高等学校化学学报 ›› 2000, Vol. 21 ›› Issue (9): 1353.

• 论文 • 上一篇    下一篇

超微NaY分子筛的合成(Ⅰ)──添加轻稀土离子的影响

晁自胜1, 林海强1, 陈国周1, 吴廷华1, 万惠霖1, 闵恩泽2   

  1. 1. 厦门大学化学系, 固体表面物理化学国家重点实验室, 厦门 361005;
    2. 中国石化集团公司北京石油化工科学研究院, 北京 100083
  • 收稿日期:1999-06-04 出版日期:2000-09-24 发布日期:2000-09-24
  • 通讯作者: 晁自胜(1967年出生),男,博士,副教授,从事分子筛合成及多相催化研究.
  • 基金资助:

    中国石化集团公司科技开发项目(批准号:X598010)资助.

Synthesis of Ultrafine Zeolite NaY(Ⅰ) Effect of Light Rare Earth Ions Additive

CHAO Zi-Sheng1, LIN Hai-Qiang1, CHEN Guo-Zhou1, WU Ting-Hua1, WAN Hui-Lin1, MIN En-Ze2   

  1. 1. Chemistry Department and State Key Laboratory for Physical Chemistry of Solid Surface of Xiamen University, Xiamen 361005, China;
    2. Research Instituteof Petroleum Processing, SINOPEC, Beijing 100083, China
  • Received:1999-06-04 Online:2000-09-24 Published:2000-09-24

摘要: 导向剂的陈化时间和反应胶的晶化温度可以影响NaY分子筛的晶化行为.随导向剂陈化时间的增加,NaY分子筛的晶化速度加快,晶粒尺寸减小;随晶化温度的升高,NaY分子筛的晶化速度加快,但晶粒尺寸增加.而向合成体系中添加轻稀土离子(Ln3+)对NaY分子筛的晶化行为影响更为明显.与未添加稀土离子时相比较,在一定的稀土离子添加量范围内[n(Ln3+)/n(Al3+)<0.2],NaY分子筛的晶化速度明显加快而晶粒尺寸显著减小,同时所合成出的NaY分子筛的n(SiO2)/n(Al2O3)比也有较大的提高.添加稀土离子使合成体系中形成异晶晶种的Ln(OH)3微晶,从而进一步引发NaY分子筛的成核.

关键词: 超微分子筛, NaY, 晶体尺寸, 合成, 稀土离子

Abstract: Ultrafine zeolite NaYwas hydrothermally crystallized with silica sol and Al2(SO4)2 as source materials via optimizing synthesis conditions and adding light rare earth ions(Ln 3+) to the synthesis batch. The crystallization performance of NaYcould be affected by the aging time of nucleation Si-Al gel and the crystallization temperature of reaction Si-Al gel. With increasing the aging time(2—7 d) of nucleation gel, the crystallization rate of zeolite NaYincreased whereas the average crystal size of zeolite NaYdecreased. When elevating the crystallization temperature(363—383 K) of reaction gel, both the crystallization rate and the average crystal size of zeolite NaYincreased. Nevertheless, the crystallization performance of zeolite NaYwas more remarkably affected by the addition of Ln3+ ions in the synthesis batch. The crystallization rate and the n(SiO2)/n(Al2O3) ratio obviously increased while the average crystal size greatly reduced when zeolite NaYwas crystallized in the presence of Ln3+ ions, comparing with that in the absence of Ln3+ ions. It was found that, with the amount of the added Ln 3+ ions increasing, the average crystal size of zeolite NaYdecreased followed by increasing, while the crystallization rate and the SiO2/Al2O3 ratio in framework changed in the opposite direction. The optimal amount of Ln 3+ additive appears to be in the range of n(Ln3+)∶n(Al 3+)=0.05∶1—0.1∶1 in mole. In the case, the as-synthesized NaYzeolites had the smallest average crystal sizes(<100 nm), the highest n(SiO2)/n(Al2O3) ratio(>5.7) and the shortest crystallization time(<36 h). The role of the added Ln3+ ions was proposed to be that there formed the micro-crystalline Ln(OH)3 under the synthesis conditions, which may present additional area to initiate the nucleation of zeolite NaY.

Key words: Ultrafine zeolite, NaY, Crystal size, Synthesis, Rare earth ions

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