Citation: ZHAO Liu, SONG Shengjie, MA Kangfu, WANG Hong, FU Lihua, LIU Xinyang, CHEN Lidong, CHENG Weiguo. Adsorption-Oxidative Desulfurization Performance of Core-Shell Polyoxometalate/Magnetic Cerium-Iron Nanocomposite Oxide@SiO₂[J]. Chinese Journal of Applied Chemistry, ;2020, 37(12): 1457-1464. doi: 10.11944/j.issn.1000-0518.2020.12.200152 shu

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

ZHAO Liu ^a ,
SONG Shengjie ^a ,
MA Kangfu ^a ,
WANG Hong ^a ,
FU Lihua ^a ,
LIU Xinyang ^a ,
CHEN Lidong ^a,, ,
CHENG Weiguo ^b,,

a.
Faculty of Chemistry and Chemical Engineering, Liaoning Normal University, Dalian, Liaoning 110629, China
b.
Beijing 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

Corresponding author: CHEN Lidong, lidongchhm0809@163.com CHENG Weiguo, wgcheng@ipe.ac.cn
Received Date: 19 May 2020
Revised Date: 10 July 2020
Accepted Date: 11 August 2020

Fund Project: 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.XDA21030500)Liaoning Provincial Education Department Serves Local Projects LF2019002the Research Project on Undergraduate Teaching Reform of General Higher Education in Liaoning Province 2018-471the Special Project of Teacher Education Center of Liaoning Normal University lsjsjyzx201905"Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences XDA21030500

Figures(8)

