钼基改性催化剂的制备及其催化氧化脱硫性能研究  

PREPARATION AND MODIFICATION OF Mo-BASED CATALYST AND ITS CATALYTIC OXIDATIVE DESULFURIZATION PERFORMANCE

作　　者：刘静[1] 刘东[1] 杜辉[1] 宋林花[1] 

机构地区：[1]中国石油大学(华东)重质油国家重点实验室,山东青岛266580

出　　处：《石油炼制与化工》2016年第3期42-47,共6页Petroleum Processing and Petrochemicals

基　　金：国家自然科学基金资助项目(21176259);山东省自然科学基金资助项目(ZR2015BM003);中央高校基本科研业务费专项资金资助项目(15CX05009A)

摘　　要：采用溶胶-凝胶法合成了氧化硅,考察了硅源浓度、模板剂用量及陈化时间对氧化硅介孔结构的影响。以氧化硅为载体,采用等体积浸渍法制备了钼基负载型催化剂,并加入柠檬酸、硝酸镧、硝酸铈对其进行改性。在温和条件下,以双氧水为氧化剂,考察了不同改性催化剂对减压馏分油(VGO)的催化氧化脱硫性能,并优化了催化氧化脱硫条件。结果表明:氧化硅的最佳合成条件为硅源浓度0.68 mol/L、CTAB/TEOS摩尔比11∶50、陈化时间2h;催化剂脱硫活性由大到小的顺序为Ce-MoO_3/SiO_2>CA-MoO_3/SiO_2>MoO_3/SiO_2>La-MoO_3/SiO_2;以Ce-MoO_3/SiO_2为催化剂时,最佳催化氧化脱硫条件为氧化温度70℃、O/S摩尔比8、氧化时间2h、催化剂加入量(w)15%,此条件下VGO脱硫率达到64.8%。SiO2 support was synthesized through sol-gel method and the effect of concentration of silica source, dosage of template, and the period of aging on the pore structure and oxidative desulfurization were investigated. The supported Mo-catalysts were prepared by incipient impregnation method using ammonium molybdate solution with citric acid （CA）, Ce（NO3）3· 6H2O, and La（NO3 ）3 · 6H2O, respectively. The catalytic oxidative desulfurization for VGO was conducted to evaluate the performance of the prepared catalysts using H2O5 as oxidant. Based on the evaluation results, the optimized reaction conditions were determined. The results indicate that the best synthesis conditions of SiO2 support are concentration of silica source of 0.68 mol/L, [CTAB]/[TEOS] of 11 ： 50 and aging time of 2 h; The order of desulfurization performance is Ce-MoO3/SiO2 〉 CA-MoO3/SiO2 〉 MoO3/SiO2 〉 La-MoO3/SiO2 ; The desulfurization rate of VGO is 64.8% with Ce-MoO3/SiO2 catalyst at the optimal reaction condi- tions： temperature of 70 ℃, reaction time of 2 h, O/S mole ratio of 8, the dosage of catalyst of 15%.

关 键 词：钼 氧化硅 改性 氧化脱硫 减压馏分油 

分 类 号：TE624.55[石油与天然气工程—油气加工工程]