Interaction of atmospheric gases with ETS-10: a DFT study

Renjith S Pillai; Miguel Jorge; Jose R. B. Gomes

doi:10.1016/j.micromeso.2014.01.022

Interaction of atmospheric gases with ETS-10: a DFT study

Renjith S Pillai, Miguel Jorge, Jose R. B. Gomes

Chemical And Process Engineering

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Abstract

Density functional theory (DFT) was used to optimize the geometries and calculate the enthalpies for the interactions between polar (H2O), quadrupolar (CO2 and N2), and apolar (H2 and CH4) atmospheric gases with a cluster model of the Engelhard titanosilicate ETS-10 having sodium extra framework cations (Na-ETS-10). The DFT calculations were performed with different exchange–correlation functionals and were corrected for the basis set superposition error with the counterpoise method. The calculated enthalpies for the interaction of the five gases with Na-ETS-10 decrease in the order H2O > CO2 ≫ N2 ≈ CH4 > H2 and compare well with experimental data available in the literature. The enthalpies calculated at the M06-L/6-31++G(d,p) level of theory for the two extreme cases, i.e., strongest and weakest interactions, are −60.6 kJ/mol (H2O) and −12.2 kJ/mol (H2). Additionally, the calculated vibrational frequencies are in very good agreement, within the approximations of the method, with the characteristic vibrational modes of ETS-10 and of the interactions of gases with Na+ in the 12-membered channel in ETS-10.

Original language	English
Pages (from-to)	38–45
Number of pages	9
Journal	Microporous and Mesoporous Materials
Volume	190
Early online date	29 Jan 2014
DOIs	https://doi.org/10.1016/j.micromeso.2014.01.022
Publication status	Published - 15 May 2014

Keywords

sorption
separation
atmospheric gases
DFT calculations

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10.1016/j.micromeso.2014.01.022

ETS_10_acceptedAccepted author manuscript, 2.53 MB

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title = "Interaction of atmospheric gases with ETS-10: a DFT study",

abstract = "Density functional theory (DFT) was used to optimize the geometries and calculate the enthalpies for the interactions between polar (H2O), quadrupolar (CO2 and N2), and apolar (H2 and CH4) atmospheric gases with a cluster model of the Engelhard titanosilicate ETS-10 having sodium extra framework cations (Na-ETS-10). The DFT calculations were performed with different exchange–correlation functionals and were corrected for the basis set superposition error with the counterpoise method. The calculated enthalpies for the interaction of the five gases with Na-ETS-10 decrease in the order H2O > CO2 ≫ N2 ≈ CH4 > H2 and compare well with experimental data available in the literature. The enthalpies calculated at the M06-L/6-31++G(d,p) level of theory for the two extreme cases, i.e., strongest and weakest interactions, are −60.6 kJ/mol (H2O) and −12.2 kJ/mol (H2). Additionally, the calculated vibrational frequencies are in very good agreement, within the approximations of the method, with the characteristic vibrational modes of ETS-10 and of the interactions of gases with Na+ in the 12-membered channel in ETS-10.",

keywords = "sorption, separation, atmospheric gases, DFT calculations",

author = "Pillai, {Renjith S} and Miguel Jorge and Gomes, {Jose R. B.}",

note = " NOTICE: this is the author{\textquoteright}s version of a work that was accepted for publication in Microporous and Mesoporous Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Microporous and Mesoporous Materials, [VOL190, (15/05/14)] DOI:10.1016/j.micromeso.2014.01.022",

year = "2014",

month = may,

day = "15",

doi = "10.1016/j.micromeso.2014.01.022",

language = "English",

volume = "190",

pages = "38–45",

journal = "Microporous and Mesoporous Materials",

issn = "1387-1811",

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TY - JOUR

T1 - Interaction of atmospheric gases with ETS-10

T2 - a DFT study

AU - Pillai, Renjith S

AU - Jorge, Miguel

AU - Gomes, Jose R. B.

N1 - NOTICE: this is the author’s version of a work that was accepted for publication in Microporous and Mesoporous Materials. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Microporous and Mesoporous Materials, [VOL190, (15/05/14)] DOI:10.1016/j.micromeso.2014.01.022

PY - 2014/5/15

Y1 - 2014/5/15

N2 - Density functional theory (DFT) was used to optimize the geometries and calculate the enthalpies for the interactions between polar (H2O), quadrupolar (CO2 and N2), and apolar (H2 and CH4) atmospheric gases with a cluster model of the Engelhard titanosilicate ETS-10 having sodium extra framework cations (Na-ETS-10). The DFT calculations were performed with different exchange–correlation functionals and were corrected for the basis set superposition error with the counterpoise method. The calculated enthalpies for the interaction of the five gases with Na-ETS-10 decrease in the order H2O > CO2 ≫ N2 ≈ CH4 > H2 and compare well with experimental data available in the literature. The enthalpies calculated at the M06-L/6-31++G(d,p) level of theory for the two extreme cases, i.e., strongest and weakest interactions, are −60.6 kJ/mol (H2O) and −12.2 kJ/mol (H2). Additionally, the calculated vibrational frequencies are in very good agreement, within the approximations of the method, with the characteristic vibrational modes of ETS-10 and of the interactions of gases with Na+ in the 12-membered channel in ETS-10.

AB - Density functional theory (DFT) was used to optimize the geometries and calculate the enthalpies for the interactions between polar (H2O), quadrupolar (CO2 and N2), and apolar (H2 and CH4) atmospheric gases with a cluster model of the Engelhard titanosilicate ETS-10 having sodium extra framework cations (Na-ETS-10). The DFT calculations were performed with different exchange–correlation functionals and were corrected for the basis set superposition error with the counterpoise method. The calculated enthalpies for the interaction of the five gases with Na-ETS-10 decrease in the order H2O > CO2 ≫ N2 ≈ CH4 > H2 and compare well with experimental data available in the literature. The enthalpies calculated at the M06-L/6-31++G(d,p) level of theory for the two extreme cases, i.e., strongest and weakest interactions, are −60.6 kJ/mol (H2O) and −12.2 kJ/mol (H2). Additionally, the calculated vibrational frequencies are in very good agreement, within the approximations of the method, with the characteristic vibrational modes of ETS-10 and of the interactions of gases with Na+ in the 12-membered channel in ETS-10.

KW - sorption

KW - separation

KW - atmospheric gases

KW - DFT calculations

U2 - 10.1016/j.micromeso.2014.01.022

DO - 10.1016/j.micromeso.2014.01.022

M3 - Article

SN - 1387-1811

VL - 190

SP - 38

EP - 45

JO - Microporous and Mesoporous Materials

JF - Microporous and Mesoporous Materials

ER -

Interaction of atmospheric gases with ETS-10: a DFT study

Abstract

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