摘要
在空气气氛中由钼酸铵和LaHY分子筛固相反应制备了MoO3-LaHY催化剂,用XRD和NH3-TPD对其进行了表征,并以二苯并噻吩/正癸烷溶液为模型反应物(二苯并噻吩的质量分数为0.6%),评价了MoO3-LaHY的加氢脱硫催化性能。结果表明,在520℃下进行固相反应制备催化剂时,4.36%的Mo物种可借助固相反应进入到分子筛的体相形成单相复合体nMoOx.LaHY,剩余的Mo物种仍以MoO3的形式分散在分子筛外表面。由于单相复合体的形成,催化剂的晶胞参数增大,酸量有所下降。硫化处理后得到的硫化态MoO3-LaHY催化剂在310℃、4.0MPa、反应空速为20h-1的条件下进行加氢脱硫时,二苯并噻吩转化率达到了86.74%。随固相反应温度的升高,所制备的催化剂中Mo物种进入LaHY体相中的量有所增大,但其硫化态催化剂的二苯并噻吩加氢脱硫活性的变化幅度并不大。
MoOx-LaHY catalysts were prepared with the mixture of(NH4)6Mo7O24·4H2O and LaHY through solid-state reaction under air atmosphere and characterized by XRD and NH3-TPD techniques;their hydrodesulfurization(HDS) performance was evaluated by using the solution of dibenzothiophene(DBT,0.6% by mass) in decane as a model reactant.The results indicated that by using solid-state reaction at 520℃,4.36% of Mo species is incorporated into the molecular sieve LaHY,which forms the single-phase complex nMoOx·LaHY,while the rest Mo species is dispersed on the outer surface of LaHY.As a result of forming the single-phase complex,the lattice parameters of MoOx-LaHY catalysts are enlarged and their acidity is reduced.Over the sulfided MoOx-LaHY catalysts,the conversion of DBT reaches 86.74% for the HDS under the conditions of 310℃,4.0MPa and a space velocity 20h-1.Raising the solid-state reaction temperature may increase the content of the single-phase complex incorporated in the resultant MoOx-LaHY catalysts,but it cannot significantly enhance their HDS activity.
出处
《燃料化学学报》
EI
CAS
CSCD
北大核心
2011年第7期538-542,共5页
Journal of Fuel Chemistry and Technology
基金
中国石油科技创新基金(2009D-5006-04-03)
关键词
固相反应
单相复合体
表征
二苯并噻吩
加氢脱硫
solid-state reaction
single-phase complex
characterization
dibenzothiophene
hydrodesulfurization