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Issue 27, 2018
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Hybrid dimers based on metal-substituted Keggin polyoxometalates (metal = Ti, Ln) for cyanosilylation catalysis

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Abstract

Six novel organic–inorganic hybrid polyoxometalate derivatives, K[(H2O)4(3-Hpic)2Ce][(H2O)5(3-Hpic)2Ce][PW10Ti2O40]·11H2O 1, K[(H2O)4(3-Hpic)2Nd][(H2O)5(3-Hpic)2Nd][PW10Ti2O40]·12H2O 2, K[(H2O)4(3-Hpic)2Sm][(H2O)5(3-Hpic)2Sm][PW10Ti2O40]·8H2O 3, H[(H2O)7(4-Hpic)La][(4-Hpic)2LaPW11O39]·14.5H2O 4, H[(H2O)7(4-Hpic)Ce][(4-Hpic)2CePW11O39]·7.5H2O 5, and K(4-Hpic)0.5[(H2O)6(4-Hpic)Nd][(4-Hpic)2NdPW11O39]·10H2O 6, (3-Hpic = 3-picolinic acid; 4-Hpic = 4-picolinic acid) have been synthesized and characterized by elemental analysis, IR, solid state UV-vis spectroscopy, thermal gravimetric analysis, powder X-ray diffraction and single-crystal X-ray diffraction. Isostructural compounds 1–3 are hybrid dimers that consist of two Ti-substituted Keggin-type polyoxoanions [PW10Ti2O40]7− and four Ln-3-Hpic coordination groups. The strong hydrogen bonds in 1–3 can make these dimers yield a 1D supramolecular chain. Compounds 4–6 are also dimers constructed from two lanthanide-substituted Keggin-type polyoxoanions [PW11LnO39]4− and four 4-Hpic ligands, which are further linked by two Ln-4-Hpic groups to form a bi-supporting structure. Then these subunits are joined together by strong hydrogen-bonding interactions between polyoxoanions and coordinated water molecules to produce a 2D supramolecular framework. All these compounds as heterogeneous Lewis acid–base catalysts show high activity and high selectivity for the cyanosilylation of different carbonyl compounds under solvent-free conditions, and can be recycled without any obvious inactivation.

Graphical abstract: Hybrid dimers based on metal-substituted Keggin polyoxometalates (metal = Ti, Ln) for cyanosilylation catalysis

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Publication details

The article was received on 30 Jan 2018, accepted on 08 Jun 2018 and first published on 09 Jun 2018


Article type: Paper
DOI: 10.1039/C8DT00389K
Citation: Dalton Trans., 2018,47, 9079-9089
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    Hybrid dimers based on metal-substituted Keggin polyoxometalates (metal = Ti, Ln) for cyanosilylation catalysis

    H. An, Y. Zhang, Y. Hou, T. Hu, W. Yang, S. Chang and J. Zhang, Dalton Trans., 2018, 47, 9079
    DOI: 10.1039/C8DT00389K

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