物理化学学报 >> 2011, Vol. 27 >> Issue (12): 2893-2899.doi: 10.3866/PKU.WHXB20112893

催化和表面科学 上一篇    下一篇

SSZ-33分子筛的合成、表征及其对汽车尾气中碳氢化合物的捕集性能

潘瑞丽1,2, 樊卫斌3, 李玉平4, 李晓峰1, 李莎1, 窦涛1,5   

  1. 1. 太原理工大学精细化工研究所, 太原 030024;
    2. 太原科技大学化学与生物工程学院, 太原 030021;
    3. 中国科学院山西煤炭化学研究所, 太原 030001;
    4. 太原理工大学材料科学与工程学院, 太原 030024;
    5. 中国石油大学北京化工学院CNPC 催化重点实验室, 北京 102249
  • 收稿日期:2011-05-23 修回日期:2011-08-25 发布日期:2011-11-25
  • 通讯作者: 窦涛 E-mail:dtao1@163.com
  • 基金资助:

    国家自然科学基金(20973123)资助项目

Synthesis, Characterization of SSZ-33 Molecular Sieves and Their Performance for the Automobile Tailpipe Hydrocarbon Trap

PAN Rui-Li1,2, FAN Wei-Bin3, LI Yu-Ping4, LI Xiao-Feng1, LI Sha1, DOU Tao1,5   

  1. 1. Research Institute of Special Chemicals, Taiyuan University of Technology, Taiyuan 030024, P. R. China;
    2. Institute of Chemicaland Biological Technology, Taiyuan University of Science and Technology, Taiyuan 030021, P. R. China;
    3. Institute of CoalChemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China;
    4. College of Materials Science and Engineering, TaiyuanUniversity of Technology, Taiyuan 030024, P. R. China;
    5. CNPC Key Laboratory of Catalysis, College of Chemical Engineering,China University of Petroleum-Beijing, Beijing 102249, P. R. China
  • Received:2011-05-23 Revised:2011-08-25 Published:2011-11-25
  • Contact: DOU Tao E-mail:dtao1@163.com
  • Supported by:

    The project was supported by the National Natural Science Foundation of China (20973123).

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摘要： 采用碘化N,N,N-三甲基-8-氨基-三环[5.2.1.02.6]癸烷为结构导向剂, 通过过程控制方法, 经3-4 d 成功合成了高性价比的B-SSZ-33 分子筛. 以B-SSZ-33 为母体, 经过Al(NO3)3溶液后处理制得了Al-SSZ-33 分子筛. 采用X射线衍射(XRD), 傅里叶变换红外(FT-IR)光谱, 扫描电子显微镜(SEM), 热重(TG)分析, 电感耦合等离子体原子发射光谱(ICP-AES), N2吸附/脱附, 27Al 核磁共振(27Al NMR)和NH3程序升温脱附(NH3-TPD)等手段对合成的B-SSZ-33、Al-SSZ-33 样品进行了物理化学性能表征. 并以甲苯作为汽车尾气中碳氢化合物的探针分子, 通过甲苯程序升温脱附测试来考察样品的碳氢捕集性能. 结果表明: 后处理过程中Al 同晶取代B, 从而制得了含骨架Al 的Al-SSZ-33; 在甲苯的程序升温脱附测试中, 由于Al-SSZ-33 相对于B-SSZ-33 具有较强的酸性位, 且表面孔口由于骨架外硅铝物种的修饰, 限制了甲苯的扩散, 致使脱附速率最大时的温度(Tmax)和脱附最终的温度(Tend)均升高, 从而形成了新型汽车尾气捕集催化剂的雏形.

关键词: SSZ-33分子筛, 汽车尾气, 过程控制方法, 碳氢捕集, 程序升温脱附

Abstract: Using N,N,N-trimethyl-8-ammonium tricyclo [5.2.1.02,6] decane iodide as a structure directing agent, B-SSZ-33 molecular sieves with an excellent price-performance ratio was successfully synthesized by process control over 3-4 days. The synthesis of Al-SSZ-33 was achieved by a post-modification procedure of B-SSZ-33 molecular sieves in an Al(NO3)3 solution. These materials were characterized in detail by various techniques such as X-ray diffraction (XRD), Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscopy (SEM), thermogravimetric (TG) analysis, inductively coupled plasma-atomic emission spectroscopy (ICP-AES), N2 adsorption/desorption, temperature programmed desorption of NH3 (NH3-TPD), and solid state 27Al nuclear magnetic resonance (27Al NMR). The temperature programmed desorption characteristics of toluene for the B-SSZ-33 and Al-SSZ-33 samples were obtained to understand the efficacy of these materials as hydrocarbon traps. The results show that Al-SSZ-33 with framework Al was obtained after the post-modification procedures. Compared with B-SSZ-33, Al-SSZ-33 has a higher acid strength and shows a comparatively higher toluene desorption temperature (Tmax). The presence of extra framework Al and Si species in Al-SSZ-33 modifies its pores and results in a higher desorption end temperature (Tend). Therefore, the synthesized Al-SSZ-33 is a novel catalyst for use as a hydrocarbon trap in automobile tailpipes.

Key words: SSZ-33 molecular sieves, Automobile tailpipe, Process control method, Hydrocarbon trap, Temperature programmed desorption