First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers
Abstract
Metal dopants in Lewis acid zeolites can be applied to manipulate the interaction between the active sites and molecular reactants. However, only a few elements can be introduced into the zeolite framework to generate strong Lewis acid sites. In this study, we propose an alternative approach to tune the interaction between zeolite and molecules by introducing energized charge carriers that are photoexcited in a complex of plasmonic metal and zeolites. Here, through density functional theory (DFT) calculations, we show that although the energized electrons do not impact the adsorption of ammonia, which is used as a probe molecule, on Zr- and Si-BEA, ammonia’s heat of adsorption can be reduced up to 60% on Sn-BEA and 20% on Ti-BEA, respectively, because of the localized population of the electrons at the Sn and Ti center. This most pronounced effect in Sn-BEA is attributed to the Sn-induced midgap states and the strong electronegativity of Sn atoms. In contrast, the energized holes can strengthen the interaction between zeolites and ammonia by at least 10%. Particularly, if an energized hole is present in the system, the heat of adsorption of ammonia within Si-BEA can increase 3-fold, shifting from weak to moderate interaction. We find that,more »
- Publication Date:
- Research Org.:
- Univ. of Oklahoma, Norman, OK (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1839385
- Grant/Contract Number:
- SC0020300
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Industrial and Engineering Chemistry Research
- Additional Journal Information:
- Journal Volume: 60; Journal Issue: 39; Journal ID: ISSN 0888-5885
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Lewis acids; Metals; Adsorption; Zeolites; Molecules
Citation Formats
Le, Tien, and Wang, Bin. First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers. United States: N. p., 2021.
Web. doi:10.1021/acs.iecr.1c02808.
Le, Tien, & Wang, Bin. First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers. United States. https://doi.org/10.1021/acs.iecr.1c02808
Le, Tien, and Wang, Bin. Wed .
"First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers". United States. https://doi.org/10.1021/acs.iecr.1c02808. https://www.osti.gov/servlets/purl/1839385.
@article{osti_1839385,
title = {First-Principles Study of Interaction between Molecules and Lewis Acid Zeolites Manipulated by Injection of Energized Charge Carriers},
author = {Le, Tien and Wang, Bin},
abstractNote = {Metal dopants in Lewis acid zeolites can be applied to manipulate the interaction between the active sites and molecular reactants. However, only a few elements can be introduced into the zeolite framework to generate strong Lewis acid sites. In this study, we propose an alternative approach to tune the interaction between zeolite and molecules by introducing energized charge carriers that are photoexcited in a complex of plasmonic metal and zeolites. Here, through density functional theory (DFT) calculations, we show that although the energized electrons do not impact the adsorption of ammonia, which is used as a probe molecule, on Zr- and Si-BEA, ammonia’s heat of adsorption can be reduced up to 60% on Sn-BEA and 20% on Ti-BEA, respectively, because of the localized population of the electrons at the Sn and Ti center. This most pronounced effect in Sn-BEA is attributed to the Sn-induced midgap states and the strong electronegativity of Sn atoms. In contrast, the energized holes can strengthen the interaction between zeolites and ammonia by at least 10%. Particularly, if an energized hole is present in the system, the heat of adsorption of ammonia within Si-BEA can increase 3-fold, shifting from weak to moderate interaction. We find that, similar to closed sites, the effect of energized charge carriers can also be extended to open sites of Lewis acid zeolites. Our study provides fundamental insights for unlocking the potentials of integrating plasmonic metals with zeolites and brings an additional degree of control to tune the interfacial interaction.},
doi = {10.1021/acs.iecr.1c02808},
journal = {Industrial and Engineering Chemistry Research},
number = 39,
volume = 60,
place = {United States},
year = {Wed Sep 22 00:00:00 EDT 2021},
month = {Wed Sep 22 00:00:00 EDT 2021}
}
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