Hydrocarbon Adsorption in the Flexible Metal Organic Frameworks MIL-53(Al, Cr)

被引:230
作者
Trung, Thuy Khuong [1 ]
Trens, Philippe [1 ]
Tanchoux, Nathalie [1 ]
Bourrelly, Sandrine [2 ]
Llewellyn, Philip L. [2 ]
Loera-Serna, Sandra [2 ]
Serre, Christian [3 ]
Loiseau, Thierry [3 ]
Fajula, Francois [1 ]
Ferey, Gerard [3 ]
机构
[1] CNRS ENSCM UM2 UM1, MACS, Inst Charles Gerhardt, F-34296 Montpellier 5, France
[2] Univ Aix Marseille 1, CNRS, Lab Chim Provence, UMR 6264,Ctr St Jerome, F-13397 Marseille 20, France
[3] Univ Versailles St Quentin, Inst Lavoisier, CNRS, UMR 8180, F-78035 Versailles, France
关键词
D O I
10.1021/ja8039579
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
A general study of the adsorption of n-alkanes in the flexible metal organic framework (MOF) MIL-53 is presented. The roles of the length of the alkyl chain (n = 1-9), the nature of the metal (Al, Cr), and temperature were investigated. The shape of the adsorption curves is driven by the alkyl chain length of the n-alkanes. While traditional typed isotherms are observed for short alkanes (n = 1, 2), adsorbates with longer chains induce clear substeps in the isotherm curves whose positions depend on the chain length. Such substeps are due to a breathing phenomenon, as proven by ex situ X-ray diffraction analysis. They strongly depend on the amount of adsorbate in the pores and on the nature of the metal (Al, Cr), which, for a given alkane, leads to a strong change in the substep positions despite the similar characteristics of the two metals. The adsorption kinetics are highly sensitive to small variations in temperature. Their detailed analysis in different regions of the isotherms shows in some cases the existence of distinct diffusion regimes and/or conformations within the flexible phases.
引用
收藏
页码:16926 / 16932
页数:7
相关论文
共 41 条
[1]   Selective adsorption and separation of xylene isomers and ethylbenzene with the microporous vanadium(IV) terephthalate MIL-47 [J].
Alaerts, Luc ;
Kirschhock, Christine E. A. ;
Maes, Michael ;
van der Veen, Monique A. ;
Finsy, Vincent ;
Depla, Anouschka ;
Martens, Johan A. ;
Baron, Gino V. ;
Jacobs, Pierre A. ;
Denayer, Joeri E. M. ;
De Vos, Dirk E. .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2007, 46 (23) :4293-4297
[2]   INDEXING OF POWDER DIFFRACTION PATTERNS FOR LOW-SYMMETRY LATTICES BY THE SUCCESSIVE DICHOTOMY METHOD [J].
BOULTIF, A ;
LOUER, D .
JOURNAL OF APPLIED CRYSTALLOGRAPHY, 1991, 24 (pt 6) :987-993
[3]   Different adsorption behaviors of methane and carbon dioxide in the isotypic nanoporous metal terephthalates MIL-53 and MIL-47 [J].
Bourrelly, S ;
Llewellyn, PL ;
Serre, C ;
Millange, F ;
Loiseau, T ;
Férey, G .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (39) :13519-13521
[4]   A microporous metal-organic framework for gas-chromatographic separation of alkanes [J].
Chen, BL ;
Liang, CD ;
Yang, J ;
Contreras, DS ;
Clancy, YL ;
Lobkovsky, EB ;
Yaghi, OM ;
Dai, S .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2006, 45 (09) :1390-1393
[5]  
Chen C. Y., 2001, STUD SURF SCI CATAL, V135, P222
[6]   Molecular competition effects in liquid-phase adsorption of long-chain n-alkane mixtures in ZSM-5 zeolite pores [J].
Denayer, JFM ;
De Meyer, K ;
Martens, JA ;
Baron, GV .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2003, 42 (24) :2774-2777
[7]   SURFACE CURVATURE EFFECTS IN PHYSISORPTION AND CATALYSIS BY MICROPOROUS SOLIDS AND MOLECULAR-SIEVES [J].
DEROUANE, EG ;
ANDRE, JM ;
LUCAS, AA .
JOURNAL OF CATALYSIS, 1988, 110 (01) :58-73
[8]   Hydrogen adsorption in the nanoporous metal-benzenedicarboxylate M(OH)(O2C-C6H4-CO2) (M = Al3+, Cr3+), MIL-53 [J].
Férey, G ;
Latroche, M ;
Serre, C ;
Millange, F ;
Loiseau, T ;
Percheron-Guégan, A .
CHEMICAL COMMUNICATIONS, 2003, (24) :2976-2977
[9]   Crystallized frameworks with giant pores:: Are there limits to the possible? [J].
Férey, G ;
Mellot-Draznieks, C ;
Serre, C ;
Millange, F .
ACCOUNTS OF CHEMICAL RESEARCH, 2005, 38 (04) :217-225
[10]   Hybrid porous solids:: past, present, future [J].
Ferey, Gerard .
CHEMICAL SOCIETY REVIEWS, 2008, 37 (01) :191-214