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TU Dresden » Fakultät Mathematik und Naturwissenschaften » Fachrichtung Chemie und Lebensmittelchemie » Metal-Organic Frameworks
Overview of granted projects - Part II

Knowledge-based development of supported ZIF membranes for
liquid mixture separation by pervaporation

 

        Consortium:

        Professor Dr. Jürgen Caro, Hannover
        Leibniz University of Hannover
        Institute of Physical Chemistry and Electrochemistry


        Dr. Christian Chmelik, Leipzig
        University of Leipzig
        Department of Physics of Interfaces


        Privatdozent Dr. Siegfried Fritzsche, Leipzig
        University of Leipzig
        Department of Molecular Dynamics and Computer Simulation


        Dr. Michael Wiebcke, Hannover
        Leibniz University of Hannover
        Institute of Inorganic Chemistry


        Project:

        Knowledge-based development of supported ZIF membranes for liquid mixture separation by pervaporation


        Abstract:

        In part I of this project, the principles of nano- and microcrystal formation and 2D layer growth on ceramic supports, the prediction of membrane selectivity by combining mixed gas adsorption and diffusion data as obtained by IR microscopy and Molecular Dynamics computer simulations including framework flexibility were studied and understood, resulting in the preparation of several new types of ZIF (Zeolitic Imidazolate Framework) membranes with molecular sieving separation patterns which have been successfully tested in gas phase separations. In this application we will go the step from gas phase separation to the liquid feed separation by MOF membranes. This has so far not been reported in the literature. By combining the determination of mixed equilibria and mixed component diffusion at high pore filling and under consideration of framework flexibility, the MOF membrane development for liquid mixture separation by pervaporation will go in part II from trial and error to knowledge-based. This new aim requires theoretical and experimental development.


        Results:

         


        From the fundamental understanding of mass transport in MOFs we could go in MOF membrane development the way from trial and error to knowledge-based. The principles of nano- and microcrystal formation and 2D layer growth on ceramic supports, the prediction of membrane selectivity by combining mixed gas adsorption and diffusion data as obtained by IR microscopy and Molecular Dynamics computer simulations including framework flexibility were studied and understood resulting in the preparation of several new types of ZIF membranes with molecular sieving separation patterns which have been successfully developed and tested in gas phase separations.


        Publications:

        Helge Bux, Fangyi Liang, Yanshuo Li, Janosch Cravillon, Michael Wiebcke, and Jürgen Caro
        "Zeolitic Imidazolate Framework Membrane with Molecular Sieving Properties by Microwave-Assisted Solvothermal Synthesis"

        JACS 131 (2009) 16000
         

         

        K. Seehamart , T. Nanok , R. Krishna , J.M. van Baten , T. Remsungnen , S. Fritzsche
        "A Molecular Dynamics investigation of the influence of framework flexibility on self-diffusivity of ethane in Zn(tbip) frameworks"

        Microporous and Mesoporous Materials 125 (2009) 97–100
         

         

        K. Seehamart, T. Nanok, J. Kärger, C. Chmelik, R. Krishna and S. Fritzsche
        "Investigating the reasons for the significant in uence of lattice exibility on self-diffusivity of ethane in Zn(tbip)"

        Micropor. Mesopor.Mater. 130 (2010) 9
         

         

        C. Chmelik , J. Kärger, M. Wiebcke, J. Caro, J.M. van Baten, R. Krishna
        "Adsorption and diffusion of alkanes in CuBTC crystals investigated using infra-red microscopy and molecular simulations"

        Microporous and Mesoporous Materials 117 (2009) 22–32
         

         

        Christian Chmelik,Lars Heinke,Pavel Kortunov,Jing Li,David Olson, Despina Tzoulaki,Jens Weitkamp,and Jörg Karger
        "Ensemble Measurement of Diffusion: Novel Beauty and Evidence"

        Chem. Phys. Chem. 10 (2009) 2623
         

         

        Janosch Cravillon, Simon Münzer,Sven-Jare Lohmeier,Armin Feldhoff, Klaus Huber,and Michael Wiebcke
        "Rapid Room-Temperature Synthesis and Characterization of Nanocrystals of a Prototypical Zeolitic Imidazolate Framework"

        Chem. Mater., Vol. 21, No. 8, 2009, 1410
         

         

        Lars Heinke,Despina Tzoulaki,Christian Chmelik,Florian Hibbe,Jasper M. van Baten, Hyuna Lim,Jing Li, Rajamani Krishna, and Jörg Kärger
        "Assessing Guest Diffusivities in Porous Hosts from Transient Concentration Profiles"