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/CeFe_xO_y@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 CeFe_xO_y 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/CeFe_xO_y@SiO₂>CeFe_xO_y@SiO₂>CeFe_xO_y. 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/CeFe_xO_y@SiO₂ catalyst becomes a kind of environmental-friendly catalysts with simple preparation method, high catalytic activity and good stability.
- adsorption-oxidative desulfurization,
- phosphomolybdic acid,
- cerium-mixed iron oxide nanocomposites,
- dibenzothiophene
1. [1]
  Song C S. An Overview of New Approaches to Deep Desulfurization for Ultra-clean Gasoline, Diesel Fuel and Jet Fuel[J]. Catal Today, 2003,86(1/2/3/4):211-263.
2. [2]
  Julião D, Mirante F, Ribeiro S O. Deep Oxidative Desulfurization of Diesel Fuels Using Homogeneous and SBA-15-Supported Peroxophosphotungstate Catalysts[J]. Fuel, 2019,241:616-624.
3. [3]
  Bazyari A, Khodadadi A A, Mamaghani A H. Microporous Titania-Silica Nanocomposite Catalyst Adsorbent for Ultra-deep Oxidative Desulfurization[J]. Appl Catal B:Environ, 2016,180(1):65-77.
4. [4]
  Hou L, Zhang Y Q, Hu Z F. Reduced Phosphomolybdate Hybrids as Efficient Visible-Light Photocatalysts for Cr(Ⅵ) Reduction[J]. Inorg Chem, 2019,58(24):16667-16675.
5. [5]
  SONG Fangyuan, DING Yong, ZHAO Congchao. Progress in Polyoxometalates-Catalyzed Water Oxidation[J]. Acta Chim Sin, 2014,72(2):133-144.
6. [6]
  Zhang X M, Zhang Z H, Zhang B H. Synergistic Effect of Zr-MOF on Phosphomolybdic Acid Promotes Efficient Oxidative Desulfurization[J]. Appl Catal B:Environ, 2019,256(1)117804.
7. [7]
  Xu J J, Zhu Z G, Su T. Green Aerobic Oxidative Desulfurization of Diesel by Constructing an Fe-Anderson Type Polyoxometalate and Benzene Sulfonic Acid-Based Deep Eutectic Solvent Biomimetic Cycle[J]. Chinese J Catal, 2020,41(5):868-876.
8. [8]
  MA Kangfu, TONG Huan, LIAO Lin. Efficient Shape-Selective Oxidative Desulfurization by Phosphotungstic Acid/Nanocrystalline Catalyst TS-1[J]. Pet Process Petrochem, 2019,50(8):38-45.
9. [9]
  SONG Shengjie, ZHAO Liu, TONG Huan. Effect of Polyoxometalate Structure on Catalytic Oxidative Desulfurization Performance of Nano-TS-1 Zeolite[J]. Chinese J Appl Chem, 2020,37(8):952-959.
10. [10]
  Guo P, Huang F, Huang Q. Optimization of Biodiesel Production Using a Magnetically Stabilized Fluidized Bed Reactor[J]. J Am Oil Chem Soc, ,89(3):497-504.
11. [11]
  Chaudhuri R G, Paria S. Core/Shell Nanoparticles:Classes, Properties, Synthesis Mechanisms, Characterization, and Applications[J]. Chem Rev, 2012,112(4):2373-2433.
12. [12]
  Wang C X, Zhong H L, Wu W J. Fe₃O₄@C Core-Shell Carbon Hybrid Materials as Magnetically Separable Adsorbents for the Removal of Dibenzothiophene in Fuels[J]. ACS Omega, 2019,4(1):1652-1661.
13. [13]
  Li S W, Wang W, Zhao J S. Magnetic-Heteropolyacid Mesoporous Catalysts for Deep Oxidative Desulfurization of Fuel:The Influence on the Amount of APES Used[J]. J Colloid Interface Sci, 2020,57:337-347.
14. [14]
  LIU Di, TONG Huan, YUAN Linjie. Preparation of High Activity Oxidative Desulfurization Catalyst from Phosphomolybdic Acid and Titania Silica Nanocomposite[J]. Chinese J Appl Chem, 2018,35(11):1351-1356.
15. [15]
  Li X H, Zhang J, Zhou F. Oxidative Desulfurization of Dibenzothiophene and Diesel by Hydrogen Peroxide:Catalysis of H₃PMo₁₂O₄₀ Immobilized on the Ionic Liquid Modified SiO₂[J]. Mol Catal, 2018,452:93-99.
16. [16]
  Xi Z W, Zhou N, Sun Y. Reaction-Controlled Phase-Transfer Catalysis for Propylene Epoxdation to Propylene Oxide[J]. Science, 2001,292(11):1139-1141.
17. [17]
  Jiang F, Wang X, Wu D. Design and Synthesis of Magnetic Microcapsules Based on n-Eicosane Core and Fe₃O₄/SiO₂ Hybrid Shell for Dual-Functional Phase Change Materials[J]. Appl Energy,, 2014,134:456-468.
18. [18]
  Zhu W, Zhu G, Li H. Oxidative Desulfurization of Fuel Catalyzed by Metal-Based Surfactant-Type Ionic Liquids[J]. J Mol Catal A:Chem, 2011,347(1/2):8-14.
19. [19]
  Laguna O H, Centeno M A, Boutonnet M. Fe-Doped Ceria Solids Synthesized by the Microemulsion Method for CO Oxidation Reactions[J]. Appl Catal B:Environ, 2011,106(3/4):621-629.
20. [20]
  Levebyre F. ³¹P MAS-NMR Study of H₃PW₁₂O₄₀ Supported on Silica:Formation of (SiOH₂)⁺(H₂PW₁₂O₄₀)[J]. J Chem Soc Chem Commun, 1992(10):756-757.
21. [21]
  Huang Y W, Wang Y J, Wei S C. Preparation of Graphene/Fe₃O₄/Ni Electromagnetic Microwave Absorbing Nano-Composite Materials[J]. Int J Mod Phys B, 2019,33:1-3.
22. [22]
  Ahmidou L, Vincent P, Ahmed B. Reduction of CeO₂ by Hydrogen-Magnetic-Susceptibility and Fourier-Transform Infrared Ultraviolet and X-Ray Photoelectron-Spectroscopy Measurements[J]. J Chem Soc Faraday Trans, 1991,87(10):1601-1609.
23. [23]
  Xu J, Li H C, Wang S T. Ultra-deep Desulfurization via Reactive Adsorption on Peroxophosphomolybdate/Agarose Hybrids[J]. Chemosphere, 2014,111:631-637.
24. [24]
  Xu L L, Li W, Hu J L. Transesterification of Soybean Oil to Biodiesel Catalyzed by Mesostructured Ta₂O₅-Based Hybrid Catalysts Functionalized by Both Alkyl-Bridged Organosilica Moieties and Keggin-Type Heteropoly Acid[J]. J Mater Chem, 2009,19(45):8571-8579.
25. [25]
  Hernández-Maldonado A J, Yang R T. Desulfurization of Commercial Liquid Fuels by Selective Adsorption via π-Complexation with Cu(Ⅰ)-Y Zeolite[J]. Ind Eng Chem Res, 2003,42(13):3103-3110.
26. [26]
  LIU Chang, YAN Zhiyi, LI Qiaoling. Research Progress of Selective Adsorption Desulfurization[J]. Chem Ind Eng Prog, 2019,38(11):5114-5126.
27. [27]
  Misono M. Unique Acid Catalysis of Heteropoly Compounds (Heteropolyoxometalates) in the Solid State[J]. Chem Commum, 2001(13):1141-1153.
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沈阳化工大学材料科学与工程学院沈阳 110142

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

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通讯作者: 陈斌, bchen63@163.com

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