Preparation of Co-Mo/SiO2-Al2O3 catalyst for hydrotreating lubricating oil

ZHANG Jin-ling; SONG Chun-min; WANG Yan-zhen; DUAN Hong-ling

Volume 46 Issue 5

May 2018

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2018 > 46(5): 543-550

ZHANG Jin-ling, SONG Chun-min, WANG Yan-zhen, DUAN Hong-ling. Preparation of Co-Mo/SiO2-Al2O3 catalyst for hydrotreating lubricating oil[J]. Journal of Fuel Chemistry and Technology, 2018, 46(5): 543-550.

Citation:

ZHANG Jin-ling, SONG Chun-min, WANG Yan-zhen, DUAN Hong-ling. Preparation of Co-Mo/SiO₂-Al₂O₃ catalyst for hydrotreating lubricating oil[J]. Journal of Fuel Chemistry and Technology, 2018, 46(5): 543-550.

Citation:

PDF( 5195 KB)

Preparation of Co-Mo/SiO₂-Al₂O₃ catalyst for hydrotreating lubricating oil

College of Chemical Engineering, China University of Petroleum(East China), Qingdao 266580, China

More Information

Corresponding author: WANG Yan-zhen, E-mail: yanzhenw@upc.edu.cn
Received Date: 2017-12-15
Rev Recd Date: 2018-03-12

Available Online: 2021-01-23

Publish Date: 2018-05-10

Abstract

Abstract

SiO₂-Al₂O₃, with a mass content of 5%, 10% and 15%, was synthesized by using a Al(NO₃)₃-NaAlO₂ double hydrolysis method, with surfactant Pluronic P₁₂₃ as template and Si(OC₂H₅)₄ as Si source. The Co-Mo/SiO₂-Al₂O₃ hydrotreating catalysts for lubricating oil were then prepared by co-impregnation method and characterized by a series of techniques such as XRD, N₂ sorption, Py-FTIR, NH₃-TPD, H₂-TPR, TEM and XRF. The results show that the SiO₂-Al₂O₃ support containing 10% Si is provided with abundant moderate-strong acid sites and partially ordered mesoporous structure; MoS₂ particles are uniformly dispersed on the SiO₂-Al₂O₃ surface. Moreover, the Co-Mo/10%SiO₂-Al₂O₃ catalyst exhibits high amount of Bronsted acid sites and type Ⅱ CoMoS active phase. The catalytic performance was evaluated in a high-pressure fixed-bed reactor, with second vacuum side distillate oil as the raw material oil. The results show that the Co-Mo/10%SiO₂-Al₂O₃ catalyst exhibits high activity in hydrotreating and paraffins and cycloalkanes are the main components in product oil. Under 380℃, 15 MPa, a space velocity of 0.6 h^-1, and a hydrogen to oil ratio of 1000, the HDS and HDN values over Co-Mo/10%SiO₂-Al₂O₃ exceed 99%. Meanwhile, the contents of S and N in the product are less than 10 and 2 μg/g, respectively, which can meet the requirements on the raw materials for the subsequent isomerization dewaxing process.
- SiO₂-Al₂O₃ support,
- Co-Mo catalyst,
- lubricating oil,
- hydrotreating

FullText(HTML)

References(24)

