应用化学 ›› 1994, Vol. 0 ›› Issue (6): 32-36.

• 研究论文 • 上一篇    下一篇

甲烷氧化偶联Ti-La-Li系氧化物催化剂制备方法的研究

赵震, 远松月, 于作龙   

  1. 中国科学院长春应用化学研究所 长春 130022
  • 收稿日期:1994-03-17 修回日期:1994-06-22 出版日期:1994-12-10 发布日期:1994-12-10
  • 基金资助:
    国家自然科学基金资助项目

Studies on Preparation Method of Mixed Li-La-Ti Oxide Catalysts for Oxidative Coupling of Methane

Zhao Zhen, Yuan Songyue, Yu Zuolong   

  1. Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, ChangChun 130022
  • Received:1994-03-17 Revised:1994-06-22 Published:1994-12-10 Online:1994-12-10

摘要: 考察了用不同来源Li(LiNO3和Li2SO4)制备的催化剂催化的甲烷氧化偶联(OCM)反应的特点,探讨了以LiNO3为锂源制备的催化剂的高温反应失活机理。XRD、IR、XPS和BET等方法的研究结果表明,以LiNO3为锂源制备的催化剂具有反应活性高、空速大的特点,而以Li2SO4为锂源制备的催化剂具有C2选择性高、活性低、空速小等特点。由LiNO3制得的催化剂的失活原因是:在较高的反应温度下由于表面Li的流失,使体相晶格中的Li向表相扩散进而导致含Li活性相LaTi1-yLiyO3-λ的分解(或部分分解),从而减少了体相和表相中氧空位的数量,导致催化剂的活性降低。设计了NH1(SO4)2浸渍法来固定表面锂。

关键词: 甲烷, 氧比偶联反应, 锂镧钛复合氧比物, 失活

Abstract: The mixed lithium-lanthnum-titanium oxide catalysts have been prepared from different Li-containing compounds(LiNO3, Li2SO4)for oxidative coupling of methane, The XRD, IR, XPS, and BET resuIts showed that LiLa0.5Ti0.5O2+λ catalysts prepared from LiNO3 possessed a higher activity and space velocity, while those from Li2SO4 possessed a much higher C2 selectivity, but lower activity and space velocity. The deactivation of LiLa0.5Ti0.5O2+λ catalysts prepared from LiNO3 is mainly caused by the loss of surface lithium. In the course of the coupling reaction the bulk lithium diffuses to the surface, leading to the decomposition of active phase containing lithium and lowering the amount of oxygen vacancies. In order to combine the advantages of both catalysts prepared from LiNO3 and Li2SO4 and to fix the surface lithium a novel preparation method with impregnation in (NH4)2SO4 is proposed.

Key words: methane, oxidative coupling, lithium-lanthanum-titanium mixed oxide, deactivation