Boal, Ben W. and Deem, Michael W. and Xie, Dan and Kang, Jong Hun and Davis, Mark E. and Zones, Stacey I. (2016) Synthesis of Germanosilicate Molecular Sieves from Mono- and Di-Quaternary Ammonium OSDAs Constructed from Benzyl Imidazolium Derivatives: Stabilization of Large Micropore Volumes Including New Molecular Sieve CIT-13. Chemistry of Materials, 28 (7). pp. 2158-2164. ISSN 0897-4756. doi:10.1021/acs.chemmater.6b00031. https://resolver.caltech.edu/CaltechAUTHORS:20160328-105032968
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Abstract
A series of monoquaternary and diquarternary benzyl-imidazolium derivatives are prepared and used as organic structure direction agents (OSDAs) in germanosilicate syntheses. The goal of this work is to create new multidimensional large pore zeolites. For the OSDA made and tested, we looked for relationships based upon stereochemistry from the benzyl ring as part of each structure. Several known molecular sieves with the *BEA, BEC, IWS, or LTA topologies are obtained. Molecular modeling is carried out with the goal of understanding: (a) the product selectivity correlation with the OSDA and the zeolite obtained, and (b) why differential rates of crystallization are observed for isomers that lead to different zeolite products. Additionally, a new molecular sieve denoted CIT-13 is prepared and shown to possess intersecting 14- and 10-membered ring pores, which gives confidence to the soundness of this approach for OSDA construction to yield new multidimensional large pore zeolites. CIT-13 is the first molecular sieve to have this combination of pore sizes.
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| Additional Information: | © 2016 American Chemical Society. Received: January 4, 2016; Revised: March 3, 2016; Publication Date (Web): March 18, 2016. We thank Chevron Energy and Technology Company for support of this research. In particular, Dr. Robert Saxton (Chevron) is thanked for his support of this research collaboration. We thank Dr. Joel Schmidt for useful comments throughout the research study. The computational method described here was developed by DOE Grant No. DE-FG02-03ER15456. Author Contributions: The manuscript was written through contributions of all authors. All authors have given approval to the final manuscript. The authors declare no competing financial interest. | |||||||||
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| Issue or Number: | 7 | |||||||||
| DOI: | 10.1021/acs.chemmater.6b00031 | |||||||||
| Record Number: | CaltechAUTHORS:20160328-105032968 | |||||||||
| Persistent URL: | https://resolver.caltech.edu/CaltechAUTHORS:20160328-105032968 | |||||||||
| Official Citation: | Synthesis of Germanosilicate Molecular Sieves from Mono- and Di-Quaternary Ammonium OSDAs Constructed from Benzyl Imidazolium Derivatives: Stabilization of Large Micropore Volumes Including New Molecular Sieve CIT-13 Ben W. Boal, Michael W. Deem, Dan Xie, Jong Hun Kang, Mark E. Davis, and Stacey I. Zones Chemistry of Materials 2016 28 (7), 2158-2164 DOI: 10.1021/acs.chemmater.6b00031 | |||||||||
| Usage Policy: | No commercial reproduction, distribution, display or performance rights in this work are provided. | |||||||||
| ID Code: | 65703 | |||||||||
| Collection: | CaltechAUTHORS | |||||||||
| Deposited By: | Tony Diaz | |||||||||
| Deposited On: | 30 Mar 2016 19:44 | |||||||||
| Last Modified: | 10 Nov 2021 23:49 |
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