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喷雾成型TS-1分子筛催化剂的制备及其性能
引用本文:刘国清,夏 珺,袁 霞,吴 剑.喷雾成型TS-1分子筛催化剂的制备及其性能[J].石油学报(石油加工),2015,31(1):126-131.
作者姓名:刘国清  夏 珺  袁 霞  吴 剑
作者单位:1. 湖南科技大学 化学化工学院 理论有机化学与功能分子教育部重点实验室,湖南 湘潭,411201;2. 湘潭大学 化工学院,湖南 湘潭,411105
基金项目:国家自然科学基金项目(21376201)、湖南省教育厅项目(13C301)、湖南科技大学博士启动基金项目(E51262)和湖南省科技计划项目(2011GK3026)资助
摘    要:制备了喷雾成型TS-1分子筛催化剂,并采用FT-IR、XRD、N2物理吸附、SEM等手段对其进行了表征,考察了SiO2 质量分数、焙烧温度、焙烧时间、焙烧气氛等工艺条件对其催化环己酮氨肟化反应活性的影响。结果表明,与TS-1原粉相比,喷雾成型TS-1分子筛催化剂的骨架保留了MFI的拓扑结构,其比表面积及微孔孔体积有所降低,颗粒粒径明显增大;适宜的制备条件为焙烧温度800℃、焙烧时间4 h、焙烧气氛O2、SiO2质量分数6%,此条件下制得的成型TS-1分子筛催化环己酮氨肟化反应的环己酮转化率及环己酮肟选择性均可达99%。该成型催化剂较TS-1原粉在分离方面有明显的优势。

关 键 词:TS-1  喷雾成型  氨肟化  焙烧  
收稿时间:2013-11-29

Preparation and Characterization of Spray Forming Titanium Silicate-1 Molecular Sieve Catalyst
LIU Guoqing,XIA Jun,YUAN Xia,WU Jian.Preparation and Characterization of Spray Forming Titanium Silicate-1 Molecular Sieve Catalyst[J].Acta Petrolei Sinica (Petroleum Processing Section),2015,31(1):126-131.
Authors:LIU Guoqing  XIA Jun  YUAN Xia  WU Jian
Affiliation:1. Key Laboratory of Theoretical Organic Chemistry and Function Molecule, Ministry of Education, School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, China;2. School of Chemical Engineering, Xiangtan University, Xiangtan 411105, China
Abstract:Formed TS-1 catalyst was prepared by spray with TS-1 powder as raw material and characterized by FT-IR, XRD, low temperature N2 adsorption and SEM. The effects of calcination temperature, calcination atmosphere,calcination time and the mass fraction of SiO2 on the catalytic performance of formed catalyst cyclohexanone ammoximation were investigated. The results showed that the MFI framework structure was well kept with slightly declining surface area and micropore volume but significantly increased particle size after spray forming. With the formed TS-1 as catalyst prepared under the conditions of 6% SiO2 mass fraction, calcined at 800℃ for 4 h in the atmosphere of O2, the cyclohexanone conversion and selectivity to oxime of cyclohexanone ammoximation were all above 99%. Compared to TS-1 powder, the separation of formed TS-1 catalyst from reaction system was more convenient.
Keywords:TS-1  spray forming  ammoximation  calcination
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