化学学报 ›› 1990, Vol. 48 ›› Issue (7): 632-638.    下一篇

研究论文

Y沸石的酸性

高滋;唐颐   

  1. 复旦大学化学系
  • 发布日期:1990-07-15

Studies on the acidity of zeolite Y

GAO ZI;TANG YI   

  • Published:1990-07-15

用^29Si MAS NMR(MAS为Magie Angle Spinning), 统计计算,NH3-TPD 等方法对(NH4)2·SiF6去铝补硅得到的高硅Y型沸石的酸位分布情况进行了研究, 并与典型酸催化反应数据相关联, 证实了Y型沸石的酸位强度取决于A1原子的周围环境, 即与次邻位A1原子数目n-NNN(NNN为Next Nearst Neighbor)有关, 沸石的强酸性来自次邻位无A1原子的AIO^-4四面体。 NH3-TPD法测量的沸石酸量和酸强度数据与^29Si MAS NMR 实验结果和统计计算得到的不同n-NNN A1位的分布是一致的。 随着A1含量减少, Y型沸石表面的总酸量是单调下降的。但强酸量却是先增加后下降, 在A1/(A1+Si)为0.15左右出现极大值。不同硅铝比的Y型沸石对典型的强酸性和弱酸性催化反应的活性变化规律亦与酸性相吻合。

关键词: 铵化合物, 沸石, 酸催化剂, 氟化物, 硅化合物, 酸性, 催化活性, 脱铝

The distribution of acid sites of different acid strengths on zeolite Y with different Si/Al ratios prepared by secondary synthesis with (NH4)2SiF6 were studied by 20Si magic angle spinning (MAS) NMR, statistical calculation, and NH3-TPD temperature- desorption. The data correlated with the activities of the zeolites toward typical acid-ctalyzed reactions. The acid strength of the Al sites in zeolite Y framework depends on their local framework environment, i.e. the no. of next nearest Al neighbors. Changes in zeolite acidity and acid strength with Al content measured by NH3-TPD with the result of 29Si MAS NMR and the distribution of Al sites obtained from statistical calculation As the Al content decreases, the total acidity of zeolite Y decreases, but the strong acidity increases first and then decreases. The max. of the curve of the strong acidity is located at Al/(Al + Si) = 0.15. The catalytic activity of the zeolites toward isopropanol dehydration, which requires only weak acidity, and the total acidity vary similarly with Al content. The catalytic activity toward cumene cracking, which needs strong acidity, parallels that of the strong acidity.

Key words: AMMONIUM COMPOUND, ZEOLITE, ACID CATALYST, FLUORIDE, SILICON COMPOUNDS, ACID PROPERTY, CATALYTIC ACTIVITY, DEALUMINIZATION

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