Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA
Abstract
Zeolite A (LTA) has many large-scale uses in separations and ion exchange applications. Because of the high aluminum content and lack of high-temperature stability, applications in catalysis, while highly desired, have been extremely limited. Herein, we report a robust method to prepare pure-silica, aluminosilicate (product Si/Al = 12–42), and titanosilicate LTA in fluoride media using a simple, imidazolium- based organic structure-directing agent. The aluminosilicate material is an active catalyst for the methanol-to-olefins reaction with higher product selectivities to butenes as well as C5 and C6 products than the commercialized silicoalumniophosphate or zeolite analogue that both have the chabazite framework (SAPO- 34 and SSZ-13, respectively). Furthermore, the crystal structures of the as-made and calcined pure-silica materials were solved using singlecrystal X-ray diffraction, providing information about the occluded organics and fluoride as well as structural information.
- Authors:
-
- Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, United States
- Departments of Bioengineering and Physics & Astronomy, Rice University, Houston, Texas 77005, United States
- Chevron Energy Technology Company, Richmond, California 94802, United States
- Publication Date:
- Research Org.:
- Rice Univ., Houston, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1225234
- Alternate Identifier(s):
- OSTI ID: 1439315
- Grant/Contract Number:
- FG02-03ER15456
- Resource Type:
- Published Article
- Journal Name:
- Chemistry of Materials
- Additional Journal Information:
- Journal Name: Chemistry of Materials Journal Volume: 27 Journal Issue: 22; Journal ID: ISSN 0897-4756
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Boal, Ben W., Schmidt, Joel E., Deimund, Mark A., Deem, Michael W., Henling, Lawrence M., Brand, Stephen K., Zones, Stacey I., and Davis, Mark E. Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA. United States: N. p., 2015.
Web. doi:10.1021/acs.chemmater.5b03579.
Boal, Ben W., Schmidt, Joel E., Deimund, Mark A., Deem, Michael W., Henling, Lawrence M., Brand, Stephen K., Zones, Stacey I., & Davis, Mark E. Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA. United States. https://doi.org/10.1021/acs.chemmater.5b03579
Boal, Ben W., Schmidt, Joel E., Deimund, Mark A., Deem, Michael W., Henling, Lawrence M., Brand, Stephen K., Zones, Stacey I., and Davis, Mark E. Thu .
"Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA". United States. https://doi.org/10.1021/acs.chemmater.5b03579.
@article{osti_1225234,
title = {Facile Synthesis and Catalysis of Pure-Silica and Heteroatom LTA},
author = {Boal, Ben W. and Schmidt, Joel E. and Deimund, Mark A. and Deem, Michael W. and Henling, Lawrence M. and Brand, Stephen K. and Zones, Stacey I. and Davis, Mark E.},
abstractNote = {Zeolite A (LTA) has many large-scale uses in separations and ion exchange applications. Because of the high aluminum content and lack of high-temperature stability, applications in catalysis, while highly desired, have been extremely limited. Herein, we report a robust method to prepare pure-silica, aluminosilicate (product Si/Al = 12–42), and titanosilicate LTA in fluoride media using a simple, imidazolium- based organic structure-directing agent. The aluminosilicate material is an active catalyst for the methanol-to-olefins reaction with higher product selectivities to butenes as well as C5 and C6 products than the commercialized silicoalumniophosphate or zeolite analogue that both have the chabazite framework (SAPO- 34 and SSZ-13, respectively). Furthermore, the crystal structures of the as-made and calcined pure-silica materials were solved using singlecrystal X-ray diffraction, providing information about the occluded organics and fluoride as well as structural information.},
doi = {10.1021/acs.chemmater.5b03579},
journal = {Chemistry of Materials},
number = 22,
volume = 27,
place = {United States},
year = {Thu Nov 05 00:00:00 EST 2015},
month = {Thu Nov 05 00:00:00 EST 2015}
}
https://doi.org/10.1021/acs.chemmater.5b03579
Web of Science
Works referenced in this record:
Benzylimidazolium cations as zeolite structure-directing agents. Differences in performance brought about by a small change in size
journal, January 2013
- Rojas, Alex; Gómez-Hortigüela, Luis; Camblor, Miguel A.
- Dalton Trans., Vol. 42, Issue 7
Impact of Zeolites on the Petroleum and Petrochemical Industry
journal, May 2009
- Vermeiren, W.; Gilson, J. -P.
- Topics in Catalysis, Vol. 52, Issue 9
Translating new materials discoveries in zeolite research to commercial manufacture
journal, October 2011
- Zones, S. I.
