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Beyond shape selective catalysis with zeolites: Hydrophobic void spaces in zeolites enable catalysis in liquid water

Gounder, Rajamani and Davis, Mark E. (2013) Beyond shape selective catalysis with zeolites: Hydrophobic void spaces in zeolites enable catalysis in liquid water. AIChE Journal, 59 (9). pp. 3349-3358. ISSN 0001-1541. doi:10.1002/aic.14016. https://resolver.caltech.edu/CaltechAUTHORS:20130913-103602906

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Abstract

Zeolites confine active sites within void spaces of molecular dimension. The size and shape of these voids can be tuned by changing framework topology, which can influence catalytic reactivity and selectivity via coupled reaction-transport phenomena that exploit differences in transport properties among reactants and/or products that differ in size and shape. The polarity and solvating properties of intrazeolite void environments can be tuned by changing chemical composition and structure, ranging from hydrophobic defect-free pure-silica surfaces to silica surfaces containing hydrophilic defect sites and/or heteroatoms. Here, we discuss how the polarity of zeolite voids influences catalytic reactivity and selectivity via the partitioning of reactant, product, and solvent molecules between intrazeolitic locations and external fluid phases. These findings provide a conceptual basis for developing selective catalytic processes in aqueous media using hydrophobic zeolites that are able to adsorb organic reactants while excluding liquid water from internal void spaces.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1002/aic.14016 DOIArticle
http://onlinelibrary.wiley.com/doi/10.1002/aic.14016/abstractPublisherArticle
ORCID:
AuthorORCID
Gounder, Rajamani0000-0003-1347-534X
Davis, Mark E.0000-0001-8294-1477
Additional Information:© 2013 American Institute of Chemical Engineers. Manuscript received Oct. 30, 2012, and revision received Dec. 10, 2012. Article first published online: 24 Jan. 2013. This work was financially supported as part of the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001004. We thank Dr. Son-Jong Hwang for the ^(13)C and ^1H NMR spectra, Yashodhan Bhawe for helpful technical discussion, and Ricardo Bermejo-Deval and Carly Bond for experimental assistance.
Funders:
Funding AgencyGrant Number
Catalysis Center for Energy InnovationUNSPECIFIED
Department of Energy (DOE) Office of Science, Office of Basic Energy SciencesDE-SC0001004
Subject Keywords:hydrophobic; Lewis acid; tin-Beta; water-tolerant; zeolites
Issue or Number:9
DOI:10.1002/aic.14016
Record Number:CaltechAUTHORS:20130913-103602906
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20130913-103602906
Official Citation:Gounder, R. and Davis, M. E. (2013), Beyond shape selective catalysis with zeolites: Hydrophobic void spaces in zeolites enable catalysis in liquid water. AIChE J., 59: 3349–3358. doi: 10.1002/aic.14016
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:41317
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:16 Sep 2013 21:14
Last Modified:10 Nov 2021 04:28

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