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Host-guest and guest-guest interactions between xylene isomers confined in the MIL-47(V) pore system

An Ghysels UGent, Matthias Vandichel UGent, Toon Verstraelen UGent, Monique A van der Veen, Dirk E De Vos, Michel Waroquier UGent and Veronique Van Speybroeck UGent (2012) THEORETICAL CHEMISTRY ACCOUNTS. 131(7).
abstract
The porous MIL-47 material shows a selective adsorption behavior for para-, ortho-, and meta-isomers of xylenes, making the material a serious candidate for separation applications. The origin of the selectivity lies in the differences in interactions (energetic) and confining (entropic). This paper investigates the xylene-framework interactions and the xylene-xylene interactions with quantum mechanical calculations, using a dispersion-corrected density functional and periodic boundary conditions to describe the crystal. First, the strength and geometrical characteristics of the optimal xylene-xylene interactions are quantified by studying the pure and mixed pairs in gas phase. An extended set of initial structures is created and optimized to sample as many relative orientations and distances as possible. Next, the pairs are brought in the pores of MIL-47. The interaction with the terephthalic linkers and other xylenes increases the stacking energy in gas phase (-31.7 kJ/mol per pair) by roughly a factor four in the fully loaded state (-58.3 kJ/mol per xylene). Our decomposition of the adsorption energy shows various trends in the contributing xylene-xylene interactions. The absence of a significant difference in energetics between the isomers indicates that entropic effects must be mainly responsible for the separation behavior.
Please use this url to cite or link to this publication:
author
organization
year
type
journalArticle (original)
publication status
published
subject
keyword
Separation, METAL-ORGANIC FRAMEWORKS, DENSITY-FUNCTIONAL THEORY, Xylenes, MIL-47, DFT-D, Adsorption, PI-STACKING INTERACTIONS, NONCOVALENT INTERACTIONS, BENZENE DIMER, SELECTIVE ADSORPTION, MOLECULAR-DYNAMICS, SEPARATION, SANDWICH
journal title
THEORETICAL CHEMISTRY ACCOUNTS
Theor. Chem. Acc.
volume
131
issue
7
article_number
1234
pages
13 pages
Web of Science type
Article
Web of Science id
000307274300002
JCR category
CHEMISTRY, PHYSICAL
JCR impact factor
2.233 (2012)
JCR rank
62/133 (2012)
JCR quartile
2 (2012)
ISSN
1432-881X
DOI
10.1007/s00214-012-1234-7
language
English
UGent publication?
yes
classification
A1
additional info
The original publication is available at www.springerlink.com
copyright statement
I have transferred the copyright for this publication to the publisher
id
2979575
handle
http://hdl.handle.net/1854/LU-2979575
date created
2012-09-06 09:06:40
date last changed
2012-09-07 12:15:13
@article{2979575,
  abstract     = {The porous MIL-47 material shows a selective adsorption behavior for para-, ortho-, and meta-isomers of xylenes, making the material a serious candidate for separation applications. The origin of the selectivity lies in the differences in interactions (energetic) and confining (entropic). This paper investigates the xylene-framework interactions and the xylene-xylene interactions with quantum mechanical calculations, using a dispersion-corrected density functional and periodic boundary conditions to describe the crystal. First, the strength and geometrical characteristics of the optimal xylene-xylene interactions are quantified by studying the pure and mixed pairs in gas phase. An extended set of initial structures is created and optimized to sample as many relative orientations and distances as possible. Next, the pairs are brought in the pores of MIL-47. The interaction with the terephthalic linkers and other xylenes increases the stacking energy in gas phase (-31.7 kJ/mol per pair) by roughly a factor four in the fully loaded state (-58.3 kJ/mol per xylene). Our decomposition of the adsorption energy shows various trends in the contributing xylene-xylene interactions. The absence of a significant difference in energetics between the isomers indicates that entropic effects must be mainly responsible for the separation behavior.},
  articleno    = {1234},
  author       = {Ghysels, An and Vandichel, Matthias and Verstraelen, Toon and van der Veen, Monique A and De Vos, Dirk E and Waroquier, Michel and Van Speybroeck, Veronique},
  issn         = {1432-881X},
  journal      = {THEORETICAL CHEMISTRY ACCOUNTS},
  keyword      = {Separation,METAL-ORGANIC FRAMEWORKS,DENSITY-FUNCTIONAL THEORY,Xylenes,MIL-47,DFT-D,Adsorption,PI-STACKING INTERACTIONS,NONCOVALENT INTERACTIONS,BENZENE DIMER,SELECTIVE ADSORPTION,MOLECULAR-DYNAMICS,SEPARATION,SANDWICH},
  language     = {eng},
  number       = {7},
  pages        = {13},
  title        = {Host-guest and guest-guest interactions between xylene isomers confined in the MIL-47(V) pore system},
  url          = {http://dx.doi.org/10.1007/s00214-012-1234-7},
  volume       = {131},
  year         = {2012},
}

Chicago
Ghysels, An, Matthias Vandichel, Toon Verstraelen, Monique A van der Veen, Dirk E De Vos, Michel Waroquier, and Veronique Van Speybroeck. 2012. “Host-guest and Guest-guest Interactions Between Xylene Isomers Confined in the MIL-47(V) Pore System.” Theoretical Chemistry Accounts 131 (7).
APA
Ghysels, A., Vandichel, M., Verstraelen, T., van der Veen, M. A., De Vos, D. E., Waroquier, M., & Van Speybroeck, V. (2012). Host-guest and guest-guest interactions between xylene isomers confined in the MIL-47(V) pore system. THEORETICAL CHEMISTRY ACCOUNTS, 131(7).
Vancouver
1.
Ghysels A, Vandichel M, Verstraelen T, van der Veen MA, De Vos DE, Waroquier M, et al. Host-guest and guest-guest interactions between xylene isomers confined in the MIL-47(V) pore system. THEORETICAL CHEMISTRY ACCOUNTS. 2012;131(7).
MLA
Ghysels, An, Matthias Vandichel, Toon Verstraelen, et al. “Host-guest and Guest-guest Interactions Between Xylene Isomers Confined in the MIL-47(V) Pore System.” THEORETICAL CHEMISTRY ACCOUNTS 131.7 (2012): n. pag. Print.