再生时间对甲醇制烯烃催化剂水蒸气再生过程的影响  

Effect of regeneration time on steam regeneration of spent catalyst in methanol to olefins process

作　　者：安怀清 周吉彬 张今令[1] 张涛[1] 叶茂[1] 刘中民[1,2] AN Huaiqing;ZHOU Jibin;ZHANG Jinling;ZHANG Tao;YE Mao;LIU Zhongmin(National Engineering Laboratory for Methanol to Olefins,Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院大连化学物理研究所甲醇制烯烃国家工程实验室,辽宁大连116023 [2]中国科学院大学,北京100049

出　　处：《化工进展》2022年第1期221-226,共6页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(91834302)。

摘　　要：对甲醇制烯烃(MTO)过程失活催化剂采用水蒸气再生不仅可以减少二氧化碳排放,而且能提高低碳烯烃选择性,具有很好的应用前景。本文针对工业MTO过程使用的SAPO-34分子筛催化剂,研究了再生时间对水蒸气再生过程的影响。采用XRD、NH3-TPD、TGA、FTIR、GC-MS以及N2物理吸脱附表征手段对再生催化剂样品的晶体结构、酸性、残炭性质以及结构参数进行了表征,并考察再生催化剂的MTO反应性能。结果表明,再生时间越长,再生催化剂上残炭量越低,其酸性、比表面积和孔结构等能较好地恢复,在MTO反应中表现出更长的催化寿命。在再生过程中,催化剂上的残炭物种由芘、菲等大分子量的有机物转变为对MTO具有反应活性的萘等小分子有机物;但是可溶性残炭物种随着再生时间的延长而减少,从而使得初始低碳烯烃选择性有所降低。The SAPO-34 zeolite catalyzed methanol to olefins(MTO)process has been shown of practical significance.Recent study has demonstrated that steam regeneration is superior to air combustion in terms of CO_(2) emission reduction and light olefins selectivity enhancement.In this work we investigated the effect of regeneration time on the steam regeneration of spent catalyst used in MTO process.The crystal structure,acidity,residual coke properties and structural parameters of the catalyst samples regenerated under different regeneration time were characterized by XRD,NH3-TPD,FTIR,TGA,GC-MS and N_(2) physical adsorption-desorption.The results showed that the increase of regeneration time would reduce the amount of residual coke on the regenerated catalyst,and yield better recovery of the acidity,BET surface area and pore structure of the catalyst samples,which could prolong catalyst’s lifetime.Furthermore,it is shown that the residual coke species on the catalyst changed from pyrene and phenanthrene to naphthalene during the steam regeneration.However,the soluble residual coke species decreased with the extension of regeneration time,which would reduce the selectivity of light olefins at the beginning of MTO reaction.

关 键 词：甲醇制烯烃 SAPO-34催化剂 失活催化剂 水蒸气再生 

分 类 号：TQ546.2[化学工程—煤化学工程]