Effect of framework structure of ZSM-11 and ZSM-5 zeolites on their catalytic performance in the conversion of methanol to olefins

Q3 Energy 燃料化学学报 Pub Date : 2023-11-01 DOI:10.1016/S1872-5813(23)60361-5
YUAN Kai , JIA Xiang-yu , WANG Sen , FAN Sheng , HE Shi-pei , WANG Peng-fei , DONG Mei , QIN Zhang-feng , FAN Wei-bin , WANG Jian-guo
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Abstract

The catalytic performance of zeolites is closely related to their framework structure and a clear understanding of such a structure-performance relationship is of great significance in revealing catalytic reaction mechanism as well as in developing efficient zeolite catalysts. Herein, ZSM-11 and ZSM-5 zeolites with similar morphology, crystal size, textural properties and acidity were hydrothermally synthesized; the effects of their differences in the 10-ring channels on the catalytic performance in the conversion of methanol to olefins (MTO) were investigated by using various characterization techniques. The results indicate that in comparison with the straight channel of ZSM-11, the sinusoidal channel of ZSM-5 has stronger diffusion resistance, which promotes the hydrogen-transfer in higher olefins, leads to forming more polymethylbenzene species and then raises the contribution of aromatic-based cycle. In contrast, ZSM-11 with straight channel can reduce the formation of polymethylbenzene species and enhance the alkene-based cycle. As a result, compared with ZSM-5-60 with similar morphology and acidity, ZSM-11-60 as a catalyst in MTO exhibits longer lifetime (98.3 h vs. 65.4 h) and higher selectivity to propene (34.6% vs. 27.4%). The insight shown in this work helps to have a better understanding of the relation between zeolite structure and catalytic performance in MTO and is then beneficial to the development of better catalysts and processes for MTO.

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ZSM-11和ZSM-5分子筛骨架结构对其催化甲醇制烯烃性能的影响
沸石的催化性能与其骨架结构密切相关,弄清这种结构-性能关系对揭示催化反应机理和开发高效沸石催化剂具有重要意义。本文采用水热法合成了形貌、晶粒尺寸、结构性质和酸度相近的ZSM-11和ZSM-5沸石;采用各种表征技术研究了它们在10环通道上的差异对甲醇制烯烃(MTO)催化性能的影响。结果表明:与ZSM-11的直线通道相比,ZSM-5的正弦通道具有更强的扩散阻力,促进了高烯烃中氢的转移,形成了更多的多甲基苯,从而提高了芳基循环的贡献。而具有直线型通道的ZSM-11则可以减少多甲基苯的生成,促进烯烃基循环。结果表明,与ZSM-5-60相比,ZSM-11-60作为MTO催化剂具有更长的寿命(98.3 h比65.4 h)和更高的丙烯选择性(34.6%比27.4%)。本研究结果有助于更好地理解沸石结构与MTO催化性能之间的关系,从而有利于开发更好的MTO催化剂和工艺。
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来源期刊
燃料化学学报
燃料化学学报 Chemical Engineering-Chemical Engineering (all)
CiteScore
2.80
自引率
0.00%
发文量
5825
期刊介绍: Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.
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