Citation: LIU Ri-Jia, WANG Rui, Korchak Vladimir. Synthesis, Characterization and Catalytic Fuel Ultra-Deep Desulfurization of Keggin-Type Polyoxometalates[J]. Chinese Journal of Inorganic Chemistry, ;2014, 30(3): 563-572. doi: 10.11862/CJIC.2014.061 shu

Synthesis, Characterization and Catalytic Fuel Ultra-Deep Desulfurization of Keggin-Type Polyoxometalates

1.
1 School of Environmental Science and Engineering, Shandong University, Jinan 250100, China;

Received Date: 16 May 2013
Available Online: 11 October 2013
Fund Project: 中国石油天然气集团公司石油科技创新基金(2010D-5006-0405) (2010D-5006-0405) 山东省自然科学基金(ZR2011BM023)资助项目。 (ZR2011BM023)

Keggin-type polyoxometalate catalysts M_x/nH_0.6PW(Zr_0.6H_0.6PW, Al_0.8H_0.6PW, Zn_1.2H_0.6PW, Fe0.8 H0.6PW, Ti_0.6H_0.6PW and Sn_0.6H_0.6PW) and Al_x/3H_3-xPW(AlPW, Al_0.8H_0.6PW, Al_0.5H_1.5PW, Al_0.3H_2.1PW and Al_0.1H_2.7PW) were prepared using 6 metal salts and phosphotungstate. The prepared catalysts were characterized by FTIR, XRD, DSC/TGA and ICP. Al_0.5H_1.5PW is the best catalyst based on the catalytic activity screening results. The catalytic oxidation extraction for fuel ultra-deep desulfurization was studied using hydrogen peroxide as the oxidant and MeCN as the extractant. The effect of catalyst dosage, O/S molar ratio, pre-immersion time of the catalyst in H₂O₂ solution, reaction temperature and initial sulfur content on the desulfurization efficiency was studied. The results show that the sulfur content of simulated diesel is reduced from 350 mg·L^-1 to 2.45 mg·L^-1 with a desulfurization efficiency of 99.3% at 60 min under the following operating conditions: Al_0.5H_1.5PW catalyst/simulated diesel, 0.25%(m/m); molar ratio of O/S=10; pre-immersion time of the catalyst in H₂O₂ solution, 8 min; reaction temperature, 60 ℃; initial sulfur content, 350 mg·L^-1. The efficiency of the oxidation extraction desulfurization is much higher than that of extraction only (45.3% higher). Moreover, very good desulfurization efficiency is obtained for real gasoline and diesel catalytic oxidative desulfurization over Al_0.5H_1.5PW catalyst, and the desulfurization efficiency is not reduced obviously after 5 cycles.
- heteropoly compound;oxidative desulfurization;organo-sulfur;hydrogen peroxide
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沈阳化工大学材料科学与工程学院沈阳 110142