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Title: Fluoride-free synthesis of a Sn-BEA catalyst by dry gel conversion

Journal Article · · Green Chemistry
DOI:https://doi.org/10.1039/c4gc02457e· OSTI ID:1385933

Sn containing molecular sieves with BEA topology (Sn-BEA) are active Lewis catalysts for a large variety of redox reactions. However, the synthesis of Sn-BEA often requires the use of toxic chemicals (e.g. hydrofluoric acid). In this study, we demonstrated that an active Sn-BEA catalyst can be directly synthesized in a non-fluoride medium via a dry gel conversion method with the aid of seed crystals. It was shown that seeding of zeolite BEA crystals can facilitate crystal growth and lead to BEA topology with framework Sn. Furthermore, it was found that ion-exchange with ammonium ions is indispensable to retain the crystal structure during calcination. The catalytic activity of the Sn-BEA catalyst was evaluated by the isomerization of glucose and reaction of pyruvaldehyde in the aqueous phase, and compared with the conventional hydrophobic Sn-BEA synthesized in a fluoride medium. The catalytic activity of the Sn-BEA synthesized in the absence of fluoride was found to be lower than that of the conventional Sn-BEA for catalyzing the isomerization of glucose in the aqueous phase, which could be attributed to its hydrophilic surface. For the reaction of pyruvaldehyde in the aqueous phase, the Sn-BEA synthesized in this study showed similar activity to the conventional hydrophobic Sn-BEA, indicating that the catalytic activity of Sn-BEA catalysts largely depends on the type of reactions. The current work provides the first example of direct preparation of a Sn-BEA catalyst in a caustic medium.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Catalysis Center for Energy Innovation (CCEI)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0001004
OSTI ID:
1385933
Journal Information:
Green Chemistry, Vol. 17, Issue 5; Related Information: CCEI partners with the University of Delaware (lead); Brookhaven National Laboratory; California Institute of Technology; Columbia University; University of Delaware; Lehigh University; University of Massachusetts, Amherst; Massachusetts Institute of Technology; University of Minnesota; Pacific Northwest National Laboratory; University of Pennsylvania; Princeton University; Rutgers University; ISSN 1463-9262
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 81 works
Citation information provided by
Web of Science

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Cited By (10)

Broadening the Scope for Fluoride-Free Synthesis of Siliceous Zeolites journal February 2018
Controllably Confined ZnO on USY Zeolites (USY@ZnO/Al 2 O 3 ) as Efficient Lewis Acid Catalysts for Baeyer-Villiger Oxidation journal April 2018
Glucose Isomerization and Epimerization over Metal‐Organic Frameworks with Single‐Site Active Centers journal February 2019
Fluoride-free and low concentration template synthesis of hierarchical Sn-Beta zeolites: efficient catalysts for conversion of glucose to alkyl lactate journal January 2017
Hydrothermal synthesis of Sn-Beta zeolites in F -free medium journal January 2018
Glucose isomerization in dioxane/water with Sn-β catalyst: improved catalyst stability and use for HMF production journal January 2019
Stoichiometric active site modification observed by alkali ion titrations of Sn-Beta journal January 2019
Sn–Al-USY for the valorization of glucose to methyl lactate: switching from hydrolytic to retro-aldol activity by alkaline ion exchange journal January 2019
Porous metallosilicates for heterogeneous, liquid-phase catalysis: perspectives and pertaining challenges journal February 2018
Broadening the Scope for Fluoride‐Free Synthesis of Siliceous Zeolites journal February 2018