CIESC Journal ›› 2017, Vol. 68 ›› Issue (12): 4607-4614.DOI: 10.11949/j.issn.0438-1157.20170702

Previous Articles     Next Articles

La2O3synergetic effect to improve catalytic performance of SAPO-34 molecular sieve used for dimethyl ether to olefins reaction

CAO Yingqian, GAO Yuli, CHEN Shengli, YUAN Guimei, WANG Ya, ZHU Ruyue, CHEN Nan   

  1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China
  • Received:2017-05-31 Revised:2017-08-18 Online:2017-12-05 Published:2017-12-05
  • Supported by:

    supported by the National Natural Science Foundation of China (91534120).

La2O3协同增强SAPO-34的二甲醚制烯烃催化性能

曹迎倩, 高玉李, 陈胜利, 袁桂梅, 王涯, 朱茹月, 陈楠   

  1. 中国石油大学(北京)重质油国家重点实验室, 北京 102249
  • 通讯作者: 陈胜利
  • 基金资助:

    国家自然科学基金项目(91534120)。

Abstract:

The working lifetime of SAPO-34 for dimethyl ether to olefins (DTO) reaction was increased by non-contact La2O3. Increasing ratio of La2O3 to SAPO-34 prolonged working lifetime of SAPO-34. When the mass ratio of La2O3 to SAPO-34 was 1:1, the working lifetime of SAPO-34 was almost twice as much as that of SAPO-34 alone. La2O3 sandwiched in SAPO-34 had improvement, whereas La2O3 in upstream and downstream of SAPO-34 did not. Reaction kinetics and coke amount on SAPO-34 indicated that La2O3 decreased coking rate of SAPO-34. A synergetic mechanism for SAPO-34 and La2O3 was proposed that a coke precursor created on SAPO-34 during DTO was converted to non-coke forming species (such as CO, CO2 and H2) upon traveling onto La2O3 surface such that SAPO-34 coking rate was decreased and its working lifetime was increased.

Key words: SAPO-34, molecular sieves, mixing, deactivation, dimethyl ether to olefins, methanol to ofefins, synergetic effects

摘要:

La2O3不需要与SAPO-34接触,便可显著延长SAPO-34的二甲醚制烯烃(DTO)反应寿命,并且La2O3与SAPO-34比例越大,SAPO-34的反应寿命越长。当La2O3和SAPO-34的质量比为1:1时,SAPO-34寿命提高了约1倍。进一步的研究表明,只有当La2O3层夹在SAPO-34层中间时,才能提高SAPO-34的寿命,La2O3无论是处于SAPO-34上游还是下游,均不能提高SAPO-34的寿命。动力学和催化剂的积炭量研究表明,La2O3是通过降低SAPO-34的积炭速度提高其反应寿命的。初步提出了La2O3提高SAPO-34寿命的机理:在DTO反应过程中,二甲醚在SAPO-34分子筛上形成一种积炭前体,这种积炭前体转移到La2O3的表面上,反应生成不能积炭的化合物(CO、CO2和H2等),从而降低了SAPO-34的积炭失活速度,提高了其寿命。

关键词: SAPO-34, 分子筛, 混合, 失活, 二甲醚制烯烃, 甲醇制烯烃, 协同作用

CLC Number: