催化学报

催化学报 ›› 2011, Vol. 32 ›› Issue (7): 1234-1241.DOI: 10.3724/SP.J.1088.2011.10138

• 研究论文 • 上一篇    下一篇

SAPO-31 分子筛的微波加热合成、表征及催化性能

杨杰 1, 吴伟 1, *, 周亚静 1, 武光 1, 赵爱娟 1, 基赫佳宁 O V2, 托克塔列夫 A V2, 伊切夫斯基 G V2   

  1. 1黑龙江大学化学化工与材料学院, 黑龙江省普通高校高效转化的化工过程与技术重点实验室, 中俄联合催化实验室, 黑龙江哈尔滨 150080; 2俄罗斯科学院西伯利亚分院鲍列斯科夫催化研究院, 新西伯利亚市 630090, 俄罗斯
  • 收稿日期:2011-02-19 修回日期:2011-04-08 出版日期:2011-07-18 发布日期:2014-11-28

Microwave Irradiation Synthesis of SAPO-31 Molecular Sieve and Its Characterization and Catalytic Performance

YANG Jie1, WU Wei1,*, ZHOU Yajing1, WU Guang1, ZHAO Aijuan1, KIKHTYANIN O V2, TOKTAREV A V2, ECHEVSKII G V2   

  1. 1Key Laboratory of Chemical Engineering Process and Technology for High-Efficiency Conversion, College of Heilongjiang Province; Sino-Russan Joint Laboratory for Catalysis, School of Chemistry and Material Sciences, Heilongjiang University, Harbin 150080, Heilongjiang, China; 2Boreskov Institute of Catalysis, Siberian Branch of the Russian Academy of Sciences, Novosibirsk 630090, Russia
  • Received:2011-02-19 Revised:2011-04-08 Online:2011-07-18 Published:2014-11-28

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1041

被引次数

12

摘要： 分别以异丙醇铝和磷酸为铝源和磷源, 二正丁胺为模板剂, 采用微波加热法成功制得 AlPO4-31 分子筛, 并对其晶化条件进行了优化. 在优化的条件下同时合成了不同含硅量的 SAPO-31 分子筛, 采用 X 射线衍射、N2 物理吸附、扫描电镜、固体 29Si 核磁共振、程序升温脱附以及吡啶吸附的红外光谱等手段对其结构和酸性进行了表征, 并考察了 Pd/SAPO-31 双功能催化剂在正癸烷加氢异构化反应中的催化性能. 结果表明, 采用微波加热法在 170 oC 晶化 2 h, 即可合成出具有 ATO 结构的高结晶度的纯相 AlPO4-31 和 SAPO-31 分子筛. 将 Si 引入到 AlPO4-31 骨架中所合成的 SAPO-31 分子筛的比表面积和微孔体积增大, 通过改变初始凝胶中原料组成可调变 SAPO-31 分子筛骨架中硅物种的分布及酸性质. 以酸性适宜的 SAPO-31 分子筛制备的 Pd/SAPO-31 双功能催化剂在正癸烷加氢异构化反应中表现出较高的活性和选择性.

关键词: 微波加热, SAPO-31 分子筛, 二正丁胺, 正癸烷, 加氢异构化

Abstract: AlPO4-31 molecular sieve was synthesized by microwave irradiation using aluminum isopropoxide, orthophosphoric acid, and di-n-butylamine as sources of aluminum, phosphorus, and template, respectively. The crystallization conditions of AlPO4-31 were optimized. SAPO-31 molecular sieve samples with different silicon contents were synthesized at the optimal conditions. The structure and acidity of the samples were characterized by X-ray diffraction, N2 physical adsorption, scanning electron microscopy, 29Si MAS NMR, NH3 temperature-programmed desorption, FT-IR of adsorbed pyridine. The catalytic performance of Pd/SAPO-31 bifunctional catalyst for hydroisomerization of n-decane was investigated. The results indicated that the AlPO4-31 and SAPO-31 molecular sieves with pure crystal phase and higher crystallinity assigned to ATO topology structure were obtained at 170 oC for 2 h by microwave irradiation. The BET surface area and micropore volume were increased because of the introduction of Si to the framework of AlPO4-31. The distribution of Si in the framework and the acidity of the SAPO-31 molecular sieve were varied by changing the composition of the reaction mixture. The bifunctional catalyst Pd/SAPO-31 with suitable acidity showed high activity and selectivity for hydroisomerization of n-decane.

Key words: microwave irradiation, SAPO-31 molecular sieve, di-n-butylamine, decane, hydroisomerization