Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites
We use a combination of experiments and molecular simulations to address the discrepancies of the force fields available in the literature to accurately reproduce CO2 adsorption in zeolites with high density of aluminum atoms and extra framework cations. We attribute these discrepancies to the fact that previous force fields are not parametrized to take into account the formation of carbonate-like complexes in these zeolites during CO2 adsorption. Our data show that the formation of carbonate-like complexes has a marked effect on the accessible porous structure of the zeolite, and the strength is controlled by the density and nature of extra framework cations. Strong carbonate-like complexes are formed in zeolite topologies containing high density of sodium, whereas bivalent cations give rise to more labile complexes. We provide a new set of parameters capable to reproduce the experimental adsorption in these systems. Our approach consists of the modification of the partial charges of the atoms of the zeolite that are directly involved in the formation of the surface complexes (oxygen atoms and cations). The new set of charges combined with our previous transferable force field reproduces the experimental adsorption in structures containing carbon dioxide–cation complexes.
Main Authors: | , , , |
---|---|
Other Authors: | |
Format: | artículo biblioteca |
Language: | English |
Published: |
American Chemical Society
2014-10-15
|
Subjects: | Adsorption, Carbon dioxide, Carbonates, LTA, Zeolites, |
Online Access: | http://hdl.handle.net/10261/128482 http://dx.doi.org/10.13039/501100003176 http://dx.doi.org/10.13039/501100000781 |
Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
id |
dig-incar-es-10261-128482 |
---|---|
record_format |
koha |
spelling |
dig-incar-es-10261-1284822018-11-15T12:58:09Z Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites Martín Calvo, Ana Parra Soto, José Bernardo Ovín Ania, María Concepción Calero, S. Ministerio de Educación, Cultura y Deporte (España) European Research Council Adsorption Carbon dioxide Carbonates LTA Zeolites We use a combination of experiments and molecular simulations to address the discrepancies of the force fields available in the literature to accurately reproduce CO2 adsorption in zeolites with high density of aluminum atoms and extra framework cations. We attribute these discrepancies to the fact that previous force fields are not parametrized to take into account the formation of carbonate-like complexes in these zeolites during CO2 adsorption. Our data show that the formation of carbonate-like complexes has a marked effect on the accessible porous structure of the zeolite, and the strength is controlled by the density and nature of extra framework cations. Strong carbonate-like complexes are formed in zeolite topologies containing high density of sodium, whereas bivalent cations give rise to more labile complexes. We provide a new set of parameters capable to reproduce the experimental adsorption in these systems. Our approach consists of the modification of the partial charges of the atoms of the zeolite that are directly involved in the formation of the surface complexes (oxygen atoms and cations). The new set of charges combined with our previous transferable force field reproduces the experimental adsorption in structures containing carbon dioxide–cation complexes. This work was supported by the Spanish “Ministerio de Educacion, Cultura y Deporte” (CTQ2010-16077/BQU), and the European Research Council through an ERC Staring Grant (ERC-StG-279520-RASPA). A. Martín-Calvo thanks the Spanish “Ministerio de Educación” for her predoctoral fellowship. Peer reviewed 2016-02-02T08:14:01Z 2016-02-02T08:14:01Z 2014-10-15 artículo http://purl.org/coar/resource_type/c_6501 Journal of Physical Chemistry C 118(44): 25460-25467 (2014) 1932-7447 http://hdl.handle.net/10261/128482 10.1021/jp507431c http://dx.doi.org/10.13039/501100003176 http://dx.doi.org/10.13039/501100000781 en Postprint http://dx.doi.org/10.1021/jp507431c Sí open American Chemical Society |
institution |
INCAR ES |
collection |
DSpace |
country |
España |
countrycode |
ES |
component |
Bibliográfico |
access |
En linea |
databasecode |
dig-incar-es |
tag |
biblioteca |
region |
Europa del Sur |
libraryname |
Biblioteca del INCAR España |
language |
English |
topic |
Adsorption Carbon dioxide Carbonates LTA Zeolites Adsorption Carbon dioxide Carbonates LTA Zeolites |
spellingShingle |
Adsorption Carbon dioxide Carbonates LTA Zeolites Adsorption Carbon dioxide Carbonates LTA Zeolites Martín Calvo, Ana Parra Soto, José Bernardo Ovín Ania, María Concepción Calero, S. Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
description |
We use a combination of experiments and molecular simulations to address the discrepancies of the force fields available in the literature to accurately reproduce CO2 adsorption in zeolites with high density of aluminum atoms and extra framework cations. We attribute these discrepancies to the fact that previous force fields are not parametrized to take into account the formation of carbonate-like complexes in these zeolites during CO2 adsorption. Our data show that the formation of carbonate-like complexes has a marked effect on the accessible porous structure of the zeolite, and the strength is controlled by the density and nature of extra framework cations. Strong carbonate-like complexes are formed in zeolite topologies containing high density of sodium, whereas bivalent cations give rise to more labile complexes. We provide a new set of parameters capable to reproduce the experimental adsorption in these systems. Our approach consists of the modification of the partial charges of the atoms of the zeolite that are directly involved in the formation of the surface complexes (oxygen atoms and cations). The new set of charges combined with our previous transferable force field reproduces the experimental adsorption in structures containing carbon dioxide–cation complexes. |
author2 |
Ministerio de Educación, Cultura y Deporte (España) |
author_facet |
Ministerio de Educación, Cultura y Deporte (España) Martín Calvo, Ana Parra Soto, José Bernardo Ovín Ania, María Concepción Calero, S. |
format |
artículo |
topic_facet |
Adsorption Carbon dioxide Carbonates LTA Zeolites |
author |
Martín Calvo, Ana Parra Soto, José Bernardo Ovín Ania, María Concepción Calero, S. |
author_sort |
Martín Calvo, Ana |
title |
Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
title_short |
Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
title_full |
Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
title_fullStr |
Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
title_full_unstemmed |
Insights on the Anomalous Adsorption of Carbon Dioxide in LTA Zeolites |
title_sort |
insights on the anomalous adsorption of carbon dioxide in lta zeolites |
publisher |
American Chemical Society |
publishDate |
2014-10-15 |
url |
http://hdl.handle.net/10261/128482 http://dx.doi.org/10.13039/501100003176 http://dx.doi.org/10.13039/501100000781 |
work_keys_str_mv |
AT martincalvoana insightsontheanomalousadsorptionofcarbondioxideinltazeolites AT parrasotojosebernardo insightsontheanomalousadsorptionofcarbondioxideinltazeolites AT ovinaniamariaconcepcion insightsontheanomalousadsorptionofcarbondioxideinltazeolites AT caleros insightsontheanomalousadsorptionofcarbondioxideinltazeolites |
_version_ |
1777668970558521344 |