【作者】 刘猛；

【导师】 刘晨光； 张孔远；

【作者基本信息】 中国石油大学 ， 化学工程与技术， 2010， 硕士

【摘要】 采用BET、XRD、NH3-TPD、FT-IR和强度测定仪等分析表征方法,考察了硫酸铝法YT-01、YT-02和YT-03及碳化法WL-01氢氧化铝干胶及配比对载体物理性质的影响,确定了制备蜡油加氢处理催化剂载体的氢氧化铝原料为硫酸铝法干胶与碳化法干胶,配料比例为1:1。考察了活性炭及羧甲基纤维素对载体物理性质的影响,选用羧基纤维素为载体的扩孔剂,优化出了羧甲基纤维素的最佳用量。选用YT-01和YT-03硫酸铝法氢氧化铝干胶与WL-01碳化法氢氧化铝干胶为原料,采用等体积浸渍法制备Ni-Mo-W/γ-Al2O3混合蜡油加氢处理催化剂。XRD分析结果表明两种催化剂具有γ-Al2O3晶相,催化剂表面没有其他晶相物种,活性金属在载体上分散均匀。FT-IR和NH3-TPD分析结果表明催化剂表面同时存在B酸、L酸中心,其中B酸中心较弱,L酸中心以中强酸为主。以中国石化青岛炼油化工有限责任公司蜡油加氢处理装置进料为原料,在100mL固定床小型加氢装置上对所制备的两种催化剂进行了蜡油加氢处理工艺条件考察,结果表明:反应温度的升高有利于提高C01、C02催化剂加氢处理活性,脱硫率、脱氮率均随反应温度的升高而相应增加。增加空速,C01、C02催化剂脱硫率、脱氮率降低。氢油比对C01、C02催化剂的反应活性影响较小。在10MPa,370℃,空速1.5 h-1,氢油比700:1的条件下,C01、C02催化剂的脱硫率均为90%左右,脱氮率均为75%左右,残炭脱除率在90%以上。C01催化剂的脱硫、脱氮活性略优于C02催化剂。在同样反应条件下将C01、C02催化剂与国内某工业催化剂C03进行了对比评价,结果表明,所研制的C01、C02催化剂脱硫活性优于C03催化剂,脱氮活性差于参比剂。更多还原

【Abstract】 The YT-01, YT-02 and YT-03 made by Al2(SO4)3 method and WL-01 made by carbonization method and the influence of mix ratio of aluminums on the properties of carrier was investigated by BET, XRD, NH3-TPD, FT-IR and manometry. Hydrotreating carrier prepared by aluminums of Al2(SO4)3 method and carbonization method and the best ingredient ratio was 1:1. The influence of activated carbon and CMC on the physical properties of carriers was investigated. CMC was chosen as the expanding agent and the best amount of CMC was decided.YT-01 and YT-03 with WL-01 was used as raw materials, Ni-Mo-W/γ-Al2O3 catalysts for mix wax oils hydrotreating was prepared by impregnation method. XRD analysis results showed that the catalyst wasγ-Al2O3 phase, without other crystalline species and active metal well dispersed on the carrier. FT-IR and NH3-TPD results showed that the catalyst surface existed Bronsted acid and Lewis acid, while the amount of Bronsted acid was weaker, and Lewis acid centers was mainly strong acid.The feed raw materials was from Chinese Sinopec Qingdao Refining & Chemical gas oil hydrotreating unit, and the catalysts were evaluated on small-scale fixed bed hydrogenation 100mL unit. Results showed that: increasing reaction temperature can improve C01, C02 catalyst performance, and the rate of desulfurization and denitrification increased with reaction temperature. The desulfurization and denitrification rate decreased while increasing LHSV. Hydrogen oil ratio had little effects on the reactivity of the C01 and C02 catalysts. At 10MPa, 370℃, space velocity of 1.5 h-1, hydrogen to oil ratio 700:1, C01 and C02 catalysts desulfurization rate was 90%, nitrogen removal rate was 75%, and residual carbon removal rate was more than 90%. Desulfurization and denitrification activity of C01 catalyst was slightly better than that of the C02 catalyst. C01, C02 catalyst and industrial catalysts C03 were compared under the same conditions. The results showed that desulfurization activity of the C01 and C02 catalyst was better than that of C03, while denitrification activity of C01 and C02 was weaker than the reference dose.更多还原