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Fundamental studies of gas sorption within mesopores situated amidst an inter-connected, irregular network

Rigby, Sean P. ; Chigada, Peter I. ; Perkins, Emily L. ; Watt-Smith, Matthew J. ; Lowe, John P. and Edler, Karen J. LU orcid (2008) In Adsorption 14(2-3). p.289-307
Abstract

There has been little, or no, direct testing of theories of gas sorption within particular pores situated amidst a highly inter-connected pore network. The concept of thermodynamically independent pores within networks has also been challenged. In this work, a novel integrated nitrogen sorption and mercury porosimetry technique has been used to deconvolve the condensation and evaporation processes within a specific subset of pores contained within a larger, irregular network. The sizes and geometry of these pores were obtained completely independently of gas sorption, using mercury porosimetry and NMR cryoporometry, respectively. Hence, various theories of capillary condensation, such as the Kelvin equation, the Broeckhoff-de Boer... (More)

There has been little, or no, direct testing of theories of gas sorption within particular pores situated amidst a highly inter-connected pore network. The concept of thermodynamically independent pores within networks has also been challenged. In this work, a novel integrated nitrogen sorption and mercury porosimetry technique has been used to deconvolve the condensation and evaporation processes within a specific subset of pores contained within a larger, irregular network. The sizes and geometry of these pores were obtained completely independently of gas sorption, using mercury porosimetry and NMR cryoporometry, respectively. Hence, various theories of capillary condensation, such as the Kelvin equation, the Broeckhoff-de Boer method, Saam-Cole theory, and NLDFT could be directly tested, and the potential influence of any collective network phenomena detected. It was found that, even for a shielded pore, the Cohan equation for a cylindrical meniscus gave rise to the best prediction for the relative pressure of capillary condensation, once the effects of surface chemical heterogeneity on multi-layer build-up had been taken into account. The results were also found to be incompatible with the presence of particular collective adsorption effects, such as advanced condensation.

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author
; ; ; ; and
publishing date
type
Contribution to journal
publication status
published
keywords
Capillary condensation, Independent pore, Network effects, Nitrogen adsorption, NMR cryoporometry
in
Adsorption
volume
14
issue
2-3
pages
19 pages
publisher
Springer
external identifiers
  • scopus:41149139386
ISSN
0929-5607
DOI
10.1007/s10450-007-9091-8
language
English
LU publication?
no
id
9a92d6cb-34f8-45f3-bd12-987536389f57
date added to LUP
2023-05-04 18:58:43
date last changed
2023-06-13 08:18:11
@article{9a92d6cb-34f8-45f3-bd12-987536389f57,
  abstract     = {{<p>There has been little, or no, direct testing of theories of gas sorption within particular pores situated amidst a highly inter-connected pore network. The concept of thermodynamically independent pores within networks has also been challenged. In this work, a novel integrated nitrogen sorption and mercury porosimetry technique has been used to deconvolve the condensation and evaporation processes within a specific subset of pores contained within a larger, irregular network. The sizes and geometry of these pores were obtained completely independently of gas sorption, using mercury porosimetry and NMR cryoporometry, respectively. Hence, various theories of capillary condensation, such as the Kelvin equation, the Broeckhoff-de Boer method, Saam-Cole theory, and NLDFT could be directly tested, and the potential influence of any collective network phenomena detected. It was found that, even for a shielded pore, the Cohan equation for a cylindrical meniscus gave rise to the best prediction for the relative pressure of capillary condensation, once the effects of surface chemical heterogeneity on multi-layer build-up had been taken into account. The results were also found to be incompatible with the presence of particular collective adsorption effects, such as advanced condensation.</p>}},
  author       = {{Rigby, Sean P. and Chigada, Peter I. and Perkins, Emily L. and Watt-Smith, Matthew J. and Lowe, John P. and Edler, Karen J.}},
  issn         = {{0929-5607}},
  keywords     = {{Capillary condensation; Independent pore; Network effects; Nitrogen adsorption; NMR cryoporometry}},
  language     = {{eng}},
  number       = {{2-3}},
  pages        = {{289--307}},
  publisher    = {{Springer}},
  series       = {{Adsorption}},
  title        = {{Fundamental studies of gas sorption within mesopores situated amidst an inter-connected, irregular network}},
  url          = {{http://dx.doi.org/10.1007/s10450-007-9091-8}},
  doi          = {{10.1007/s10450-007-9091-8}},
  volume       = {{14}},
  year         = {{2008}},
}