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La2O3协同增强SAPO-34的二甲醚制烯烃催化性能
引用本文:曹迎倩,高玉李,陈胜利,袁桂梅,王涯,朱茹月,陈楠.La2O3协同增强SAPO-34的二甲醚制烯烃催化性能[J].化工学报,2017,68(12):4607-4614.
作者姓名:曹迎倩  高玉李  陈胜利  袁桂梅  王涯  朱茹月  陈楠
作者单位:中国石油大学(北京)重质油国家重点实验室, 北京 102249
基金项目:国家自然科学基金项目(91534120)。
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  
收稿时间:2017-05-31
修稿时间:2017-08-18

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.La2O3synergetic effect to improve catalytic performance of SAPO-34 molecular sieve used for dimethyl ether to olefins reaction[J].Journal of Chemical Industry and Engineering(China),2017,68(12):4607-4614.
Authors:CAO Yingqian  GAO Yuli  CHEN Shengli  YUAN Guimei  WANG Ya  ZHU Ruyue  CHEN Nan
Affiliation:State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Beijing 102249, China
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.
Keywords:SAPO-34  molecular sieves  mixing  deactivation  dimethyl ether to olefins  methanol to ofefins  synergetic effects  
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