CIESC Journal ›› 2014, Vol. 65 ›› Issue (8): 3012-3018.doi: 10.3969/j.issn.0438-1157.2014.08.023

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Catalytic performance of metal phthalocyanine loaded on MCM-41 molecular sieve in oxidation desulfurization

ZHANG Juan, REN Tengjie, HU Yanhui, LI Junpan, WANG Chunfang, ZHAO Dishun   

  1. College of Chemistry and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, Hebei, China
  • Received:2013-11-11 Revised:2014-04-12 Online:2014-08-05
  • Supported by:

    supported by the National Natural Science Foundation of China (21106032).

Abstract: Eight kinds of metal phthalocyanine (Pc) were loaded into MCM-41 by impregnation method,and were characterized by infrared spectrum. The catalytic activities of the eight supported metal phthalocyanine in the desulfurization were investigated with dibenzothiophene (DBT) as the reaction substrate, air as oxidant and caprolactam-tetrabutylammonium bromide ionic liquid as solvent. The reaction condition was investigated in detail. The results showed that MCM-41/CoPc was the best catalyst among the eight supported metal phthalocyanine catalysts. The removal ratio of DBT is up to 97.56% for 1 h under the optimal reaction condition (the ratio of ionic liquid to model oil 1:1, the amount of catalyst 0.004 g·(10 ml model oil)-1, air flow rate 50 ml·min-1 and room temperature). The oxidized product of DBT is DBT sulphone. Different sulfur compounds were also investigated. The result shows that sulfur removal of different sulfur all are up to 90%. The removal ratio of DBT doesn't decrease obviously, after reused for four times with this catalyst.

Key words: metal phthalocyanine, molecular sieve, dibenzothiophene, catalysis, ionic liquids

CLC Number: 

  • O623.83
[1] Castillo K, Parsons J G, Chavez D, Chianelli R R. Oxidation of dibenzothiophene to dibenzothiophene-sulfone using silica gel [J]. J.Catal., 2009, 268 (2): 329-334
[2] Zhang Juan (张娟), Zhao Dishun (赵地顺), Yang Jie (杨洁), et al. Study on photosensitied oxidative desulfurization of dibenzothiophene by riboflavin [J]. Chemical Journal of Chinese Univeristies (高等学校化学学报),2011, 32 (5): 1118-1122
[3] Yu Weizhao (于维钊), Zheng Jingtang (郑经堂), He Xiaochao (何小超), et al. Synthesis of spherical activated carbon loaded with metal particles and its performance of thiophene adsorption [J]. Journal of Chemical Industry and Engineering (China) (化工学报), 2008, 59 (11): 2824-2829
[4] Wang Jianlong (王建龙), Zhao Dishun (赵地顺), Zhou Erpeng (周二鹏), et al. Desulfurization of gasoline by extraction with N-alkyl-pyridinium-based ionic liquid [J]. Journal of Fuel Chemistry and Technology (燃料化学学报), 2007, 35 (3): 293-296
[5] Han Jinyu (韩金玉), Wu Yilin (吴懿琳), Li Yi (李毅). Applied research on biodesulfurization technique [J]. Chemical Industry and Engineering Progress (化工进展), 2003, 22 (10): 1072-1075
[6] Sujit Mondal, Yelda Hangun-Balki, Larissa Alexandrova, et al. Oxidation of sulfur components in diesel fuel using Fe-TAML catalysts and hydrogen peroxide [J]. Catalysis Today, 2006, 116 (7): 554-5611
[7] Zhang Juan (张娟), Zhao Dishun (赵地顺), Chen Yingman (陈英曼), et al. Development on oxidant in oxidative desulfurization of fuel oil [J]. Chemical Research and Application (化学研究与应用), 2007, 19 (6): 577-582
[8] Vasily H, Fajula F, Bousquet J. Mild oxidation with H2O2 over Ti-containing molecular sieves-a very efficient method removing aromatic sulfur compounds from fuels [J]. J.Catal., 2001, 198: 179-186
[9] Shen Yongjia (沈永嘉). The Synthesis and Application of Phthalocyanin (酞菁的合成与应用) [M]. Beijing: Chemical Industry Press, 2000:166-183
[10] Grootboorn N, Nyokong T. Iron perchloric phthalocyanine and tetra-sulfo phthalocyanine catalyzed oxidation of cyclohexane using hydrogen peroxide, chloroperoxybenzoic acid and tert-butyl hydroperoxide as oxidants [J]. J.Mol.Catal.A: Chem., 2002, 179: 113-123
[11] Chauhan S M S, Kumar A, Srinivas K A. Oxidation of thiols with molecular oxygen catalyzed by cobalt(Ⅱ) phthalocyanines in ionic liquid [J]. Chem.Commun., 2003 (18): 2348-2349
[12] Zhou Xinrui, Li Juan, Wang Xiuna, et al. Oxidative desulfurization of dibenzothiophene based on molecular oxygen and iron phthalocyanine [J].Fuel Process Technology, 2009, 90: 317-323
[13] Cao Yucai (曹育才), Li Jianlong (李建龙), Jiang Xuanzhen (姜玄珍). Selective hydrodechlorodechlorination of dichlorodifluorination of dichlorodifluoromethane over supported palladium phthalocyanine catalysts [J]. Journal of Chemical Industry and Engineering (China) (化工学报), 2004, 55 (3): 373-378
[14] Jin Chun (晋春), Ma Jinghong (马静红), Fan Binbin (范彬彬), et al. Preparation, characterization and properties of cobalt phthalocyanine covalent bonded to MCM-41 [J]. Chinese Journal of Inorganic Chemistry (无机化学学报), 2005, 21 (12):1838-1843
[15] Zhang Dan (张丹), Chang Xiaohong (常晓红), Zhang Bing (张兵), et al. Enzyme-like catalytic function of metalphthalocyanine derivatives and their applications [J]. Journal of Liaoning University: Natural Sciences Edition (辽宁大学学报:自然科学版), 2003, 30 (1): 87-90
[16] Kadgaonkara M D, Iahaa S C, Pandey R K, et al. Cerium-containing MCM-41 materials as selective acylation and acylation catalysts [J]. Catal.Today, 2004, 97 (4): 225-231
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