摘要
在氢分压4.0 MPa、523~723 K硫化温度范围内,考察了硫化温度对含和不含柠檬酸的NiW/Al2 O3催化剂的4,6-二甲基二苯并噻吩(4,6-DMDBT)加氢脱硫活性的影响,并采用X射线光电子能谱(XPS)和高分辨透射电镜(HRTEM)对硫化态催化剂进行了表征.结果表明,含柠檬酸的NiW/Al2O3催化剂的加氢脱硫活性随硫化温度的变化规律与无柠檬酸催化剂相似,脱硫活性均在673 K时达到最高值,并且前者的脱硫活性明显高于后者.随着硫化温度的升高,催化剂中W物种的硫化度快速上升,WS2微晶数量增多,尺寸增大;当硫化温度高于623 K后,W物种硫化度增幅变小.催化剂脱硫活性与W物种硫化度存在较高的关联度.
NiW/Al2O3catalysts with and without citric acid were sulfided at H2 pressure of 4.0 MPa and temperature from 523 K to 723 K. The effects of sulfuration temperature on the catalytic activity of these NiW/Al2O3 catalysts in 4,6-DMDBT hydrodesulfurization (HDS) reaction were investigated. These sulfided catalysts were characterized by means of XPS and HRTEM techniques. The results showed that the HDS activity of citric acid containing NiW/Al2O3(NiWCA)displayed a similar variation trend to that of NiW/Al2O3without citric acid (NiW) with the increase of sulfuration temperature, and reached its highest value at the sulfuration temperature around 673 K. Moreover, it was observed that the catalyst with citric acid exhibited significantly higher HDS activity than the catalyst without citric acid. When the sulfuration temperature increased, sulfuration degree of W species in catalyst was speeded and more WS2 crystallites were formed with larger sizes. At sulfuration temperatures above 623 K, the increment of W sulfuration degree became smaller. A good correlation was found between the catalyst HDS activity and W sulfuration degree.
出处
《石油学报(石油加工)》
EI
CAS
CSCD
北大核心
2014年第1期7-14,共8页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家重点基础研究发展计划"973"项目(2012CB224802)资助
关键词
NIW
AL2O3
柠檬酸
硫化温度
加氢脱硫活性
NiW/Al2O3
citric acid
sulfuration temperature
hydrodesulfurization activity