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

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


        Professor 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:

        Aim of this joint project is the rational development of MOF materials for applications in selective adsorption and selective catalysis based on a fundamental understanding of their structure-related functions. Three research groups combine their experience in synthesis/structural analysis, sorption and heterogeneous catalysis to achieve a deeper knowledge on MOF materials with specific functions for technical applications.
        The investigations focus on porous Cu-MOFs with substituted triazolyl benzoate or isophthalate linkers, developed in the first period of this program. They will be modified in order to adjust the pore geometry and to generateactive sites. Size and geometry of the pores and the pore windows will be controlled by linker design (substitution pattern of the triazole and aromatic groups) in order to achieve shape selectivity in adsorption and catalysis, due to differences in shape and size of the adsorptives. Active centres in the MOFs will be generated by introducing a second type of metal ions into the framework. Such heteronuclear MOFs can be synthesized by isomorphous substitution. The resulting selectivity in adsorption and redox catalysis will be studied, e.g., for alkane/alkene separation and alkene oxidation reactions. The correlation of the sorption behavior of the reactants (e.g. CO, O2, hydrocarbons) on MOFs with different linkers and metal sites to their catalytic properties will provide a deeper understanding of the framework-based functions of MOF materials.


        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:

        F. Gul-E-Noor, D. Michel, H. Krautscheid, J. Haase, M. Bertmer
        "Time dependent water uptake in Cu3(btc)2 MOF: Identification of different water adsorption states by H MAS NMR"

        Micropor. Mesopor. Mat. 180 (2013) 8–13.
         

         

        F. Kettner, C. Worch, J. Moellmer, R. Gläser, R. Staudt, H. Krautscheid
        "Synthesis, Crystal Structure and Catalytic Behavior of Homo- and Heteronuclear Coordination Polymers [M(tdc)(bpy)] (M = Fe, Co, Zn, Cd; tdc2– = 2,5-thiophenedicarboxylate)"

        Inorg. Chem. (2013) DOI: 10.1021/ic400857s.
         

         

        F. Gul-E-Noor, D. Michel, H. Krautscheid, J. Haase, M. Bertmer
        "Investigation of the Spin-Lattice Relaxation of 13CO and 13CO2 Adsorbed in the Metal-organic Frameworks Cu3(btc)2 and Cu3-xZnx(btc)2"

        J. Chem. Phys. 139 (2013) 034202.
         

         

        F. Gul-E-Noor, M. Mendt, D. Michel, A. Pöppl, H. Krautscheid, J. Haase, M. Bertmer
        "Adsorption of Small Molecules on Cu3(btc)2 and Cu3-xZnx(btc)2 Metal-Organic Frameworks (MOF) as Studied by Solid-State NMR"

        J. Phys. Chem. C 117 (2013) 7703-7712.
         

         

        A. Viswanath Kuttatheyil, D. Lässig, J. Lincke, M. Kobalz, M. Baias, K. König, J. Hofmann, H. Krautscheid, C. J. Pickard, J. Haase, M. Bertmer
        "Synthesis, Crystal Structure and Solid State NMR Investigations of Heteronuclear Zn/Co MOFs – A Comparative Study"

        Inorg. Chem. 52 (2013) 4431-4442.
         

         

        G. A. Senchyk, A. B. Lysenko, H. Krautscheid, E. B. Rusanov, A. N. Chernega, K. W. Kramer, S.-X. Liu, S. Decurtins, K. V. Domasevitch
        "Functionalized Adamantane Tectons Used in the Design of Mixed-Ligand Copper(II) 1,2,4-Triazolyl/Carboxylate Metal-Organic Frameworks"

        Inorg. Chem. 52 (2013) 863-872.
         

