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
1. [1]
  [1] Service R F. Science, 1999,285:682-682
2. [2]
  [2] Voss D. Science, 1999,285:683-683
3. [3]
  [3] Yang R T, Hemandez M, Yang E H, et al. Science, 2003, 301:79-81
4. [4]
  [4] WANG En-Bo(王恩波), HU Chang-Wen(胡长文), XU Lin (许林). Introduction to Polyoxometalate Chemistry(多酸化学导论). Beijing: Chemical Industry Press, 1998.
5. [5]
  [5] WANG En-Bo(王恩波), XU Lin(许林), HUANG Ru-Dan (黄如丹), et al. Sci. China B(中国科学 B), 1991,11:1121-1129
6. [6]
  [6] Kozhevnikov I V. Catalysis by Polyxometalates: Catalysis forFine Chemical Synthesis, Vol.2)(精细化学品的催化合成:多酸及其催化). Translated by TANG Pei-He(唐培堃), LI Xiang-Gao(李祥高), WANG Shi-Rong(王世荣), Beijing: Chemical Industry Press, 2005.
7. [7]
  [7] Chen N, Yang R T. J. Catal., 1995,157:76-86
8. [8]
  [8] Yazu K, Yamamoto Y, Furuya T, et al. Energy Fuels. 2001, 15(6):1535-1538
9. [9]
  [9] Hirai T, Shiraishi Y, Ogawa K, et al. Ind. Eng. Chem. Res., 1997,36(3):530-533
10. [10]
  [10] He L N, Li H M, Zhu W S, et al. Ind. Eng. Chem. Res., 2008,47(8):6890-6895
11. [11]
  [11] Wang R, Zhang G F, Zhao H X. Catal. Today, 2010,149 (1/2):117-121
12. [12]
  [12] Wang R, Yu F L, Zhang G F, et al. Catal. Today, 2010,150 (1/2):37-41
13. [13]
  [13] Wang H, Wang R. Collect. Czech. Chem. Commun., 2011, 76(12):1595-1605
14. [14]
  [14] Zang G F, Wang R, Yu F L, et al. Chem. Pap., 2009,63(5): 617-619
15. [15]
  [15] SONG Hua(宋华), LI Guo-Zhong(李国忠), LI Zheng-Guang(李正光). J. Fuel Chem. Technol. (燃料化学学报), 2010,38(4):439-444
16. [16]
  [16] REN Xiang-Hong(任祥红). Thesis for Masterate of Tianjin University(天津大学硕士论文). 2007.
17. [17]
  [17] Qiu J H, Wang G H, Zeng D L, et al. Fuel Process. Technol., 2009,90(12):1538-1542
18. [18]
  [18] QIU Jiang-Hua(邱江华), WANG Guang-Hui(王光辉), QIUWen-Jie(邱文杰), et al. J. Yunan. Univ.: Nat. Sci. End. (云南大学学报:自然科学版), 2009,31(5):499-504
19. [19]
  [19] Li J, Wang X H, Zhu W M, et al. ChemSusChem. 2009,2(2): 177-183
20. [20]
  [20] Shi W, Zhao J, Yuan X, et al. Chem. Eng. Technol., 2012, 35(2):347-352
21. [21]
  [21] WANG En-Bo(王恩波), ZHANG Lan-Cui(张澜翠), SHEN En-Hong(沈恩洪), et al. Sci. China B(中国科学 B), 1992,7: 673-682
22. [22]
  [22] WANG En-Bo(王恩波), REN Qun-Xiang(任群翔), WANG Zuo-Ping(王作屏), et al. Chinese J. Inorg Chem.(无机化学学报), 1993,1(9):65-70
23. [23]
  [23] Catherine A, Genevieve C, Nicole P, et al. Inorg. Chem., 1991,30(23):4409-4415
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