Effect of Polyoxometalate Structure on Catalytic Oxidative Desulfurization Performance of Nano Titanium Silicalite-1 Zeolite

doi:10.11944/j.issn.1000-0518.2020.08.200046

Chinese Journal of Applied Chemistry ›› 2020, Vol. 37 ›› Issue (8): 952-959.DOI: 10.11944/j.issn.1000-0518.2020.08.200046

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Effect of Polyoxometalate Structure on Catalytic Oxidative Desulfurization Performance of Nano Titanium Silicalite-1 Zeolite

SONG Shengjie^a, ZHAO Liu^a, TONG Huan^a, ZHAO Peng^a, MA Kangfu^a, CHU Yu^a, CHEN Lidong^a*, CHENG Weiguo^b*

^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:2020-02-18 Published:2020-08-01 Online:2020-08-07
Contact: CHEN Lidong, lecturer; Tel/Fax:0411-82158329; E-mail:lidongchhm0809@163.com; Research interests:catalysis of polyacid, energy chemical industy; CHENG Weiguo, researcher, Tel: 010-62554241; E-mail:wgcheng@ipe.ac.cn; Research interests:green catalysis science and engineering.
Supported by:
Liaoning Provincial Education Department Serves Local Projects (No. LF2019002), Research Project on Undergraduate Teaching Reform of General Higher Education in Liaoning Province(No.2018-471), Special Project of Teacher Education Center of Liaoning Normal University(No.lsjsjyzx201905) and “Transformational Technologies for Clean Energy and Demonstration”, Strategic Priority Research Program of the Chinese Academy of Sciences, Grant(No.XDA 21030500)

Abstract

Abstract: Nano titanium silicalite-1 (TS-1) zeolite catalysts loaded with a series of molybdenum-containing polyoxometalate (POM) were synthesized by the impregnation method. These catalysts were characterized by SEM, UV-vis, BET, XRD, ³¹P MAS-NMR and ²⁹Si MAS-NMR spectroscopy. The characterization results show that the Keggin structure in the catalysts can be remained after calcination or drying under the low temperature, but ammonium molybdate changed into molybdenum trioxide after calcination at 550 ℃. A model of oil (n-octane solution of thiophene, benzothiophene and dibenzothiophene) was used to value catalytic oxidation desulfurization performance of these catalysts. It is found that the oxidative desulfurization efficiencies decrease in the order of Mo-POM (Keggin type)＞Mo-POM (Anderson type)＞Mo-POM (Dawson type)＞molybdenum trioxide. When the reaction conditions are the model of V(simulated oil)=V(ethanol)=10.0 mL, m(catalyst)=0.2 g, n(H₂O₂)∶n(S)=10∶1, temperature=60 ℃, the desulfurization activity order of sulfur compounds is thiophene＞dibenzothiophene＞benzothiophene, which is obviously different from that of either TS-1 zeolite or POM. This may be derived from the synergy of the shape selectivity of nano-TS-1 zeolite and the electron cloud density of POM on the oxidation activity of organic sulfur molecules. Furthermore, the Keggin type Mo-POM-TS-1 catalysts show excellent recycling stability. All of which cause Mo-POM (Keggin type)-TS-1 catalysts to become a kind of environmental-friendly catalysts with simple preparation method, high catalytic activity and good stability.

Key words: polyoxometalate, nano-TS-1 zeolite, oxidative desulfurization, structural effect

SONG Shengjie, ZHAO Liu, TONG Huan, ZHAO Peng, MA Kangfu, CHU Yu, CHEN Lidong, CHENG Weiguo. Effect of Polyoxometalate Structure on Catalytic Oxidative Desulfurization Performance of Nano Titanium Silicalite-1 Zeolite[J]. Chinese Journal of Applied Chemistry, 2020, 37(8): 952-959.

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Effect of Polyoxometalate Structure on Catalytic Oxidative Desulfurization Performance of Nano Titanium Silicalite-1 Zeolite

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