Preparation, characterization and catalytic performance of polyoxometalate immobilized on the surface of halloysite
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2019
Authors
Ma, Z.
Wang, R.
Yu, T.
Bi, L.
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Journal of Materials Science, 2019; 54(5):3817-3831
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Polyoxometalates (POMs) are well known to have excellent catalytic performances for oxidation of organic substrates. In this paper, we immobilized POM, Cs₃(NH₄)[{Ru₄O₆(H₂O)₉}₂Sb₂W₂ₒO₆₈(OH)₂]∙9H₂O (SbWRu), on the surface of halloysite nanotubes (HNTs) functionalized by 3-aminopropyltriethoxysilane (Apts) to prepare a novel heterogeneous catalyst, HNTs/Apts/SbWRu, which is never reported in the literature to our knowledge. The catalyst HNTs/Apts/SbWRu was characterized by elemental analysis, IR spectroscopy, X-ray photoelectron spectroscopy, X-ray diffraction, scanning electron microscopy,transmission electron microscopy and N2 adsorption measurements to determine its composition, structure and morphology. The catalytic performance of this catalyst was tested in green oxidation system of n-tetradecane using air as oxidant under the mild reaction condition with normal atmospheric pressure and low temperature and without adding any solvents and additives. Furthermore,in order to find the optimum catalytic reaction condition, we prepared five catalysts containing different amounts of SbWRu, 0.97%, 1.94%, 2.80%,4.23% and 5.87%. The results of the controlled experiments confirmed that the catalyst containing SbWRu of 1.94% exhibited high activity with a conversion(53.30%) and turnover frequency (TOF: 52396 h⁻¹) at the optimal reaction condition.Moreover, this catalyst can be recovered and reused by filtration without significant loss of its catalytic performance for at least five times. The finalconversion of n-tetradecane runs up to 87.97% after five consecutive cycles without the separation of the catalyst HNTs/Apts/SbWRu (1.94%).
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Copyright 2018 Springer Science+Business Media, LLC, part of Springer Nature
Access Condition Notes: Accepted manuscript available after 1 January 2020