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Journal of Coordination Chemistry Volume 67, 2014 - Issue 3
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Original Articles

Four organic–inorganic compounds based on polyoxometalates: crystal structures and catalytic epoxidation of styrene

Chunling WangShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China;Low Carbon Energy Conversion Technology Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, PR China
,
Yuanhang RenShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China
,
Sujiao FengShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China
,
Zuping KongShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China
,
Yichen HuShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China
,
Bin YueShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR ChinaCorrespondence[email protected]
,
Mingli DengShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR China
&
Heyong HeShanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Department of Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials, Fudan University, Shanghai, PR ChinaCorrespondence[email protected]
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Pages 506-521 | Received 10 Nov 2013, Accepted 14 Jan 2014, Published online: 05 Mar 2014
 
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Abstract

Four compounds based on polyoxometalates, [Cu(4-bpo)(H2O)][Cu2(μ2-Cl)(4-bpo)2(H2O)][SiW12O40][N(CH3)4]2·H2O (1), [Cu(4-bpo)]4[P2W18O62][N(CH3)4]2·6H2O (2), [Cu2(μ2-OH)(4-bpo)2(Hina)(H2O)2]2[P2W18O62]·4H2O (3), and [Cu2(Hina)4(H2O)2][H2P2W18O62](Hina)·11H2O (4) (4-bpo=2,5-bis(4-pyridyl)-1,3,4-oxadiazole, ina=isonicotinic acid), have been hydrothermally synthesized and characterized by elemental analysis, IR, and single-crystal X-ray diffraction. The 3-D framework of 1 is composed by Keggin-type polyoxoanions {SiW12} and two types of infinite chains, {Cu(4-bpo)(H2O)}n and {Cu2(μ2-Cl)(4-bpo)2(H2O)}n, through hydrogen bonds. Compound 2 has a 3-D rigid framework which is fabricated by Wells–Dawson type polyoxoanions {P2W18} and Cu-(4-bpo) chains through covalent bonds. Compound 3 contains an infinite {Cu2(μ2-OH)(4-bpo)2(Hina)(H2O)2}n double-chain and {P2W18} polyoxoanions immobilized in the voids between the chains. Compound 4 exhibits a 3-D supramolecular network directed by hydrogen bonds between {P2W18} polyoxoanions and the double paddle-wheel {Cu2(Hina)4(H2O)2}. Compounds 1–4 were tested as heterogeneous catalysts for the epoxidation of styrene using tert-butyl hydroperoxide (TBHP) as oxidant. The compounds show catalytic activity with 2 giving the highest yield of styrene oxide.

Four organic–inorganic hybrid compounds were hydrothermally synthesized based on polyoxometalates, copper salts, and 2,5-bis(4-pyridyl)-1,3,4-oxadiazole or isonicotinic acid ligands. Among those four compounds, compound 2, [Cu(4-bpo)]4[P2W18O62][N(CH3)4]2·6H2O, showed the best catalytic activity for heterogeneous epoxidation of styrene to styrene oxide using tert-butyl hydroperoxide as oxidant.

Funding

This work was supported by the National Natural Science Foundation [grant number 21371035], [grant number 21173050]; and the National Science Foundation for Young Scientists of China [grant number B010204].

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