References

[1]	TAGUCHI A, SCHÜTH F. Ordered mesoporous materials in catalysis[J]. Microporous Mesoporous Mater, 2005, 77(1):1-45. doi: 10.1016/j.micromeso.2004.06.030
[2]	SHYAMAL K B, SAMIR K M, UDAY T T. Search for an efficient 4, 6-DMDBT hydrodesulfurization catalyst:A review of recent studies[J]. Energy Fuels, 2004, 18(5):1227-1237. doi: 10.1021/ef030179+
[3]	王延臻, 张金玲, 宋春敏, 段红玲. Co-Mo/meso-Al₂O₃蜡油加氢处理催化剂的制备[J].石油炼制与化工, 2017, (12):68-73. doi: 10.3969/j.issn.1005-2399.2017.12.014 WANG Yan-zhen, ZHANG Jin-ling, SONG Chun-min, DUAN Hong-ling. Preparation of Co-Mo/meso-Al₂O₃ for vacuum distillate oil hydrotreating[J]. Pet Process Petrochem, 2017, (12):68-73. doi: 10.3969/j.issn.1005-2399.2017.12.014
[4]	岳宝华, 周仁贤, 郑小明. 耐高温高比表面Ce-Zr复合氧化铝的制备及在汽车尾气净化催化剂中的应用研究[C]. 第十三届全国催化学术会议论文集, 2006. YUE Bao-hua, ZHOU Ren-xian, ZHENG Xiao-ming. Preparation and application of Ce-Zr modified alumina with high surface area and high temperature resistance in the automobile emission purification catalyst[C]. 13^th Nationwide Academic Conference Proceedings on Catalysis, 2006.
[5]	金政伟. 弱酸性体系中非离子表面活性剂导向下硅基介孔材料的合成研究[D]. 北京: 北京化工大学, 2007. http://cdmd.cnki.com.cn/Article/CDMD-10010-1014452123.htm JIN Zheng-wei. Synthesis of silica mesoporous materials by using nonionic surfactant as template under mildly acidity conditions[D]. Beijing: Beijing University of Chemical Technology, 2007. http://cdmd.cnki.com.cn/Article/CDMD-10010-1014452123.htm
[6]	SUZUKI N, SAKKA Y, YAMAUCHI Y. Simple preparation of silica and alumina with a hierarchical pore system via the dual-templating method[J]. Sci Technol Adv Mater, 2009, 10(2):1-6. https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5090446
[7]	LI D, LIN Y S, GULIANTS V V. Synthesis and characterization of ordered meso-macro-porous silica membranes on a porous alumina support[J]. Tsinghua Sci Technol, 2010, 15(4):377-384. doi: 10.1016/S1007-0214(10)70076-6
[8]	FU W, ZHANG L, WU D, XIANG M, ZHUO Q, HUANG K, TAO Z, TANG T. Mesoporous zeolite-supported metal sulfide catalysts with high activities in the deep hydrogenation of phenanthrene[J]. J Catal, 2015, 330:423-433. doi: 10.1016/j.jcat.2015.07.026
[9]	LI G C, LIU Y Q, TANG Z, LIU C G. Effects of rehydration of alumina on its structural properties, surface acidity, and HDN activity of quinolone[J] Appl Catal A:Gen, 2012, 437/438:79-89. doi: 10.1016/j.apcata.2012.06.017
[10]	PARRY E P. An infrared study of pyridine adsorbed on acidic solids. Characterization of surface acidity[J]. J Catal, 1963, 2(5):371-379. doi: 10.1016/0021-9517(63)90102-7
[11]	BUSCA G. Spectroscopic characterization of the acid properties of metal oxide catalysts[J]. Catal Today, 1998, 41(1/3):191-206. https://www.sciencedirect.com/science/article/pii/S0920586198000492
[12]	GRZECHOWIAK J R, RYNKOWSKI J, WERESZCZAKO-ZIELINSKA I. Catalytic hydrotreatment on alumina-titania supported NiMo sulphides[J]. Catal Today, 2001, 65(2/4):225-231. https://www.sciencedirect.com/science/article/pii/S0920586100005629
[13]	ARRIBAS M A, CONCEPCIÓN P, MARTÍNEZ A. The role of metal sites during the coupled hydrogenation and ring opening of tetralin on bifunctional Pt(Ir)/USY catalysts[J]. Appl Catal A:Gen, 2004, 267(1/2):111-119. https://www.sciencedirect.com/science/article/pii/S0926860X04001565
[14]	SANTI D, HOLL T, CALEMMA V, WEITKAMP J. High-performance ring-opening catalysts based on iridium-containing zeolite Beta in the hydroconversion of decalin[J]. Appl Catal A:Gen, 2013, 455(2):46-57. https://www.sciencedirect.com/science/article/pii/S0926860X13000471
[15]	GALPERIN L B, BRICKER J C, HOLMGREN J R. Effect of support acid-basic properties on activity and selectivity of Pt catalysts in reaction of methylcyclopentane ring opening[J]. Appl Catal A:Gen, 2003, 239(1/2):297-304. https://www.sciencedirect.com/science/article/pii/S0926860X02004167
[16]	VALENCIA D, KLIMOVA T. Citric acid loading for MoS₂-based catalysts supported on SBA-15. New catalytic materials with high hydrogenolysis ability in hydrodesulfurization[J]. Appl Catal B:Environ, 2013, 129(2):137-145. http://www.doc88.com/p-9813440340424.html
[17]	EJKA J. Organized mesoporous alumina:Synthesis, structure and potential in catalysis[J]. Appl Catal A:Gen, 2003, 254(2):327-338. doi: 10.1016/S0926-860X(03)00478-2
[18]	WANG N, SHEN K, HUANG L, YU X, QIAN W, CHU W. Facile route for synthesizing ordered mesoporous Ni-Ce-Al oxide materials and their catalytic performance for methane dry reforming to hydrogen and syngas[J]. Acs Catal, 2013, 3(3):1638-1651. doi: 10.1021/cs4003113
[19]	SONI K, RANA B S, SINHA A K, BHAUMIK A, NANDI M, KUMAR M, DHAR G M. 3-D ordered mesoporous KIT-6 support for effective hydrodesulfurization catalysts[J]. Appl Catal B:Environ, 2009, 90(1):55-63. https://www.sciencedirect.com/science/article/pii/S092633730900071X
[20]	PARRY E P. An infrared study of pyridine adsorbed on acidic solids. Characterization of surface acidity[J]. J Catal, 1963, 2(5):371-379. doi: 10.1016/0021-9517(63)90102-7
[21]	LIU H, LIU C, YIN C, CHAI Y, LI Y, LIU D, LIU B, LI X, WANG Y, LI X. Preparation of highly active unsupported nickel-zinc-molybdenum catalysts for the hydrodesulfurization of dibenzothiophene[J]. Appl Catal B:Environ, 2015, s174-175:264-276. https://www.sciencedirect.com/science/article/pii/S0926337315000600
[22]	LÓPEZ C R, LÓPEZ A A. Effect of water extraction on the surface properties of Mo/Al₂O₃ and NiMo/Al₂O₃ hydrotreating catalysts[J]. Appl Catal A:Gen, 2000, 202(1):23-28. doi: 10.1016/S0926-860X(00)00449-X
[23]	OKAMOTO Y, ISHIHARA S, KAWANO M. Preparation of Co-Mo/Al₂O₃ model sulfide catalysts for hydrodesulfurization and their application to the study of the effects of catalyst preparation[J]. J Catal, 2003, 217(1):12-22. http://www.doc88.com/p-6911574757666.html
[24]	杨占林, 姜虹, 彭绍忠, 王继锋, 唐兆吉.制备技术对加氢处理催化剂性能的影响[J].石油化工, 2012, 41(8):885-889. http://www.cnki.com.cn/Article/CJFDTOTAL-SYHG201208005.htm YANG Zhan-lin, JIANG Hong, PENG Shao-zhong, WANG Ji-feng, TANG Zhao-ji. Influence of preparation techniques on the structure and activity of hydrogenation catalysts[J]. Petrochem Technol, 2012, 41(8):885-889. http://www.cnki.com.cn/Article/CJFDTOTAL-SYHG201208005.htm