催化学报 ›› 2010, Vol. 31 ›› Issue (8): 1083-1089.DOI: 10.3724/SP.J.1088.2010.00701

• 研究论文 • 上一篇    

有机胺在离子热合成 LTA 型磷酸铝分子筛中的助模板作用

裴仁彦1,2, 徐云鹏1, 魏莹1,2, 温国栋1,2, 李科达1,2, 王磊1, 马怀军1, 田志坚1,3, 林励吾3   

  1. 1 中国科学院大连化学物理研究所清洁能源国家实验室, 辽宁大连 116023 2 中国科学院研究生院, 北京 100049 3 中国科学院大连化学物理研究所催化基础国家重点实验室, 辽宁大连 116023
  • 收稿日期:2010-07-01 出版日期:2010-08-30 发布日期:2013-12-26
  • 通讯作者: 裴仁彦
  • 基金资助:

    国家自然科学基金

The Cooperative Templating Effect of Organic Amine in the Ionothermal Synthesis of LTA Type Aluminophosphate Molecular Sieves

PEI Renyan1,2, XU Yunpeng1,2, WEI Ying1,2, WEN Guodong 1,2, LI Keda1,2, WANG Lei1, MA Huaijun1, TIAN Zhijian1,3,*, LIN Liwu3   

  1. 1Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China 2Graduate University of Chinese Academy of Sciences, Beijing 100049, China 3State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
  • Received:2010-07-01 Online:2010-08-30 Published:2013-12-26

摘要: 在 1-丁基-3-甲基溴化咪唑 ([bmim]Br) 离子液体中引入有机胺合成了 LTA 型磷酸铝分子筛 (AlPO4-42), 采用热重分析、核磁共振光谱、红外光谱以及荧光光谱对所得晶化产物进行了表征, 并考察了体系的晶化动力学. 结果表明, 有机胺以特定的聚集形态协同离子液体阳离子起到助模板剂的作用, 并填充在 AlPO4-42 分子筛孔道中. 晶化产物随晶化时间的演变表明, 体系中有机胺浓度的变化改变了动力学路径. 高浓度有机胺所形成的聚集体组装周围的无机物种, 促进了 sod 或 lta 笼结构的形成, 并导致立方相的 LTA 骨架晶化.

关键词: 离子热合成, 磷酸铝分子筛, 有机胺, 助模板剂, LTA 型结构

Abstract: The LTA type aluminophosphate molecular sieve (AlPO4-42) was ionothermally synthesized by introducing organic amine into the 1-butyl-3-methylimidazolium bromide ([bmim]Br) ionic liquid. The as-synthesized products were characterized and the crystallization ki-netics was investigated. Thermal gravimetric analysis, nuclear magnetic resonance spectroscopy, and infrared spectroscopy demonstrated that the organic amine and the cation of the ionic liquid filled in the channels of the molecular sieve together. The introduced amine acted as the synergetic templates in a certain aggregated state according to the result of photoluminescence emission spectroscopy. The final products varied with the crystallization time, and the kinetic pathway was influenced by the amine concentration, which decreased with the growth of the crystal product during the crystallization. The inorganic materials reassembled around these aggregated templates when they exist in a high concentration to form sod or lta cages, resulting in the crystallization of cubic LTA framework.

Key words: ionothermal synthesis, aluminophosphate molecular sieve, organic amine, co-template, LTA type structure