摘要
采用水热一步合成法制备了SBA-15和Ti-SBA-15分子筛,采用等体积浸渍法和H_2原位还原法制备了Ni_2P/SBA-15和Ni_2P/Ti-SBA-15催化剂。采用X射线衍射(XRD)、N_2吸附脱附(BET)、透射电镜(TEM)、能量色散X射线光谱(EDX)等技术,研究了掺杂Ti原子对SBA-15分子筛及其催化剂形貌和织构性质的影响,并以喹啉为模型化合物,采用微型固定床反应器考察了不同硅/钛摩尔比对催化剂加氢脱氮(HDN)性能的影响。结果表明,Ti的掺杂并没有改变SBA-15高度有序的介孔结构,但改性后载体比表面积略有增大,孔径有所降低;Ni_2P/Ti-SBA-15中Ti以锐钛矿TiO_2和Ti_9O_(17)形式存在,而活性组分还原后所形成的物相为Ni_2P。Ni_2P/Ti-SBA-15催化剂的HDN活性均高于Ni_2P/SBA-15催化剂,并且不同硅/钛摩尔比的催化剂呈现不同的HDN活性,n(Si)/n(Ti)=25的Ni_2P/Ti-SBA-15催化剂具有最高的HDN活性。
The Ti-SBA-15 and SBA-15 support were synthesized by hydrothermal synthesis method, and Ni2P/SBA-15 and Ni2P/Ti-SBA-15 catalysts were prepared by incipient wetness impregnation and in-situ H2 reduction method. The prepared samples were characterized by N2 adsorption- desorption, X-ray diffraction（XRD）, temperature-programmed desorption of ammonia（NH3-TPD）, Energy dispersive X-ray spectrum（EDX） and TEM to investigate the effects of Ti doping on the properties of morphology and texture of the prepared supports and catalysts, and their hydrodenitrogenation（HDN） performances were evaluated in a continuous-flow fixed-bed reactor by using quinoline as the model compound. The results showed that the Ti doping did not change the highly ordered mesoporous structure of SBA-15, after modification the surface area increased slightly, but the pore radius decreased. The Ti existed in the form of TiO2 and Ti9 O17 and the phase of active component after reduction was Ni2P in NizP/Ti-SBA-15 catalyst. The HDN activity of Ni2P/Ti-SBA-15 catalysts was higher than that of Ni2P/SBA-15 catalyst, and Ni2P/Ti-SBA-15 with different n（Si）/n（Ti） presented different HDN activity, among which the Ni2P/Ti-SBA-15 withn（Si）/n（Ti） of 25 was the best one.
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2015年第6期1281-1287,共7页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
辽宁省教育厅科学研究一般项目(L2014507)资助
关键词
SBA-15
TIO2
磷化镍
喹啉
加氢脱氮
SBA-15
titanium dioxide
nickel phosphide
quinoline
hydrodenitrogenation
作者简介
通讯联系人：王海彦，男，教授，博士，从事清洁燃料生产新工艺；E—mail：fswhy@126．com