- Microporous and Mesoporous Materials, Vol. 144, Issue 1-3
Computational prediction of chemically synthesizable organic structure directing agents for zeolites
journal, January 2013
- Pophale, Ramdas; Daeyaert, Frits; Deem, Michael W.
- Journal of Materials Chemistry A, Vol. 1, Issue 23
Studies on the Role of Fluoride Ion vs Reaction Concentration in Zeolite Synthesis
journal, January 2005
- Zones, Stacey I.; Darton, Richard J.; Morris, Russell
- The Journal of Physical Chemistry B, Vol. 109, Issue 1
An Extra-Large-Pore Zeolite with Intersecting 18-, 12-, and 10-Membered Ring Channels
journal, July 2014
- Chen, Fei-Jian; Xu, Yan; Du, Hong-Bin
- Angewandte Chemie International Edition, Vol. 53, Issue 36
Facile Preparation of Aluminosilicate RTH across a Wide Composition Range Using a New Organic Structure-Directing Agent
journal, December 2014
- Schmidt, Joel E.; Deimund, Mark A.; Davis, Mark E.
- Chemistry of Materials, Vol. 26, Issue 24
Catalytic Applications of Zeolites in Chemical Industry
journal, April 2009
- Yilmaz, Bilge; Müller, Ulrich
- Topics in Catalysis, Vol. 52, Issue 6-7
Facile and reproducible synthesis of ITQ-29 zeolite by using Kryptofix 222 as the structure directing agent
journal, May 2010
- Huang, Aisheng; Weidenthaler, Claudia; Caro, Jürgen
- Microporous and Mesoporous Materials, Vol. 130, Issue 1-3
Pure-silica LTA, CHA, STT, ITW, and -SVR thin films and powders for low-k applications
journal, May 2010
- Hunt, Heather K.; Lew, Christopher M.; Sun, Minwei
- Microporous and Mesoporous Materials, Vol. 130, Issue 1-3
Supramolecular self-assembled molecules as organic directing agent for synthesis of zeolites
journal, September 2004
- Corma, Avelino; Rey, Fernando; Rius, Jordi
- Nature, Vol. 431, Issue 7006
A Dynamic Organic Structuring-Directing Agent for Pure-Silica-Zeolite AST and LTA Syntheses
journal, January 2012
- Sun, Minwei; Hunt, Heather K.; Lew, Christopher M.
- Chinese Journal of Catalysis, Vol. 33, Issue 1
Effects of cage shape and size of 8-membered ring molecular sieves on their deactivation in methanol-to-olefin (MTO) reactions
journal, April 2008
- Park, Ji Won; Lee, Jae Youl; Kim, Kwang Soo
- Applied Catalysis A: General, Vol. 339, Issue 1
The synthesis of aluminophosphate and germanosilicate LTA using a triquaternary structure directing agent
journal, December 2014
- Schmidt, Joel E.; Zones, Stacey I.; Xie, Dan
- Microporous and Mesoporous Materials, Vol. 200
High resolution, quasi-equilibrium sorption studies of molecular sieves
journal, January 1990
- Hathaway, Paul E.; Davis, Mark E.
- Catalysis Letters, Vol. 5, Issue 4-6
Unraveling the Reaction Mechanisms Governing Methanol-to-Olefins Catalysis by Theory and Experiment
journal, April 2013
- Hemelsoet, Karen; Van der Mynsbrugge, Jeroen; De Wispelaere, Kristof
- ChemPhysChem, Vol. 14, Issue 8
Synthesis Strategies for Preparing Useful Small Pore Zeolites and Zeotypes for Gas Separations and Catalysis
journal, July 2013
- Moliner, Manuel; Martínez, Cristina; Corma, Avelino
- Chemistry of Materials, Vol. 26, Issue 1
A Rational Approach to the Ionothermal Synthesis of an AlPO4 Molecular Sieve with an LTA-Type Framework
journal, May 2010
- Fayad, Elie J.; Bats, Nicolas; Kirschhock, Christine E. A.
- Angewandte Chemie International Edition, Vol. 49, Issue 27
Steam-stable hydrophobic ITQ-29 molecular sieve membrane with H2 selectivity prepared by secondary growth using Kryptofix 222 as SDA
journal, January 2010
- Huang, Aisheng; Caro, Jürgen
- Chemical Communications, Vol. 46, Issue 41
Preparation of ITQ-29 (Al-free zeolite A) membranes
journal, April 2008
- Tiscornia, Inés; Valencia, Susana; Corma, Avelino
- Microporous and Mesoporous Materials, Vol. 110, Issue 2-3