乙二醇对磷掺杂NiMo/Al2O3加氢催化剂性能的影响  

Effect of ethylene glycol on the hydrogenation performance of P-doped NiMo/Al2O3 catalysts

作　　者：尹海亮[1] 刘新亮[1] 周同娜 赵健[1] 蔺爱国[1] YIN Hai-liang;LIU Xin-liang;ZHOU Tong-na;ZHAO Jian;LIN Ai-guo(Academy of Science&Technology,China University of Petroleum(East China),Dongying 257061,China;Environmental Protection Agency of Dongying,Dongying 257091,China)

机构地区：[1]中国石油大学(华东)科学技术研究院,山东东营257061 [2]东营市生态环境局,山东东营257091

出　　处：《燃料化学学报》2019年第12期1458-1467,共10页Journal of Fuel Chemistry and Technology

基　　金：国家自然科学基金(21206197);山东省自然科学基金(ZR2019MB022);中央高校基本科研业务费专项资金(19CX02063A)资助~~

摘　　要：采用水热合成法,在合成过程中通过添加矿化剂、尿素和改变硅源,制备了不同骨架铝落位的ZSM-5分子筛。通过SEM、XRD、BET、XRF、MAS NMR、NH3-TPD和Py-FTIR等表征手段对分子筛的形貌、织构、骨架铝落位和酸性进行了系统研究,同时考察了不同ZSM-5分子筛催化剂甲醇制芳烃的催化性能。研究结果表明,制备的ZSM-5分子筛均具有结晶度高和形貌均一等特点,但在骨架铝落位和酸性方面存在显著差异。椭球状ZSM-5分子筛的骨架铝主要分布于直通孔道或正弦孔道中,并表现出较多的酸性位。块状分子筛中骨架铝主要落位在孔道交叉处,且具有较低的强酸量。在甲醇制芳烃反应中,骨架铝主要位于直通或正弦孔道并表现出较多酸性位的椭球状ZSM-5分子筛催化剂具有较高的活性稳定性和芳烃选择性。NiMoP(x)/Al2O3 catalysts with different ethylene glycol(EG) contents were prepared by impregnating NiMoP solution containing EG into Al2O3. The hydrodesulfurization(HDS) and hydrodenitrogenation(HDN) performances of the catalysts were evaluated using dibenzothiophene(DBT) and quinoline(Q) as the model compounds. The results showed that the HDS and HDN performances of the catalysts could be improved by adding of EG when the amount of EG was low(nEG/nNi ratio value was 0, 0.5, 1, 2, 3, respectively), and the improvement of HDN performance was more obvious than HDS performance. With the increase of EG content, the activity of HDS and HDN of the catalysts was further improved. TEM and XPS analysis showed that EG was helpful to increase the stacking layer number and lamellar length of MoS2 particles in the catalysts, and with the increase of EG content, the stacking layer number and lamellar length of MoS2 particles increased. EG could improve the surface atomic concentration of Mo, but practically had no influence on the surface atomic distribution of Ni. However, EG significantly increased the sulfuration degree of Mo and Ni. TG characterization showed that EG interacted with alumina and metal active components in various ways, and there were high temperature resistant organic species interacting with active components.

关 键 词：乙二醇 催化剂 加氢脱硫 加氢脱氮 

分 类 号：O643.36[理学—物理化学]