Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis
Abstract
Zeolites, having widespread applications in chemical industries, are often synthesized using organic templates. These can be cost-prohibitive, motivating investigations into their role in promoting crystallization. Herein, the relationship between framework structure, chemical composition, synthesis conditions and the conformation of the occluded, economical template tetraethylammonium (TEA+) has been systematically examined by experimental and computational means. The results show two distinct regimes of occluded conformer tendencies: 1) In frameworks with a large stabilization energy difference, only a single conformer was found (BEA, LTA and MFI). 2) In the frameworks with small stabilization energy differences (AEI, AFI, CHA and MOR), less than the interconversion of TEA+ in solution, a heteroatom-dependent (Al, B, Co, Mn, Ti, Zn) distribution of conformers was observed. Our findings demonstrate that host–guest chemistry principles, including electrostatic interactions and coordination chemistry, are as important as ideal pore-filling.
- Authors:
-
[1];
[1];
[2];
[1]
- Univ. of Utrecht (Netherlands). Debye Inst. for Nanomaterials Science
- Rice Univ., Houston, TX (United States). Dept. of Bioengineering and Physics and Dept. of Astronomy
- Publication Date:
- Research Org.:
- Rice Univ., Houston, TX (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Univ. of Utrecht (Netherlands); Netherlands Organization for Scientific Research (NWO); Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC); European Research Council (ERC)
- OSTI Identifier:
- 1429472
- Grant/Contract Number:
- FG02-03ER15456; 321140
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Angewandte Chemie (International Edition)
- Additional Journal Information:
- Journal Name: Angewandte Chemie (International Edition); Journal Volume: 55; Journal Issue: 52; Journal ID: ISSN 1433-7851
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING; 36 MATERIALS SCIENCE; computational chemistry; conformational analysis; host–guest systems; Raman spectroscopy; zeolites
Citation Formats
Schmidt, Joel E., Fu, Donglong, Deem, Michael W., and Weckhuysen, Bert M. Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis. United States: N. p., 2016.
Web. doi:10.1002/anie.201609053.
Schmidt, Joel E., Fu, Donglong, Deem, Michael W., & Weckhuysen, Bert M. Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis. United States. https://doi.org/10.1002/anie.201609053
Schmidt, Joel E., Fu, Donglong, Deem, Michael W., and Weckhuysen, Bert M. Tue .
"Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis". United States. https://doi.org/10.1002/anie.201609053. https://www.osti.gov/servlets/purl/1429472.
@article{osti_1429472,
title = {Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis},
author = {Schmidt, Joel E. and Fu, Donglong and Deem, Michael W. and Weckhuysen, Bert M.},
abstractNote = {Zeolites, having widespread applications in chemical industries, are often synthesized using organic templates. These can be cost-prohibitive, motivating investigations into their role in promoting crystallization. Herein, the relationship between framework structure, chemical composition, synthesis conditions and the conformation of the occluded, economical template tetraethylammonium (TEA+) has been systematically examined by experimental and computational means. The results show two distinct regimes of occluded conformer tendencies: 1) In frameworks with a large stabilization energy difference, only a single conformer was found (BEA, LTA and MFI). 2) In the frameworks with small stabilization energy differences (AEI, AFI, CHA and MOR), less than the interconversion of TEA+ in solution, a heteroatom-dependent (Al, B, Co, Mn, Ti, Zn) distribution of conformers was observed. Our findings demonstrate that host–guest chemistry principles, including electrostatic interactions and coordination chemistry, are as important as ideal pore-filling.},
doi = {10.1002/anie.201609053},
journal = {Angewandte Chemie (International Edition)},
number = 52,
volume = 55,
place = {United States},
year = {Tue Nov 22 00:00:00 EST 2016},
month = {Tue Nov 22 00:00:00 EST 2016}
}
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