|
制备条件对MoNiFe/Al2O3催化剂性质和性能的影响
|
Abstract:
本文采用一步浸渍法和两步浸渍法制备了三种MoNiFe/Al2O3催化剂。通过XRD、Raman、H2-TPR、NH3-TPD、CO吸附原位红外和吡啶吸附红外技术对催化剂的结构和性质进行了表征。以减压渣油为反应物,考察了制备条件对催化剂性能的影响。采用MoNiFe有机酸浸渍液一步浸渍法制备的催化剂MoNiFe/Al2O3具有较高的加氢脱硫、加氢脱残炭和加氢脱金属活性,明显优于采用两步浸渍法制备的MoNiFe/Al2O3催化剂。
Three MoNiFe/Al2O3 catalysts were prepared by one-step and two-step impregnation methods in this paper. The structure and property of the catalysts were characterized by XRD, Raman, H2-TPR, FT-IR of pyridine adsorption, NH3-TPD and FT-IR of CO absorbed. The effect of preparation conditions on the catalytic performance of MoNiFe/Al2O3 catalysts was investigated with vacuum residue as reactant. The MoNiFe/Al2O3 catalyst prepared by one-step impregnation method with MoNiFe organic acid solution exhibited higher hydrodesulfurization activity, residual carbon removing activity and hydrodemetallization activity, whose activity was significantly superior to that of the MoNiFe/Al2O3 catalyst prepared by two-step impregnation method.
[1] | Schweitze, J.-M. and Kressmann, S. (2004) Ebullated Bed Reactor Modeling for Residue Conversion. Chemical Engineering Science, 59, 5637-5645. https://doi.org/10.1016/j.ces.2004.08.018 |
[2] | Rana, M.S., Sámano, V., Ancheyta, J. and Diaz, J.A.I. (2007) A Review of Recent Advances on Process Technologies for Upgrading of Heavy Oils and Residua. Fuel, 86, 1216-1231. https://doi.org/10.1016/j.fuel.2006.08.004 |
[3] | 姚国欣. 渣油沸腾床加氢裂化技术在超重原油改质厂的应用[J]. 当代石油石化, 2008, 16(1): 23-29, 43. |
[4] | 方向晨. 国内外渣油加氢处理技术发展现状及分析[J]. 化工进展, 2011, 30(1): 95-104. |
[5] | 李大东. 加氢处理工艺与工程[M]. 北京: 中国石化出版社, 2004. |
[6] | 方向晨. 加氢精制[M]. 北京: 中国石化出版社, 2006. |
[7] | Hubaut, R., Rives, A., Luis, M. and Scott, C. (2003) Surface Characterization of Bulk Fe-Mo Mixed Sulphide Catalysts. Catalysis Communications, 4, 134-139. https://doi.org/10.1016/S1566-7367(03)00005-0 |
[8] | 吕振辉, 彭绍忠, 张学辉, 高玉兰, 佟佳. 不同官能团有机物对MoNiP/Al2O3催化剂的组成、结构和性能的影响[J]. 石油化工, 2017, 46(1): 27-35. |
[9] | 许灵瑞, 王继锋, 杨占林, 唐兆吉, 姜虹. 载体焙烧温度对MoNiP/γ-Al2O3加氢催化剂活性的影响[J]. 石油化工, 2014, 43(8): 908-913. |
[10] | Vakrosa, J., Lycourghiotisa, A., Voyiatzisb, G.A., Siokoub, A. and Kordulis, C. (2010) Co-Mo/Al2O3-SiO2 Catalysts Prepared by Co-Equilibrium Deposition Filtration: Characterization and Catalytic Behavior for the Hydrodesulphurization of Thiophene. Applied Catalysis B: Environmental, 96, 496-507. https://doi.org/10.1016/j.apcatb.2010.03.011 |
[11] | 赵国利, 王少军, 凌凤香, 吴洪新, 崔晓莉, 张玉涵. 磷对CoMoP浸渍液及催化剂活性组分结构影响的激光拉曼光谱法研究[J]. 分析测试学报, 2012, 31(10): 1298-1302. |
[12] | 徐斌, 朱崇业, 李全芝. 相镍负载催化剂表面组份及其活性的研究[J]. 物理化学学报, 1994, 10(6): 543-548. |
[13] | López Cordero, R. and López Agudo, A. (2000) Effect of Water Extraction on the Surface Properties of Mo/Al2O3 and NiMo/Al2O3 Hydrotreating Catalysts. Applied Catalysis A: General, 202, 23-35.
https://doi.org/10.1016/S0926-860X(00)00449-X |
[14] | Qu, L., Zhang, W., Kooyman, P.J. and Prins, R. (2003) MAS NMR, TPR and TEM Studies of the Interaction of NiMo with Alumina and Silica-Alumina Supports. Journal of Catalysis, 215, 7-13.
https://doi.org/10.1016/S0021-9517(02)00181-1 |
[15] | Hadjiivanov, K.I. and Vayssilov, G.N. (2002) Oxide Surfaces and Zeolites by Carbon Monoxide as an IR Probe Molecule. Advances in Catalysis, 47, 307-511. https://doi.org/10.1016/S0360-0564(02)47008-3 |