerous other phases were produced without significant variation in synthesis conditions, including LTA, RTH, IWV, CSV, as well as several phases that could not be identified or consisted of layered organosilicate materials. Synthesis of these microporous materials is not unexpected, because they have all been shown to be derived from similarly shaped imidazole-based OSDAs under crystallization conditions similar to those reported here (25)(26)(27)(28)32).…”

Section: Resultssupporting

confidence: 59%

“…This work demonstrated the feasibility of a priori predicting chemically synthesizable monoquaternary, imidazolium OSDAs to create a specified, fluoride-mediated, pure-silica framework. Additionally, STW has been reported to form using diquaternary imidazolium-based OSDAs that are of sufficient size to conform to 10MR channel structure, implying more rigid, chiral analogs may be included in the framework of STW, and may potentially impart structural chirality (24)(25)(26)(27)(28). Here, we implemented the previously published computational method implemented by Schmidt et al (24) and Pophale et al (29) and used the molecular design constraints suggested by Davis and Lobo (15).…”

Section: Resultsmentioning

confidence: 99%

“…S3). Additionally, 19 F, 29 Si, and 27 Al solid-state NMR (SS NMR) spectra, a representative thermogravimetric analysis, and a selection of scanning electron micrographs are listed as supporting characterizations (SI Appendix, Figs. S4-S8).…”

Section: Resultsmentioning

confidence: 99%

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Enantiomerically enriched, polycrystalline molecular sieves

Brand

Schmidt

Deem

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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Zeolite and zeolite-like molecular sieves are being used in a large number of applications such as adsorption and catalysis. Achievement of the long-standing goal of creating a chiral, polycrystalline molecular sieve with bulk enantioenrichment would enable these materials to perform enantioselective functions. Here, we report the synthesis of enantiomerically enriched samples of a molecular sieve. Enantiopure organic structure directing agents are designed with the assistance of computational methods and used to synthesize enantioenriched, polycrystalline molecular sieve samples of either enantiomer. Computational results correctly predicted which enantiomer is obtained, and enantiomeric enrichment is proven by high-resolution transmission electron microscopy. The enantioenriched and racemic samples of the molecular sieves are tested as adsorbents and heterogeneous catalysts. The enantioenriched molecular sieves show enantioselectivity for the ring opening reaction of epoxides and enantioselective adsorption of 2-butanol (the R enantiomer of the molecular sieve shows opposite and approximately equal enantioselectivity compared with the S enantiomer of the molecular sieve, whereas the racemic sample of the molecular sieve shows no enantioselectivity). chirality | zeolite | asymmetric catalysis | chiral adsorption

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Section: Resultssupporting

confidence: 59%

Section: Resultsmentioning

confidence: 99%

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Enantiomerically enriched, polycrystalline molecular sieves

Brand

Schmidt

Deem

et al. 2017

Proc. Natl. Acad. Sci. U.S.A.

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116

140

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“… Initial propane selectivities (time‐on‐stream=7–10 min) as a function of tetrahedral Si/Al for zeolite catalysts. The initial propane data points for SSZ‐17, RTH, LTA, Rho, SSZ‐13, and SSZ‐39 are from previous literature reports at the same reaction conditions.…”

Section: Resultsmentioning

confidence: 99%

“…Figure 9. Product selectivities of zeolitecatalysts compared to SAPO-34.The selectivity valuesa re obtained by averaging hydrocarbon selectivities for conversions of methanoli nthe range of 98-100%.S electivity data of SSZ-17 [7] (LEV),S SZ-39 [6] (AEI), SSZ-50 [31] (RTH), LTA, [32] and Rho [33] are from previous literature reports at the same reaction conditions. ChemPhysChem 2018, 19,412 -419 www.chemphyschem.org…”

Section: Resultsmentioning

confidence: 99%

Further Studies on How the Nature of Zeolite Cavities That Are Bounded by Small Pores Influences the Conversion of Methanol to Light Olefins

et al. 2018

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A series of small-pore zeolites are synthesized and investigated as catalysts for the methanol-to-olefins (MTO) reaction. Small-pore zeolites SSZ-13, SSZ-16, SSZ-27, SSZ-28, SSZ-52, SSZ-98, SSZ-99, SSZ-104, SSZ-105 and an ITQ-3-type material are synthesized, and the results from their use as catalytic materials in the MTO reaction compared to those obtained from SAPO-34. The production of propane that tends to correlate with catalytic material lifetime (higher initial propane yields lead to shorter lifetimes) declines with increasing Si/Al (as has been observed previously for SSZ-13), and a larger cage dimension leads to higher propane yields at a fixed Si/Al. Data from these materials and others reported previously, for example, SSZ-39 and Rho, that were tested at the same reaction conditions, revealed four different patterns of light olefin selectivities: 1) ethylene greater than propylene with low butene, for example, SSZ-17, SSZ-98, SSZ-105, 2) ethylene equal to propylene and low butene, for example, SAPO-34, SSZ-13, SSZ-16, SSZ-27, SSZ-52, SSZ-99, SSZ-104, 3) propylene greater than ethylene with butene similar to ethylene, for example, SSZ-28, SSZ-39, and 4) ethylene equal to propylene equal to butene, for example, Rho. No clear relationships between zeolite cage architecture and light olefin selectivity emerged from this investigation, although several trends are presented as suggestions for further study.

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Zeolite and Zeolite‐Like Materials

Chaikittisilp

Okubo

2017

Handbook of Solid State Chemistry

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Zeolites are crystalline microporous aluminosilicates that are constructed from corner‐sharing, tetrahedrally coordinatedTO4/2primary units (where T is a tetrahedral atom – silicon or aluminum). Thanks to their unique crystalline framework structures, well‐defined channels and cavities in a nanometer length scale, high surface areas, and several intrinsic properties arising from their anionic nature, zeolites have been widely used in various practical applications as adsorbents, ion exchangers, and catalysts. Zeolites have found their solid positions as key materials in industries and will continue to be the dominant industrial materials in future. Following a brief description of zeolite framework structures, in this chapter, the historical, fundamental, and recent aspects of zeolite synthesis are described. In addition, future prospects of zeolite toward the sustainable development are addressed.

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Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA

Cited by 82 publications

References 23 publications

Enantiomerically enriched, polycrystalline molecular sieves

Enantiomerically enriched, polycrystalline molecular sieves

Further Studies on How the Nature of Zeolite Cavities That Are Bounded by Small Pores Influences the Conversion of Methanol to Light Olefins

Zeolite and Zeolite‐Like Materials

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