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作 者:宋华[1,2] 孙恩浩[1] 李锋[2] 宋华林[3] 石洋[1]
机构地区:[1]东北石油大学化学化工学院,黑龙江大庆163318 [2]东北石油大学石油与天然气化工黑龙江省重点实验室,黑龙江大庆163318 [3]牡丹江医学院黑龙江省高校肿瘤疾病防治重点实验室,黑龙江牡丹江157011
出 处:《燃料化学学报》2013年第6期715-721,共7页Journal of Fuel Chemistry and Technology
基 金:中国石油天然气股份有限公司科技风险创新研究(07-06D-01-04-03-02)
摘 要:过微乳液法负载Pt制备了Pt-S2O28-/ZrO2-Al2O3(Pt-SZA-X)催化剂,并采用XRD、BET、FT-IR、TPR、TEM等手段对催化剂进行了表征。以正戊烷异构化反应为探针,考察了焙烧温度对催化剂异构化性能的影响。结果表明,焙烧温度对Pt-SZA-X的还原温度影响不大,但催化剂表面S含量随着焙烧温度的升高而下降;焙烧温度为600~650℃时形成O=S=O结构,此时S与催化剂载体结合比较稳定;焙烧温度为650℃时,可得到单一的ZrO2四方晶相,焙烧温度高于650℃时,比表面积迅速降低,催化剂表面S6+流失严重。在不同温度下焙烧得到的催化剂中,经650℃焙烧的催化剂具有适宜的超强酸位和比表面积,异构化活性最高。在反应温度为230℃、反应压力2.0 MPa、氢烃物质的量比4∶1、质量空速1.0 h-1时,催化异戊烷产率达到60.8%。Pt-S2O8^2-/ZrO2-Al2O3(Pt-SZA-X) solid superacid catalysts were prepared by microemulsion method and characterized by XRD,BET,FT-IR,TPR and TEM.The effects of calcination temperatures on the isomerization performance were studied by using n-pentane isomerization as a probe reaction.It was found that the calcination temperature has less influence on the reduction temperature of the Pt-SZA-X,but the S content over catalyst decreased with increasing calcination temperature.The O=S=O structure formed at calcination temperature range of 600 to 650℃ and the combination between of S and catalyst support was relatively stable.The pure monoclinic phase of ZrO2 were observed with sample calcined at 650℃.When the calcination temperature is higher than 650℃,the specific surface area decreases rapidly and the loss of S^6+ on the surface of catalyst is seriously.Among the catalysts obtained at various calcination temperatures,the catalyst calcined at 650℃ has appropriate amount of superacid sites and surface area and the highest isomerization activity.At reaction temperature of 230℃,pressure of 2.0MPa,hydrogen/hydrocarbon molar ratio of 4∶1 and mass hourly space velocity of 1.0h^-1,the isopentane yield is 60.8%.
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