Intracrystalline diffusivities and surface permeabilities deduced from transient concentration profiles:: Methanol in MOF manganese formate

被引:64
作者
Kortunov, Pavel V.
Heinke, Lars
Arnold, Mirko
Nedellec, Yannic
Jones, Deborah J.
Caro, Jurgen
Kaerger, Joerg
机构
[1] Univ Leipzig, D-04103 Leipzig, Germany
[2] ExxonMobil Res & Engn Co, Annandale, NJ 08801 USA
[3] Leibniz Univ Hannover, D-30167 Hannover, Germany
[4] Univ Montpellier 2, F-34095 Montpellier, France
关键词
D O I
10.1021/ja071265h
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The intracrystalline concentration profiles during molecular uptake of methanol by an initially empty, single crystal of microporous manganese(II) formate (Mn(HCO2)(2)), representing an ionic inorganic-organic hybrid within the MOF family, are monitored by interference microscopy. Within these profiles, a crystal section could be detected where over the total of its extension (approximate to 2 mu m x 50 mu m x 30 mu m) molecular uptake ideally followed the pattern of one-dimensional diffusion. Analysis of the evolution of intracrystalline concentration in this section directly yields the permeability of the crystal surface and the intracrystalline diffusivity as a function of the concentration of the total range of 0 <= theta <= 0.57 covered in the experiments. Within this range, the surface permeability is found to increase by 1 order of magnitude, while, within the limits of accuracy (+/- 30%), the transport diffusivity remains constant, thus reflecting the properties of the lattice gas model.
引用
收藏
页码:8041 / 8047
页数:7
相关论文
共 40 条
[1]   Oriented crystallisation on supports and anisotropic mass transport of the metal-organic framework manganese formate [J].
Arnold, Mirko ;
Kortunov, Pavel ;
Jones, Deborah J. ;
Nedellec, Yannig ;
Kaerger, Joerg ;
Caro, Juergen .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2007, (01) :60-64
[2]   PULSED FIELD GRADIENT NUCLEAR MAGNETIC-RESONANCE AS A PROBE OF LIQUID-STATE MOLECULAR-ORGANIZATION [J].
CALLAGHAN, PT .
AUSTRALIAN JOURNAL OF PHYSICS, 1984, 37 (04) :359-387
[3]  
Chen N. Y., 1994, MOL TRANSPORT REACTI
[4]   Concentration dependence of transport diffusion of ethane in silicalite: A comparison between neutron scattering experiments and atomically detailed simulations [J].
Chong, SS ;
Jobic, H ;
Plazanet, M ;
Sholl, DS .
CHEMICAL PHYSICS LETTERS, 2005, 408 (1-3) :157-161
[5]  
Crank J., 1975, The Mathematics of Diffusion, V1
[6]   Ordered porous materials for emerging applications [J].
Davis, ME .
NATURE, 2002, 417 (6891) :813-821
[7]   SORPTION AND DIFFUSION OF NORMAL-HEPTANE IN 5A ZEOLITE [J].
DOETSCH, IH ;
RUTHVEN, DM ;
LOUGHLIN, KF .
CANADIAN JOURNAL OF CHEMISTRY-REVUE CANADIENNE DE CHIMIE, 1974, 52 (15) :2717-2724
[8]   Microporous manganese formate: A simple metal-organic porous material with high framework stability and highly selective gas sorption properties [J].
Dybtsev, DN ;
Chun, H ;
Yoon, SH ;
Kim, D ;
Kim, K .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2004, 126 (01) :32-33
[9]   Adsorption of gases in metal organic materials: Comparison of simulations and experiments [J].
Garberoglio, G ;
Skoulidas, AI ;
Johnson, JK .
JOURNAL OF PHYSICAL CHEMISTRY B, 2005, 109 (27) :13094-13103
[10]   EFFECT OF CONCENTRATION-DEPENDENCE OF DIFFUSIVITY ON ZEOLITIC SORPTION CURVES [J].
GARG, DR ;
RUTHVEN, DM .
CHEMICAL ENGINEERING SCIENCE, 1972, 27 (02) :417-&