Effects of rare-earth metal oxides on the desulfurization of Y zeolite
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摘要: 以Y分子筛为母体,采用浸渍法制备了Y2O3/Y、CeO2/Y和La2O3/Y三种吸附剂.以脱除正辛烷中的苯并噻吩为探针反应,考察了稀土金属氧化物负载量、吸附温度、吸附时间和剂油比对吸附剂脱硫性能的影响.结果表明,稀土金属氧化物最佳负载量为5%(质量分数),所得吸附剂在50 ℃、1 h、剂油比1∶30条件下,脱硫率均达到60%以上.甲苯的存在明显降低了吸附剂的脱硫性能.稀土金属氧化物在吸附过程中发生流失,在相同的条件下,三种稀土金属氧化物中,Y2O3的流失量最小,而CeO2的流失量最大,CeO2的流失量是Y2O3的10倍.Abstract: Y2O3/Y, CeO2/Y and La2O3/Y samples were prepared by impregnation with Y zeolites as precursor. Removal of benzothiophene from octane was employed as probe reaction. The effects of loading amount of rare-earth metal oxide, adsorption temperature, adsorption time and ratio of adsorbent to oil on desulfurization have been investigated. The results showed that the optimum loading amount of the rare-earth metal oxide was 5%. More than 60% of benzothiophene was removed over the obtained samples at conditions of 50 ℃, 1 h and 1∶30 of adsorbent to oil ratio. Addition of toluene to the mixture of octane and benzothiophene depressed obviously the desulfurization capability of the samples. The rare-earth metal oxides were washed away during the desulfurization process. The loss amount of Y2O3 was the least, while CeO2 was the largest. The loss amount of CeO2 was 10 times larger than that of Y2O3.
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Key words:
- desulfurization /
- Y zeolites /
- rare-earth metal oxide /
- benzothiophene /
- toluene
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SONG C. An overview of new approaches to deep for desulfurization ultra-clean gasoline, diesel fuel and jet fuel[J].Catal Today, 2003, 86(1/4): 211-263. 王洪国, 姜恒, 徐静, 孙兆林, 张晓彤, 朱赫礼, 宋丽娟. 苯和1-辛烯对Ce(IV)Y分子筛选择性吸附脱硫的影响[J].物理化学学报, 2008, 24(9): 1714-1718. (WANG Hong-guo, JIANG Heng, XU Jing, SUN Zhao-lin, ZHANG Xiao-tong, ZHU He-li, SONG Li-juan.Effects of benzene and 1-octene on desulfurization by selective adsorption with Ce(Ⅳ)Y[J]. Acta Physico-Chimica Sinica, 2008, 24(9): 1714-1718.) 郑珊, 高濂, 郭景坤. 温和条件下介孔分子筛MCM-41的修饰与表征[J]. 无机材料学报, 2000, 15(5): 844-848. (ZHENG Shan, GAO Lian, GUO Jing-kun. Under the mild condition modification and characterization of mesoporous molecular sieve MCM-41[J]. Jounral of Inorganic Materials, 2000, 15(5): 844-848.) VELU S, MA X, SONG C. Selective adsorption for removing sulfur from jet fuel over zeolite-based adsorbents[J]. Ind Eng Chem Res, 2003, 42(21): 5293-5304. HERNANDEZ-MALDONADO A J, YANG R T. Desulfurization of commercial liquid fuels by selective adsorption via-complexation with Cu(Ⅰ)-Y zeolite[J]. Ind Eng Chem Res, 2003, 42(13): 3103-3110. HERNANDEZ-MALDONADO A J, YANG R T.Desulfurization of liquid fuels by adsorption via complexation with Cu(Ⅰ)-Y and Ag-Y zeolite [J]. Ind Eng Chem Res, 2003, 42(1): 123-129. YANG R T, HERNANDEZ-MALDONADO A J, YANG F H. Desulfurization of transportation fuels with zeolites under ambient conditions[J]. Science, 2003, 301(5629): 79- 81. WANG J, XU F, XIE W J, MEI Z J, ZHANG Q Z, CAI J, CAI W M. The enhanced adsorption dibenzothiophene onto cerium/nickel-exchanged zeolite Y[J]. J Hazard Mater, 2009, 163(2/3): 538-543. SHAN J H, LIU X Q, SUN L B, CUI R. Cu-Ce bimetal ion-exchanged Y zeolites for selective adsorption of thiophenic sulfur[J]. Energy Fuels, 2008, 22(6): 3955-3959. POSPISIL M, KANOKOVA P. Effect of different treatments on the reducibilityof NiO-Y2O3 mixed oxides by hydrogen[J]. J Therm Anal Calorim, 1999, 58(1): 77-88. 