石油炼制与化工 ›› 2017, Vol. 48 ›› Issue (3): 48-53.

• 基础研究 • 上一篇    下一篇

正辛烷在不同稀土含量Y型分子筛上吸附热力学的研究

廖贞贞1,张乐2,秦玉才1,宋丽娟1,2   

  1. 1. 辽宁石油化工大学辽宁石油化工催化科学与技术重点实验室
    2. 中国石油大学(华东)化学工程学院
  • 收稿日期:2016-08-30 修回日期:2016-10-09 出版日期:2017-03-12 发布日期:2017-02-24
  • 通讯作者: 宋丽娟 E-mail:lsong56@lnpu.edu.com
  • 基金资助:
    国家自然科学基金项目

ADSORPTION THERMODYNAMICS OF n-OCTANE OVER ZEOLITES WITH DIFFERENT CONTENT OF RARE EARTH

    

  1.  
  • Received:2016-08-30 Revised:2016-10-09 Online:2017-03-12 Published:2017-02-24
  • Supported by:
     

摘要: 以正辛烷为吸附质,采用智能质量分析仪(IGA)和程序升温脱附(TPD)技术考察了不同稀土含量对Y型分子筛吸附热力学参数(吸附热Qst、焓变ΔH、熵变ΔS)的影响及变化规律。结合TPD数据剖析了稀土含量调变分子筛催化活性的实质。结果表明:吸附质在分子筛上的吸附位作用力的大小与分子筛内稀土含量有关;较高含量稀土的引入,使得吸附质与分子筛的作用力加强,从而使吸附质在吸附剂上较难脱附,在分子筛上的停留时间较长,容易过度裂解,结焦生炭;而适量稀土的引入[(w)Ce2O3=4%],可以调变分子筛活性位上的吸附选择性,使得吸附质分子在吸附剂孔道内有序化呈现规律性,可以改变其在分子筛上的停留时间,进而有利于大分子裂解反应的发生,提高目标产物的收率。

关键词: 稀土含量, 吸附热力学, 作用力, 活性, 催化活性

Abstract: The adsorption thermodynamics (adsorption heat, enthalpy change, entropy change) and the related regularities of n-octane adsorbed on REY zeolites with different content of rare earth ion was studied by high precision intelligent gravimetric analyzer (IGA) and temperature programmed desorption (TPD) techniques. The activity modification principle was analyzed by TPD combined with dynamic results. It is discovered that the interaction magnitude of the adsorbent with the adsorption sites on the zeolite is related to the content of the rare earth. A higher content of rare earth introduction strengthens interaction and make the adsorbent stay in zeolite long time, leading to an excessive cracking and coking due to strong adsorption and difficult desorption. The introduction of appropriate amount of rare earth (4% Ce2O3) can mildly modulate the adsorption strength on zeolite active sites, so that the order is regularized and the residence time of adsorbate molecule in the zeolite pores is changed, which is helpful macromolecule cracking reaction occur and improve the yield of the target product.

Key words: rare earth content, adsorption thermodynamics, interaction, activity, catalytic activity

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