Chinese Journal of Applied Chemistry ›› 2020, Vol. 37 ›› Issue (12): 1457-1464.DOI: 10.11944/j.issn.1000-0518.2020.12.200152

• Full Papers • Previous Articles    

Adsorption-Oxidative Desulfurization Performance of Core-Shell Polyoxometalate/Magnetic Cerium-Iron Nanocomposite Oxide@SiO2

ZHAO Liua, SONG Shengjiea, MA Kangfua, WANG Honga, FU Lihuaa, LIU Xinyanga, CHEN Lidonga*, CHENG Weiguob*   

  1. aFaculty of Chemistry and Chemical Engineering,Liaoning Normal University,Dalian,Liaoning 110629,China;
    bBeijing Key Laboratory of Ionic Liquids Clean Process,Key Laboratory of Green Process and Engineering,Chinese Academy of Sciences,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 110190,China
  • Received:2020-05-19 Revised:2020-07-10 Accepted:2020-08-11 Online:2020-12-01 Published:2020-12-07
  • Contact: CHEN Lidong,lecturer; Tel/Fax:0411-82158329;; Research interests:catalysis of polyacid; energy chemical industy
    Co-corresponding author:CHENG Weiguo, professor; Tel:010-62554241; Fax:010-62561822;; Research interests:green catalysis science and engineering
  • Supported by:
    Liaoning Provincial Education Department Serves Local Projects(No.LF2019002), the Research Project on Undergraduate Teaching Reform of General Higher Education in Liaoning Province(No.2018-471), the Special Project of Teacher Education Center of Liaoning Normal University(No.lsjsjyzx201905), “Transformational Technologies for Clean Energy and Demonstration”, Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA 21030500)

Abstract: The manganese-cerium mixed iron oxide nanocomposites were synthesized by hydrothermal synthesis method. The surface was wrapped by SiO2 by chemical vapor deposition to prepare the core-shell magnetic material which was then loaded by H2O2 with Keggin structure phosphomolybdic acid (HPMo) to synthesize the HPMo-H2O2/CeFexOy@SiO2 adsorption-oxidative desulfurization catalyst. The catalyst was characterized by SEM, TEM, FT-IR, XRD, 31P MAS-NMR and XPS. The results of SEM, TEM and XPS characterization show that CeFexOy is wrapped by SiO2 to form core-shell nanocomposite material. The Keggin-type structure is retained after being loaded by HPMo-H2O2 and a little peroxophosphomolybdate active species are produced in this process. The active order of different catalysts on the adsorption and oxidation desulfurization presents as the following:HPMo-H2O2/CeFexOy@SiO2>CeFexOy@SiO2>CeFexOy. The introduction of HPMo greatly improves the adsorption activity of organic sulfides, especially its remarkable performance in oxidative desulfurization. The improvement of the performance in oxidative desulfurization is due to the “pseudo-liquid phase” reaction process of polyoxometalate. The dibenzothiophene(DBT) oxidation removal rate reaches 99.4% under such conditions:m(oil)∶m(catalyst)=35∶1, n(H2O2)∶n(S)=10∶1 at 60 ℃ for 3 h. The prepared magnetic core-shell oxidative-desulfurization catalyst has ideal recycling performance for oxidative removal of DBT. HPMo-H2O2/CeFexOy@SiO2 catalyst becomes a kind of environmental-friendly catalysts with simple preparation method, high catalytic activity and good stability.

Key words: adsorption-oxidative desulfurization, phosphomolybdic acid, cerium-mixed iron oxide nanocomposites, dibenzothiophene

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