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

Heteronuclear MOFs for applications in adsorption and redox catalysis

 

        Consortium:

        Professor Dr. Roger Gläser, Leipzig
        University of Leipzig
        Department of Chemistry and Mineralogy
        Institute of Chemical Technology

        Professor Dr. Harald Krautscheid, Leipzig
        University of Leipzig
        Department of Chemistry and Mineralogy
        Institute of Inorganic Chemistry

        Prof. Dr.-Ing. Reiner Staudt, Offenburg
        University of Applied Sciences Offenburg
        Department of Mechanical and Process Engineering

        Project:

        Heteronuclear MOFs for applications in adsorption and redox catalysis

        Abstract:

        The purpose of this joint project is the development of strategies for synthesis of metal organic frameworks (MOFs) with a stable and accessible pore system, in which adsorption of gases and/or catalytic conversions are possible. In one- and two-step syntheses especially heteronuclear MOFs will be prepared with one type of metal ions as nodes giving rise to high stability, the other metal ions with flexible coordination or oxidation number should allow specific host-guest interactions.
        One aim is to determine adsorption equilibrium and kinetic data of pure gases and gas mixtures on MOFs for hydrogen and methane cleaning and storage. These investigations will deliver to the partners in the priority program gas adsorption equilibrium data, i.e. the adsorption isotherms (or adsorption isobars). This information is necessary to calculate isosteric heats of adsorption, selectivities of multicomponent adsorption and, by analyzing uptake curves, the thermodynamic factor correlating transport and self-diffusivities. The prepared MOFs will be evaluated as catalysts for selected redox conversions. These include the decomposition of N2O, the oxidation of CO, lower alkanes and lower alcohols as well as the hydrogenation of CO and lower olefins.

        Results:

         

        In order to explore the potential of selected novel open metal organic frameworks (MOFs) for gas storage applications, we performed a systematic physical adsorption study with hydrogen, methane and carbon dioxide as adsorptives over a wide range of temperatures (from 77 - 323 K) and pressures (0 – 3 MPa) by using a volumetric low-pressure adsorption analyzer and a high pressure gravimetric system. The advanced interpretation of these adsorption data in combination with the results from a comprehensive structural and surface characterization (by a combination of experimental methods including nitrogen and argon adsorption at 77 and 87 K) allows one assessing the potential of this novel soc-MOF for gas storage applications.

         

        The influence of the incorporation of redox-active transition metals into MOF materials towards their catalytic performance is investigated in this subproject. At first, the Lewis-acidic nature as one catalytically relevant property of MOFs is tested in the rearrangement of ?-pinene oxide to characterize these materials. Further research is aimed at probing the behavior of redox-active, heteronuclear MOFs in selected heterogeneously catalyzed liquid- and gas-phase conversions.

        Publications:

        J.Moellmer, E.B. Celer, R. Luebke, A.J. Cairns, R. Staudt, M. Eddaoudi and M. Thommes
        "Insights on Adsorption Characterization of Metal-Organic Frameworks: A Benchmark Study on the Novel soc-MOF"
        Micropor. Mesopor. Mater. 2011, 138, 140-148
         

         

        J. Moellmer, A. Moeller, F. Dreisbach, R. Glaeser, R. Staudt
        "High pressure adsorption of hydrogen, nitrogen, carbon dioxide and methane on the metal–organic framework HKUST-1"
        Micropor. Mesopor. Mater. 2011, 138, 140-148
         

         

        C. Reichenbach, G. Kalies, J. Lincke, D. Lässig, H. Krautscheid, J. Moellmer, M. Thommes
        "Unusual Adsorption Behavior of a Highly Flexible Copper-Based MOF"
        Micropor. Mesopor. Mater. 2011, doi: 10.1016/j.micromeso.2011.01.005
         

         

        C. Reichenbach, G. Kalies, J. Lincke, D. Lässig, H. Krautscheid, J. Moellmer, M. Thommes
        "Unusual Adsorption Behavior of a Highly Flexible Copper-Based MOF"
        Micropor. Mesopor. Mater. 2011, doi: 10.1016/j.micromeso.2011.01.005
         

         

        D. Lässig, J. Lincke, J. Griebel, R. Kirmse, H. Krautscheid
        "Synthesis, Crystal Structure, and Electron Paramagnetic Resonance Investigations of Heteronuclear CoII/ZnII and CoII/CdIICoordination Polymers"
        Inorg. Chem. 2011, 50, 213-219.
         

         

        E. V. Govor, A. B. Lysenko, D. Quinonero, E. B. Rusanov, A. N. Chernega,J. Moellmer, R. Staudt, H. Krautscheid, A. Frontera, K. V. Domasevitch
        "Self-assembly hexanuclear metallacontainer hosting halogenated guest species and sustaining structure of 3D coordination framework"
        Chem. Commun. 2010, doi: 10.1039/C0CC04433D
         

         

        J. Lincke, D. Lässig, J. Moellmer, C. Reichenbach, A. Puls, A. Moeller, R. Gläser, G. Kalies, R. Staudt, H. Krautscheid
        "A novel copper-based MOF material: synthesis, characterization and adsorption studies"
        Micropor. Mesopor. Mater. 2010, doi: 10.1016/j.micromeso.2010.11.017
         

         

        J. Lincke, D. Lässig, H. Krautscheid
        "Highly functionalised 3,4,5-trisubstituted 1,2,4-triazoles for future use as ligands in coordination polymers"
        Tetrahedron Letters 2010, 51, 653-656
         

         

        O. V. Sharga, A. B. Lysenko, H. Krautscheid, K. V. Domasevitch
        "A three-dimensional heterometallic CuI/VIV 1,2-bis(1,2,4-triazol-4-yl)ethane framework: a new insight into the structure of vanadium oxyfluoride coordination hybrids"
        Acta Crystallogr. 2010, C66, m269-m272.
         

         

        A. B. Lysenko, G. A. Senchyk, J. Lincke, D. Lässig, A. A. Fokin, E. D. Butova, P. R. Schreiner, H. Krautscheid, K. V. Domasevitch
        "Metal oxide-organic frameworks (MOOFs), a new series of coordination hybrids constructed from molybdenum(VI) oxide and bitopic 1,2,4-triazole linkers"
        Dalton Trans. 2010, 4223-4231
         

         

        E. V. Govor, A. B. Lysenko, E. B. Rusanov, A. N. Chernega, H. Krautscheid, K. V. Domasevitch
        "Anion Tuning of Cu(II)/4,4'-Bi-1,2,4-Triazole Coordination Polymers"
        Z. Anorg. Allg. Chem. 2010, 636, 209-217
         

         

        J. Lincke, D. Lässig, H. Krautscheid
        "Halogeno(triazolyl)zinc complexes as molecular building blocks for metal–organic frameworks"
        Acta Crystallogr. 2009, C65, m488-m490
         

         

        G. A. Senchyk, A. B. Lysenko, E. B. Rusanov, A. N. Chernega, H. Krautscheid, K. V. Domasevitch
        "Polynuclear and polymeric metal complexes based upon 1,2,4-triazolyl functionalized adamantanes"
        Inorg. Chim. Acta 2009, 362, 4439-4448
         

         

        I. A. Gural'skiy, D. Escudero, A. Frontera, P. V. Solntsev, E. B. Rusanov, A. N. Chernega, H. Krautscheid, K. V. Domasevitch
        "1,2,4,5-Tetrazine: an unprecedented µ4-coordination that enhances ability for anion...p interactions"
        Dalton Trans. 2009, 2856-2864
 
 

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