         

        F. Gul-E-Noor, B. Jee, M. Mendt, D. Himsl, A. Pöppl, M. Hartmann, J. Haase, H. Krautscheid, M. Bertmer
        "Formation of Mixed Metal Cu3-xZnx(btc)2 Frameworks with Different Zinc Contents: Incorporation of Zn2+ into the MOF Structure as Studied by Solid-State NMR"

        J. Phys. Chem. 116 (2012) 20866-20873.
         

         

        P. Schmiedel, H. Krautscheid
        "Koordinationspolymeren mit Tris(4-carboxyphenyl)-phosphanoxid als Ligand – Synthese, Kristallstrukturen und topologische Untersuchung"

        Z. anorg. allg. Chem. 638 (2012) 1839-1848.
         

         

        J. Lincke, D. Lässig, M. Kobalz, J. Bergmann, M. Handke, J. Möllmer, M. Lange, C. Roth, A. Moeller, R. Staudt, H. Krautscheid
        "An Isomorphous Series of Cubic, Copper Based Triazolyl Isophthalate MOFs: Linker Substitution and Adsorption Properties"

        Inorg. Chem. 51 (2012) 7579-7586.
         

         

        G. A. Senchyk, A. B. Lysenko, I. Boldog, E. B. Rusanov, A. N. Chernega, H. Krautscheid, K. V. Domasevitch
        "1,2,4-Triazole functionalized adamantanes: a new library of polydentate tectons for designing structures of coordination polymers"

        Dalton Trans. 41 (2012) 8675-8689.
         

         

        M. Bastos Neto, C. Patzschke, M. Lange, J. Möllmer, A. Möller, S. Fichtner, C. Schrage, D. Lässig, J. Lincke, R. Staudt, H. Krautscheid, R. Gläser
        "Assessment of Hydrogen Storage by Physisorption in Porous Materials"

        Energy Environ. Sci. 5 (2012) 8294-8303.
         

         

        Daniel Lässig, Jörg Lincke, Renata Gerhardt and Harald Krautscheid
        "Solid State Syntheses of Coordination Polymers by Thermal Conversion of Molecular Building Blocks and Polymeric Precursors"

        Inorg. Chem. 51 (2012) 6180-6189.
         

         

        J. Moellmer, A. Moeller, C. Patzschke, K. Stein, D. Lässig, J. Lincke, R. Gläser, H. Krautscheid, R. Staudt
        "Pure and mixed gas adsorption of CH4 and N2 on the metal-organic framework Basolite® A100 and a novel copper-based 1,2,4-triazolyl benzoate MOF"

        J. Mater. Chem. 22 (2012) 10274-10286.
         

         

        J. Lincke, D. Lässig, K. Stein, J. Moellmer, A. Viswanath Kuttatheyil, C. Reichenbach, A. Moeller, R. Staudt, G. Kalies, M. Bertmer, H. Krautscheid
        "A Novel Zn4O-Based Triazolyl Benzoate MOF: Synthesis, Crystal Structure, Adsorption Properties and Solid State 13C NMR Investigations"

        Dalton Trans. 41 (2012) 817-824.
         

         

        S. Hertel, M. Wehring, S. Amirjalayer, M. Gratz, J. Lincke, H. Krautscheid, R. Schmid, F. Stallmach
        "NMR studies of benzene mobility in metal-organic framework MOF-5"

        Eur. Phys. J., Appl. Phys. 55 (2011) 20702/1-10.
         

         

        D. Lässig, J. Lincke, J. Möllmer, C. Reichenbach, A. Möller, R. Gläser, G. Kalies, K. A. Cychosz, M. Thommes, R. Staudt, H. Krautscheid
        "A Microporous Copper Metal-Organic Framework with High H2 and CO2 Adsorption Capacity at Ambient Pressure"

        Angew. Chem. 2011, 123, 10528-10532; Angew. Chem. Int. Ed. 2011, 50, 10344-10348.
         

         

        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, 142, 592-600.
         

         

        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.
         

         

        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. 2011, 62-69.
         

         

        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, 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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