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
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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