李晓庆,张微,马守涛,所艳华,崔艳红,汪颖军.超声辅助制备Ni-Mo/USY催化剂上正庚烷异构化性能研究[J].分子催化,2018,32(5):434-443
超声辅助制备Ni-Mo/USY催化剂上正庚烷异构化性能研究
Studyof Isomerization Performance of n-Heptane on Ultrasound-Assisted Preparation of Ni-Mo/USY Catalysts
投稿时间:2018-07-13  修订日期:2018-08-25
DOI:
中文关键词:  Ni  Mo  USY分子筛  正庚烷异构化
英文关键词:Ni  Mo  USY molecular sieve  Isomerization of n-heptane
基金项目:东北石油大学"国家基金"培育基金(2017PYYL-03);黑龙江省大学生创新创业训练计划项目(201710220030)
作者单位E-mail
李晓庆 东北石油大学 化学化工学院, 黑龙江 大庆 163318  
张微 东北石油大学 化学化工学院, 黑龙江 大庆 163318  
马守涛 东北石油大学 化学化工学院, 黑龙江 大庆 163318
中国石油大庆化工研究中心, 黑龙江 大庆 163714 
 
所艳华 东北石油大学 化学化工学院, 黑龙江 大庆 163318  
崔艳红 东北石油大学 化学化工学院, 黑龙江 大庆 163318
黑龙江八一农垦大学, 黑龙江 大庆 158308 
 
汪颖军 东北石油大学 化学化工学院, 黑龙江 大庆 163318 wangying-jun@163.com 
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中文摘要:
      以USY分子筛作为载体,Ni和Mo作为活性组分,利用超声辅助浸渍法(US-IM)和常规浸渍法(C-IM)制备了Ni/USY(US-IM)和Ni-Mo/USY催化剂.采用X射线衍射(XRD)、吡啶-红外光谱分析(Py-IR)和N2吸附-脱附等对催化剂进行理化性质表征,综合考察了不同改性方法以及单金属和双金属改性前后分子筛酸性和孔结构性质等的变化及其对正庚烷异构化性能的影响.实验结果表明:Mo对于Ni在USY分子筛上的均匀分布以及异构化催化性能具有协同促进作用;超声条件对双金属改性的USY结构基本无影响;超声空化作用降低了催化剂金属粒子的团聚,使其在USY表面均匀分散,增加了催化反应中所需的金属活性位点.超声辅助浸渍制备的Ni-Mo/USY中较高的金属分散度导致了较强的金属-载体相互作用,使其活性和稳定性高于常规浸渍法.在优化超声条件下,反应温度和反应时间分别为250℃和3 h,还原温度和还原时间分别为550℃和5 h,H2/C7摩尔比为0.14时,正庚烷的转化率和异构化选择性分别可以达到65.7%和74.1%.
英文摘要:
      Ni/USY(US-IM) and Ni-Mo/USY catalysts were prepared by ultrasonic assisted impregnation method (US-IM) and conventional impregnation method (C-IM) using USY molecular sieve as carrier, Ni and Mo as metal active components. The physical and chemical properties of the catalysts were characterized by X-ray diffraction (XRD), pyridine-infrared spectroscopy (Py-IR) and N2 adsorption-desorption methods. In addition, the influences of the changes of acidity and pore structure properties of molecular sieves before and after metal modification on the isomerization performances of n-heptane of the catalyst were investigated comprehensively. The experimental results showed that Mo had a synergistic effect on both the uniform distribution of Ni on USY molecular sieves and the isomerization performances. There were no substantial effects on the structure of USY after bimetallic modification under ultrasonic conditions. Ultrasonic cavitation reduced the agglomeration of the metal particles which led to the uniform dispersion of the metal particles on the USY surface, and thus the metal active sites required in the cataly-tic reaction were increased. The higher metal dispersion in Ni-Mo/USY catalyst prepared by ultrasonic assisted impregnation resulted in stronger metal-support interaction, which made it exhibit higher activity and stability than that of conventional impregnation method. Under the optimized ultrasonic conditions, the conversion and isomerization selectivity of n-heptane reached 65.7% and 74.1%, respectively, when the reaction temperature was 250℃, reaction time was 3 h, reduction temperature was 550℃, reduction time was 5 h, and the molar ratio of H2/C7 was 0.14.
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