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Title: Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis

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:
ORCiD logo [1] ; ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Univ. of Utrecht (Netherlands). Debye Inst. for Nanomaterials Science
  2. Rice Univ., Houston, TX (United States). Dept. of Bioengineering and Physics and Dept. of Astronomy
Publication Date:
Grant/Contract Number:
FG02-03ER15456; 321140
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
Research Org:
Rice Univ., Houston, TX (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Univ. of Utrecht (Netherlands); Netherlands Organization for Scientific Research (NWO); Netherlands Center for Multiscale Catalytic Energy Conversion (MCEC); European Research Council (ERC)
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
OSTI Identifier:
1429472

Schmidt, Joel E., Fu, Donglong, Deem, Michael W., and Weckhuysen, Bert M.. Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis. United States: N. p., 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. doi:10.1002/anie.201609053.
Schmidt, Joel E., Fu, Donglong, Deem, Michael W., and Weckhuysen, Bert M.. 2016. "Template-Framework Interactions in Tetraethylammonium-Directed Zeolite Synthesis". United States. doi: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 = {2016},
month = {11}
}

Works referenced in this record:

The Hydrothermal Synthesis of Zeolites: History and Development from the Earliest Days to the Present Time
journal, March 2003
  • Cundy, Colin S.; Cox, Paul A.
  • Chemical Reviews, Vol. 103, Issue 3, p. 663-702
  • DOI: 10.1021/cr020060i