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Synthesis of Convertible {PO4[WO3\(\rightleftharpoons\) W(O)2(O2)]4}-DMA16 in SBA-15 Nanochannels and Its Catalytic Oxidation Activity

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Abstract

A phase transfer catalyst ({PO4[WO3]4}-DMA16) had been first synthesized and stabilized in mesochannels of (3-chloropropyl)trimethoxysilane-functionalized mesoporous silica SBA-15 to build an active nano-environment for triphase cyclohexene oxidation. Tungsten precursor ({PO4[WO3]4}3−) and organic amino N,N-dimethylhexadecan-1-amine (DMA16) self-assembled in channels of SBA-15 to form a hybrid catalyst {PO4[WO3]4}-DMA16-SBA-15, which combined advantages of homogeneous and heterogeneous catalysts. Insoluble {PO4[WO3]4}-DMA16 formed soluble {PO4[W(O)2(O2)]4}-DMA16 active species with the aid of H2O2, and when H2O2 was consumed out, {PO4[WO3]4}-DMA16 was recombined. In addition, free remaining organic moieties (–Cl and -DMA16) on the surface of SBA-15 allowed {PO4[WO3]4}-DMA16-SBA-15 catalyst possessed more hydrophobic surface property, which further facilitated the compatibility between organic reactant cyclohexene and inorganic H2O2 molecules. The easy reusability of {PO4[WO3]4}-DMA16-SBA-15 catalyst for five catalytic runs without distinct change in catalytic activity was a significant “green” attribute of this catalyst.

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Acknowledgements

This work was supported by Major Program of Shandong Province Natural Science Foundation [Grant No. ZR2017ZC0632]; National Natural Science Foundation of China [Grant No. NSFC21376128].

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Authors and Affiliations

  1. State Key Laboratory Base for Eco-Chemical Engineering, College of Chemical Engineering, Qingdao University of Science and Technology, No. 53 Zhengzhou Road, Qingdao, 266042, China

    Manman Jin & Zhiguo Lv

  2. College of Marine Science and Biological Engineering, Qingdao University of Science and Technology, No. 53 Zhengzhou Road, Qingdao, 266042, China

    Zhenmei Guo

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  1. Manman Jin
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Correspondence to Zhiguo Lv.

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Jin, M., Guo, Z. & Lv, Z. Synthesis of Convertible {PO4[WO3\(\rightleftharpoons\) W(O)2(O2)]4}-DMA16 in SBA-15 Nanochannels and Its Catalytic Oxidation Activity. Catal Lett 149, 2794–2806 (2019). https://doi.org/10.1007/s10562-019-02761-3

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