Adsorption of light hydrocarbons in the flexible MIL-53(Cr) and rigid MIL-47(V) metal-organic frameworks: a combination of molecular simulations and microcalorimetry/gravimetry measurements

被引：81

作者：

Rosenbach, N., Jr. ^{[1
]}

Ghoufi, A. ^{[2
]}

Deroche, I. ^{[1
]}

Llewellyn, P. L. ^{[3
]}

Devic, T. ^{[4
]}

Bourrelly, S. ^{[3
]}

Serre, C. ^{[4
]}

Ferey, G. ^{[4
]}

Maurin, G. ^{[1
]}

机构：

[1] CNRS, Inst Charles Gerhardt Montpellier, ENSCM, UMR 5253,UM2, F-34095 Montpellier 05, France

[2] Univ Rennes 1, CNRS, Inst Phys Rennes, UMR 6251, F-35042 Rennes, France

[3] Univ Aix Marseille I II & III, Lab Chim Prov, CNRS, Ctr St Jerome,UMR 6264, F-13397 Marseille, France

[4] Univ Versailles St Quentin Yvelines, CNRS, Inst Lavoisier, UMR 8180, F-78035 Versailles, France

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2010年 / 12卷 / 24期

关键词：

ALKANE ISOMER MIXTURES; SHORT LINEAR ALKANES; HIGH-PRESSURE; FORCE-FIELD; METHANE ADSORPTION; PORE-SIZE; SEPARATION; CH4; TRANSITION; DIFFUSION;

D O I：

10.1039/c001173h

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The adsorption of short linear alkanes has been explored in the highly flexible MIL-53(Cr) porous metal-organic framework by means of molecular simulations based on configurational bias grand canonical Monte Carlo. The unusual shape of the adsorption isotherms with the existence of steps has been successfully modelled by creating a (narrow pore, large pore) phase mixture domain, the composition of which varies with pressure. A further step consisted of combining our computational approach with several experimental tools including microcalorimetry, gravimetry and in situ X-ray diffraction, to fully characterize the adsorption behaviour of the isostructural MIL-47(V) rigid MOF, i.e. the preferential arrangement of each type of alkane inside the pores and the resulting interaction energy. Finally, relationships are established between the adsorption enthalpies and both alkyl chain length and polarisability of the alkanes that can be further utilised to predict the energetics of the adsorption process for longer alkane chains.

引用

页码：6428 / 6437

页数：10

共 57 条

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