NiW/Al<sub>2</sub>O<sub>3</sub>-Y催化剂的制备及其对煤焦油加氢处理的研究

张海永; 王永刚; 张培忠; 林雄超; 朱豫飞

NiW/Al₂O₃-Y催化剂的制备及其对煤焦油加氢处理的研究

1.
中国矿业大学(北京) 化学与环境工程学院, 北京 100083;
2.
北京低碳清洁能源研究所, 北京 102209

基金项目: National Natural Science Foundation of China (U1261213) and the National High-Tech R&D Program of China (863 Program, 2011AA05A203).

详细信息

中图分类号: TQ519
计量
- 文章访问数: 1352
- HTML全文浏览量: 18
- PDF下载量: 825
- 被引次数: 0
出版历程
- 收稿日期: 2013-04-27
- 修回日期: 2013-06-18
- 刊出日期: 2013-09-30

Preparation of NiW catalysts with alumina and zeolite Y for hydroprocessing of coal tar

1.
School of Chemical and Environmental Engineering, China University of Mining &Technology (Beijing), Beijing 100083, China;
2.
National Institute of Clean-and-Low-Carbon Energy, Beijing 102209, China

摘要

摘要: 以不同比例的γ-Al₂O₃和Y型分子筛为混合载体制备NiW/Al₂O₃-Y催化剂,采用N₂低温吸附、XRD、H₂-TPR 和 NH₃-TPD对其进行表征,并在固定床上通过甲酚-萘溶液的加氢处理反应对催化剂活性进行评价。结果表明,催化剂均具有良好的加氢脱氧及加氢饱和性能,异构化及裂化产物随分子筛含量的增加而增加,催化剂酸性增加更有利于萘加氢产物中反式十氢萘的生成。以较佳催化剂对低温煤焦油馏分进行加氢处理,采用GC-MS和元素分析等对油品进行分析。原料中绝大部分酚类化合物及双环芳烃转化为茚、环烷烃和氢化芳烃等化合物,同时明显降低了杂原子尤其是硫和氧的含量。
- 低温煤焦油 /
- 加氢处理 /
- 催化剂 /
- 分子筛
Abstract: γ-alumina supported Ni-W catalysts with different zeolite Y contents were prepared and characterized by N₂ sorption, XRD, H₂-TPR and NH₃-TPD. Their catalytic activities were investigated on a trickle bed reactor by hydroprocessing cresol-naphthalene model compounds in n-heptane solution. The results show that all the catalysts exhibit excellent hydrodeoxygenation and hydrogenation activities, while the isomerization and ring-opening products increase with the addition of zeolite, and trans-decalin is preferred with acid sites. A better catalyst was selected for hydroprocessing a low temperature coal tar fraction and the product oil was analyzed by GC-MS and elementary analysis. Phenols and di-aromatics in the tar are almost converted into indans, cycloalkanes and hydro-aromatics. In the meantime, heteroatoms, especially S and O atoms, reduce remarkably.
- low temperature coal tar /
- hydroprocessing /
- catalyst /
- zeolite

HTML全文

参考文献(18)

SAYAN S, PAUL J. Hydrogenation of naphthalene and methylnaphthalene: modeling and spectroscopy[J]. J Mol Catal A: Chem, 2002, 185(1/2): 211-222.

FURIMSKY E. Catalytic hydrodeoxygenation[J]. Appl Catal A: Gen, 2000, 199(2): 147-190.

RAM REZ J, RAYO P, GUTI RREZ-ALEJANDRE A, ANCHEYTA J, RANA M S. Analysis of the hydrotreatment of Maya heavy crude with NiMo catalysts supported on TiO₂-Al₂O₃ binary oxides: Effect of the incorporation method of Ti[J]. Catal Today, 2005, 109(1/4): 54-60.

WANG L, SHEN B, FANG F, WANG F, TIAN R, ZHANG Z, CUI L. Upgrading of light cycle oil via coupled hydrogenation and ring-opening over NiW/Al₂O₃-USY catalysts[J]. Catal Today, 2010, 158(3/4): 343-347.

ARRIBAS M A,MARTNEZ A. The influence of zeolite acidity for the coupled hydrogenation and ring opening of 1-methylnaphthalene on Pt/USY catalysts[J]. Appl Catal A: Gen, 2002, 230(1/2): 203-217.

LEITE L, BENAZZI E, MARCHAL-GEORGE N. Hydrocracking of phenanthrene over bifunctional Pt catalysts[J]. Catal Today, 2001, 65(2/4): 241-247.

HASSAN A, AHMED S, ALI M A, HAMID H, INUI T. A comparison between - and USY-zeolite-based hydrocracking catalysts[J]. Appl Catal A: Gen, 2001, 220(1/2): 59-68.

GALLEZOT P. The state and catalytic properties of platinum and palladium in faujasite-type zeolites[J]. Cat Re-Sci Eng, 1979, 20(1): 121-154.

ZHENG J, GUO M, SONG C. Characterization of Pd catalysts supported on USY zeolites with different SiO₂/Al₂O₃ ratios for the hydrogenation of naphthalene in the presence of benzothiophene[J]. Fuel Process Technol, 2008, 89(4): 467-474.

YASUDA H, SATO T, YOSHIMURA Y. Influence of the acidity of USY zeolite on the sulfur tolerance of Pd-Pt catalysts for aromatic hydrogenation[J]. Catal Today, 1999, 50(1): 63-71.

INAMURA K,IINO A. Development of zeolite hydrocracking catalyst and system for resid hydrodesulfurization unit[J]. Catal Today, 2011, 164(1): 204-208.

BREYSSE M, CATTENOT M, KOUGIONAS V, LAVALLEY J C, MAUGE F, PORTEFAIX J L, ZOTIN J L. Hydrogenation properties of ruthenium sulfide clusters in acidic zeolites[J]. J Catal, 1997, 168(2): 143-153.

SIMON L J, VAN OMMEN J G, JENTYS A, LERCHER J A. Sulfur-tolerant Pt-supported zeolite catalysts for benzene hydrogenation: I. Influence of the support[J]. J Catal, 2001, 201(1): 60-69.

WANDAS R, SURYGALA J, SLIWKA E. Conversion of cresols and naphthalene in the hydroprocessing of three-component model mixtures simulating fast pyrolysis tars[J]. Fuel, 1996, 75(6): 687-694.

MOREAU C, AUBERT C, DURAND R, ZMIMITA N, GENESTE P. Structure-activity relationships in hydroprocessing of aromatic and heteroaromatic model compounds over sulphided NiO-MoO₃/γ-Al₂O₃ and NiO-WO₃/ γ -Al₂O₃ catalysts; chemical evidence for the existence of two types of catalytic sites[J]. Catal Today, 1988, 4(1): 117-131.

MOREAU C, JOFFRE J, SAENZ C, GENESTE P. Hydroprocessing of substituted benzenes over a sulfided CoO-MoO₃/γ-Al₂O₃catalyst[J]. J Catal, 1990, 122(2): 448-451.

SONG C, ESER S, SCHOBERT H H, HATCHER P G. Pyrolytic degradation studies of a coal-derived and a petroleum-derived aviation jet fuel[J]. Energy Fuels, 1993, 7(2): 234-243.

SCHMITZ A D, BOWERS G, SONG C. Shape-selective hydrogenation of naphthalene over zeolite-supported Pt and Pd catalysts[J]. Catal Today, 1996, 31(1/2): 45-56. NiW/Al₂O₃-Y催化剂的制备及其对煤焦油加氢处理的研究

施引文献

资源附件(0)

访问统计