        PRL 102, 065901 (2009), 065901-1 - 065901-4
         

         

        Despina Tzoulaki, Lars Heinke, Hyuna Lim, Jing Li, David Olson, Jürgen Caro, Rajamani Krishna, Christian Chmelik, and Jörg Kärger
        "Assessing Surface Permeabilities from Transient Guest Profiles in Nanoporous Host Materials"

        Angew. Chem. Int. Ed. 2009, 48, 3525 –3528
         

         

        Yan-Shuo Li, Fang-Yi Liang, Helge Bux, Armin Feldhoff, Wei-Shen Yang, and Jürgen Caro
        "Molecular Sieve Membrane: Supported Metal–Organic Framework with High Hydrogen Selectivity"

        Angew. Chem. Int. Ed. 2010, 49, 548 –551
         

         

        Christian Chmelik, Helge Bux,Jürgen Caro, Lars Heinke, Florian Hibbe, Tobias Titze, and Jörg Kärger
        "Mass Transfer in a Nanoscale Material Enhanced by an Opposing Flux"

        PRL 104, 085902 (2010), 085902-1 –085902-4
         

         

        Christian Chmelik, Florian Hibbe, Despina Tzoulaki, Lars Heinke, Jürgen Caro, Jing Li, Jörg Kärger
        "Exploring the nature of surface barriers on MOF Zn(tbip) by applying IR microscopy in high temporal and spatial resolution"

        Microporous and Mesoporous Materials 129 (2010) 340–344
         

         

        Aisheng Huang, Helge Bux, Frank Steinbach, and Jürgen Caro
        "Molecular-Sieve Membrane with Hydrogen Permselectivity: ZIF-22 in LTA Topology Prepared with 3-Aminopropyltriethoxysilane as Covalent Linker"

        Angew. Chem. Int. Ed. 2010, 49, 4958 –4961
         

         

        Yanshuo Li, Fangyi Liang, Helge Bux, Weishen Yang, Jürgen Caro
        "Zeolitic imidazolate framework ZIF-7 based molecular sieve membrane for hydrogen separation"

        Journal of Membrane Science 354 (2010) 48–54
         

         

        Yan-Shuo Li , Helge Bux , Armin Feldhoff , Guo-Ling Li , Wei-Shen Yang and Jürgen Caro
        "Controllable Synthesis of Metal–Organic Frameworks: From MOF Nanorods to Oriented MOF Membranes"

        Adv. Mater. 2010, 22, 3322
         

         

        H. Bux, C. Chmelik, J.M. van Baten, R. Krishna, J. Caro
        "Novel MOF-membrane for molecular sieving predicted by IR-diffusion studies and molecular modeling"

        Advanced Materials 22 (2010) 4741.
         

         

        J. Caro
        "Neue nanoporöse Molekularsiebmembranen: Zeolithe contra MOFs – Gewinner und Verlierer,"

        Chemie Ingenieur Technik 82 (2010) 837
         

         

        C. Chmelik, L. Heinke, R. Valiullin, J. Kärger
        "New view of diffusion in nanoporous materials"

        Chem. Ingen. Tech. 82 (2010) 779.
         

         

        D. Tzoulaki, L. Heinke, H. Lim, J. Li, D. Olson, J. Caro, R. Krishna, C. Chmelik, J. Kärger
        "Bestimmung der Oberflächenpermeabilitäten aus transienten Konzentrationsprofilen in nanoporösen Materialien"

        Angew. Chemie, 121 (2009) 3577.
         

         

        H. Bux, C. Chmelik, R. Krishna, J. Caro
        "Ethene/ethane separation by the MOF membrane ZIF-8: Molecular correlation of Permeation,adsorption, diffusion"

        J. Membr. Sci. (2011), doi:10.1016/j.memsci.2010.12.001.
         

         

        C. Chmelik, H. Bux, H. Voß, J. Caro
        "Adsorption and diffusion - basis for molecular understanding of permeation through molecular sieve membranes"

        Chemie Ingenieur Technik, accepted.
         

         

        L. Hertäg, J. Caro, H. Bux, J. Kärger, C. Chmelik, T. Remsungnen, M. Knauth and S. Fritzsche
        "Diffusion of Methane and Hydrogen in ZIF-8"

        J. Membr. Sci. 377, 36 (2011)
         

         

        K. Seehamart, C. Chmelik, R. Krishna and S. Fritzsche
        " Molecular Dynamics Investigation of the Self-Diffusion of Binary mixture diffusion in the Metal Organic Framework Zn(tbip) accounting for framework exibility"

        Microporous and Mesoporous Materials 143, 125 (2011)


 
 

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