于善青, 田辉平, 龙军. 改性金属离子对Y型分子筛水热稳定性的影响[J]. 燃料化学学报, 2011, 39(12): 936-943. (YU Shan-qing, TIAN Hui-ping, LONG Jun. Effect of metal element modification on the hydrothermal stability of Y zeolite[J]. Journal of Fuel Chemistry and Technology, 2011, 39(12): 936-943.) SUN L P, GUO X W, XIONG G, WANG X S. Ethylation of coking benzene with ethanol over nano-sized ZSM-5 zeolites: Effects of rare earth oxides on catalyst stability[J]. Catal Commun, 2012, 25(5): 18-21. 韩春玉, 刘道胜, 宋丽娟, 张晓彤, 孙兆林. 噻吩在CeY分子筛上的吸附行为[J]. 工业催化, 2008, 16(6): 27-30. (HAN Chun-yu, LIU Dao-sheng, SONG Li-juan, ZHANG Xiao-tong, SUN Zhao-lin. Absorption behaviors of thiophene on CeY zeolites[J]. Industrial Catalysis, 2008, 16(6): 27-30.) ADRIANA D, CLARK A E.Thermodynamic and structural features of aqueous Ce(III)[J]. J Phys Chem A, 2008, 112(44): 11198-11206. MAGALI D, RICCARDO S, THIERRY C, PIERRE V. Temperature dependence of hydrated La3+ properties in liquid water, a molecular dynamics simulations study[J]. Chem Phys Lett, 2007, 448(1/3): 41-45. ABBASI A, LINDQVIST-REIS P, ERIKSSON L, SANDSTROM D, LIDIN S, PERSSON I, SANDSTROM M. Highly hydrated cations: Deficiency, mobility, and coordination of water in crystalline nonahydrated scandium(III), yttrium(III), and lanthanoid(III) trifluoromethanesulfonates[J]. Chem Eur J, 2005, 11(14): 4065-4077. 刘光华. 稀土材料与应用技术[M]. 北京: 化学工业出版社, 2005. (LIU Guang-hua. Rare earth material and application technology[M]. Beijing: Chemical Industry Press, 2005.) 陈焕章, 李永丹, 赵地顺. 制备条件对吸附剂脱硫性能的影响[J]. 化工科技, 2005, 13(4): 23-26. (CHEN Huan-zhang, LI Yong-dan, ZHAO Di-shun. The effect of preparation condition on the desulfurization capacity of adsorbent[J]. Science & Technology in Chemical Industry, 2005, 13(4): 23-26.) 代镇华, 宋丽娟, 段林海, 孙兆林, 李秀奇, 张晓彤. 噻吩, 苯和正辛烷在NaY和CeY分子筛上的热脱附[J]. 化工科技, 2007, 15(1): 1-4. (DAI Zhen-hua, SONG Li-juan, DUAN Lin-hai, SUN Zhao-lin, LI Xiu-qi, ZHANG Xiao-tong. The thermal desorption of thiophene,benzene and octane on NaY and CeY zeolites[J]. Science & Technology in Chemical Industry, 2007, 15(1): 1-4.) RICHARDEAU D, JOLY G, CANAFF C, MAGNOUX P, GUISNET M, THOMAS M, NICOLAOS A.Adsorption and reaction over HFAU zeolites of thiophene in liquid hydrocarbon solutions [J]. Appl Catal A, 2004, 263(1): 49-61. 张晓彤, 徐静, 宋丽娟, 靳玲玲, 孙兆林. 烯烃对CeY分子筛脱硫效果影响的红外光谱研究[J]. 燃料化学学报, 2010, 38(1): 91-95. (ZHANG Xiao-tong, XU Jing, SONG Li-juan, JIN Ling-ling,SUN Zhao-lin. FT-IR studies on the effect of olefins on desulfurization of a CeY zeolite[J]. Journal of Fuel Chemistry and Technology, 2010, 38(1): 91-95.) GIL B, MIERZYNSKA K, SZCZERBINSKA M, DATKA J. In situ IR and catalytic studies of the effect of coke on acid properties of steamed zeolite Y[J]. Microporous Mesoporous Mater, 2007, 99(3): 328-333.
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