Gas adsorption in active carbons and the slit-pore model 2: mixture adsorption prediction with DFT and IAST

M.B. Sweatman, N. Quirke

Research output: Contribution to journalArticle

19 Citations (Scopus)

Abstract

We use a fast density functional theory (a 'slab-DFT') and the polydisperse independent ideal slit-pore model to predict gas mixture adsorption in active carbons. The DFT is parametrized by fitting to pure gas isotherms generated by Monte Carlo simulation of adsorption in model graphitic slit-pores. Accurate gas molecular models are used in our Monte Carlo simulations with gas-surface interactions calibrated to a high surface area carbon, rather than a low surface area carbon as in all previous work of this type, as described in part 1 of this work (Sweatman, M. B.; Quirke, N. J. Phys. Chem. B 2005, 109, 10381). We predict the adsorption of binary mixtures of carbon dioxide, methane, and nitrogen on two active carbons up to about 30 bar at near-ambient temperatures. We compare two sets of results; one set obtained using only the pure carbon dioxide adsorption isotherm as input to our pore characterization process, and the other obtained using both pure gas isotherms as input. We also compare these results with ideal adsorbed solution theory (IAST). We find that our methods are at least as accurate as IAST for these relatively simple gas mixtures and have the advantage of much greater versatility. We expect similar results for other active carbons and further performance gains for less ideal mixtures.
LanguageEnglish
Pages10389-10394
Number of pages5
JournalJournal of Physical Chemistry B
Volume109
Issue number20
DOIs
Publication statusPublished - 30 Apr 2005

Fingerprint

Gas adsorption
Discrete Fourier transforms
slits
Carbon
porosity
Adsorption
Gases
adsorption
carbon
predictions
gases
isotherms
Carbon Dioxide
Gas mixtures
gas mixtures
Isotherms
carbon dioxide
Carbon dioxide
Methane
versatility

Keywords

  • gas adsorption
  • carbon
  • mixture adsorption
  • DFT
  • IAST

Cite this

@article{c57ff51fcbdd42a19d8240fb11a46c9d,
title = "Gas adsorption in active carbons and the slit-pore model 2: mixture adsorption prediction with DFT and IAST",
abstract = "We use a fast density functional theory (a 'slab-DFT') and the polydisperse independent ideal slit-pore model to predict gas mixture adsorption in active carbons. The DFT is parametrized by fitting to pure gas isotherms generated by Monte Carlo simulation of adsorption in model graphitic slit-pores. Accurate gas molecular models are used in our Monte Carlo simulations with gas-surface interactions calibrated to a high surface area carbon, rather than a low surface area carbon as in all previous work of this type, as described in part 1 of this work (Sweatman, M. B.; Quirke, N. J. Phys. Chem. B 2005, 109, 10381). We predict the adsorption of binary mixtures of carbon dioxide, methane, and nitrogen on two active carbons up to about 30 bar at near-ambient temperatures. We compare two sets of results; one set obtained using only the pure carbon dioxide adsorption isotherm as input to our pore characterization process, and the other obtained using both pure gas isotherms as input. We also compare these results with ideal adsorbed solution theory (IAST). We find that our methods are at least as accurate as IAST for these relatively simple gas mixtures and have the advantage of much greater versatility. We expect similar results for other active carbons and further performance gains for less ideal mixtures.",
keywords = "gas adsorption, carbon, mixture adsorption, DFT, IAST",
author = "M.B. Sweatman and N. Quirke",
year = "2005",
month = "4",
day = "30",
doi = "10.1021/jp045272t",
language = "English",
volume = "109",
pages = "10389--10394",
journal = "Journal of Physical Chemistry B",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "20",

}

Gas adsorption in active carbons and the slit-pore model 2 : mixture adsorption prediction with DFT and IAST. / Sweatman, M.B.; Quirke, N.

In: Journal of Physical Chemistry B, Vol. 109, No. 20, 30.04.2005, p. 10389-10394.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Gas adsorption in active carbons and the slit-pore model 2

T2 - Journal of Physical Chemistry B

AU - Sweatman, M.B.

AU - Quirke, N.

PY - 2005/4/30

Y1 - 2005/4/30

N2 - We use a fast density functional theory (a 'slab-DFT') and the polydisperse independent ideal slit-pore model to predict gas mixture adsorption in active carbons. The DFT is parametrized by fitting to pure gas isotherms generated by Monte Carlo simulation of adsorption in model graphitic slit-pores. Accurate gas molecular models are used in our Monte Carlo simulations with gas-surface interactions calibrated to a high surface area carbon, rather than a low surface area carbon as in all previous work of this type, as described in part 1 of this work (Sweatman, M. B.; Quirke, N. J. Phys. Chem. B 2005, 109, 10381). We predict the adsorption of binary mixtures of carbon dioxide, methane, and nitrogen on two active carbons up to about 30 bar at near-ambient temperatures. We compare two sets of results; one set obtained using only the pure carbon dioxide adsorption isotherm as input to our pore characterization process, and the other obtained using both pure gas isotherms as input. We also compare these results with ideal adsorbed solution theory (IAST). We find that our methods are at least as accurate as IAST for these relatively simple gas mixtures and have the advantage of much greater versatility. We expect similar results for other active carbons and further performance gains for less ideal mixtures.

AB - We use a fast density functional theory (a 'slab-DFT') and the polydisperse independent ideal slit-pore model to predict gas mixture adsorption in active carbons. The DFT is parametrized by fitting to pure gas isotherms generated by Monte Carlo simulation of adsorption in model graphitic slit-pores. Accurate gas molecular models are used in our Monte Carlo simulations with gas-surface interactions calibrated to a high surface area carbon, rather than a low surface area carbon as in all previous work of this type, as described in part 1 of this work (Sweatman, M. B.; Quirke, N. J. Phys. Chem. B 2005, 109, 10381). We predict the adsorption of binary mixtures of carbon dioxide, methane, and nitrogen on two active carbons up to about 30 bar at near-ambient temperatures. We compare two sets of results; one set obtained using only the pure carbon dioxide adsorption isotherm as input to our pore characterization process, and the other obtained using both pure gas isotherms as input. We also compare these results with ideal adsorbed solution theory (IAST). We find that our methods are at least as accurate as IAST for these relatively simple gas mixtures and have the advantage of much greater versatility. We expect similar results for other active carbons and further performance gains for less ideal mixtures.

KW - gas adsorption

KW - carbon

KW - mixture adsorption

KW - DFT

KW - IAST

U2 - 10.1021/jp045272t

DO - 10.1021/jp045272t

M3 - Article

VL - 109

SP - 10389

EP - 10394

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

SN - 1520-6106

IS - 20

ER -