Diffusion of Xylene Isomers in the MIL-47(V) MOF Material: A Synergic Combination of Computational and Experimental Tools | Sciact - CRIS-system of Boreskov Institute of Catalysis

Diffusion of Xylene Isomers in the MIL-47(V) MOF Material: A Synergic Combination of Computational and Experimental Tools Full article

Journal

The Journal of Physical Chemistry C
ISSN: 1932-7447 , E-ISSN: 1932-7455

Output data

Year: 2013, Volume: 117, Number: 12, Pages: 6293-6302 Pages count : 10 DOI: 10.1021/jp400507w

Tags

Activation energy; Crystalline materials; Diffusion; Isomers; Molecular dynamics; Molecules; Nuclear magnetic resonance spectroscopy

Authors

Rives S. ^1,2 , Jobic H. ² , Kolokolov D.I. ³ , Gabrienko A.A. ³ , Stepanov A.G. ³ , Ke Y. ¹ , Frick B. ⁴ , Devic T. ⁵ , Férey G. ⁵ , Maurin G. ¹

Affiliations

1	Institut Charles Gerhardt Montpellier, UMR 5253 CNRS, UM2, UM1, ENSCM, Université Montpellier 2, Pl. E. Bataillon, 34095 Montpellier Cedex 05, France
2	Institut de Recherches sur la Catalyse et l’Environnement de Lyon, Université de Lyon 1, CNRS, 2. Av. A. Einstein, 69626 Villeurbanne, France
3	Boreskov Institute of Catalysis, Siberian Branch of Russian Academy of Sciences, Prospekt Akademika Lavrentieva 5, Novosibirsk 630090, Russia
4	Institut Laue Langevin, BP 156, 38042 Grenoble, France
5	Institut Lavoisier, UMR CNRS 8180, Université de Versailles Saint-Quentin-en-Yvelines, 45 avenue des Etats-Unis, 78035 Versailles cedex, France

Funding (3)

1	Russian Foundation for Basic Research	13-03-00327
2	European Commission	228862 FP7-NMP-2008-LARGE-2 MACADEMIA
3	The Ministry of Education and Science of the Russian Federation

The dynamics of xylene isomers in the metal-organic framework MIL-47(V) has been investigated by combining molecular dynamics (MD) simulations and experimental tools including quasi-elastic neutron scattering (QENS) and deuterium nuclear magnetic resonance (H-2 NMR). The experimental and simulated self-diffusion coefficients (D-s) values for each single component isomer are in reasonable agreement in the whole range of temperatures. More interestingly, the simulations predict a nonmonotonous evolution of D-s with the temperature for all xylenes. Such an unusual trend is experimentally confirmed for p-xylene. Two distinct diffusion regimes are elucidated at the microscopic level: a low-temperature regime where the xylene molecules are close to the MIL-47(V) pore wall with a high activation energy barrier for the diffusion and a high-temperature regime where the xylene molecules are mainly located in the center of the channel associated with a lower activation energy for the diffusion. This dynamic behavior remains also true whatever the degree of pore filling. It has been further shown that the diffusivity is only slightly affected when one compares the case of xylenes in single component and in mixture. H-2 NMR experiments enlighten that packing effects and guest-guest interactions are crucial when considering the dynamics of confined xylenes in MIL-47(V).

Rives S. , Jobic H. , Kolokolov D.I. , Gabrienko A.A. , Stepanov A.G. , Ke Y. , Frick B. , Devic T. , Férey G. , Maurin G.
Diffusion of Xylene Isomers in the MIL-47(V) MOF Material: A Synergic Combination of Computational and Experimental Tools
The Journal of Physical Chemistry C. 2013. V.117. N12. P.6293-6302. DOI: 10.1021/jp400507w WOS Scopus РИНЦ ANCAN OpenAlex

Submitted:	Jan 16, 2013
Accepted:	Mar 4, 2013
Published online:	Mar 18, 2013
Published print:	Mar 28, 2013

Web of science:	WOS:000317032100034
Scopus:	2-s2.0-84875751856
Elibrary:	20430368
Chemical Abstracts:	2013:368327
Chemical Abstracts (print):	158:458110
OpenAlex:	W2099489034

DB	Citing
Web of science	45
Scopus	45
Elibrary	44
OpenAlex	44