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	热重-质谱联用研究甲醇制烯烃反应的积炭裂解特性
	张明烨 ; 崔宇 ; 李玉新 ; 魏飞 ; 王垚 ; ZHANG Ming-ye ; CUI Yu ; LI Yu-xin ; WEI Fei ; WANG Yao
	2016-03-30 ; 2016-03-30
关键词	甲醇制烯烃 MTO SAPO-34催化剂 积炭裂解 活化能 热重质谱联用 methanol to olefins MTP SAPO-34 catalyst coke cracking activation energy TGA-MS TQ221.2
其他题名	TGA-MS study oncracking of the coke deposited on catalyst for MTO Reaction
中文摘要	考察了甲醇制烯烃(MTO)过程使SAPO-34沸石催化剂失活的积炭在惰性气氛程序升温下的裂解反应,发现积炭中存在大量在400℃~600℃可裂解的组分。通过热重-质谱联用研究了积炭的裂解特性,确认裂解的气体产物主要为丙烯和乙烯。通过气质联用及原位红外分析裂解前后的积炭组成变化,证明乙烯、丙烯是部分积炭物种(如:多甲基苯、多甲基萘等)在高温下裂解脱甲基侧链的产物,同时生成无侧链的稠环芳烃。通过不同升温速率下乙烯和丙烯生成速率变化,计算得到积炭物种裂解生成乙烯和丙烯的表观活化能分别为68.4kJ/mol和47.5kJ/mol。上述结果说明,在失活催化剂烧焦再生之前,可采用高温汽提裂解积炭,降低MTO过程的焦炭选择性,增产烯烃产品。由于裂解生成乙烯的表观活化能高于生成丙烯的活化能,因此降低温度有利于提高丙烯与乙烯之比。; The cracking behaviors of the coke deposited on the SAPO-34 zeolite catalyst in the methanol-to-olefins(MTO) process, which resulted in the deactivation of catalyst, were investigated by temperature programmed heating in an inert atmosphere, and it was found that much of the coke could be cracked at 400-600℃. TGA-MS analysis showed that the main gaseous cracking products were propylene and ethylene. The change of coke before and after cracking was determined by GC-MS and in situ IR, and the results indicated that ethylene and propylene were produced by the cracking of the side chain of the multi-methylbenzene and multi-methylnaphthalene species in the coke, which then formed polycyclic aromatic hydrocarbons without methyl side chains. From the production rates of ethylene and propylene under different temperature-increased rates, the apparent activation energies for the formation of ethylene and propylenewere calculated to be 68.4kJ/mol and 47.5kJ/mol, respectively. The results implied that the coke selectivity in MTO process could be reduced by high temperature stripping of the catalyst before the burning regeneration, which would increase the yield of olefins. Since the apparent activation energy for ethylene formation is higher than that for propylene formation, the ratio of propylene to ethylene in the cracking gaseous product would increase with decreasing temperature.
语种	中文 ; 中文
内容类型	期刊论文
源URL	[http://ir.lib.tsinghua.edu.cn/ir/item.do?handle=123456789/144032]
专题	清华大学
推荐引用方式 GB/T 7714	张明烨,崔宇,李玉新,等. 热重-质谱联用研究甲醇制烯烃反应的积炭裂解特性[J],2016, 2016.
APA	张明烨.,崔宇.,李玉新.,魏飞.,王垚.,...&WANG Yao.(2016).热重-质谱联用研究甲醇制烯烃反应的积炭裂解特性..
MLA	张明烨,et al."热重-质谱联用研究甲醇制烯烃反应的积炭裂解特性".(2016).

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