| H-ZSM-5分子筛不同孔道处的酸位在甲醇制烯烃反应中的催化作用 |
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| 引用本文： | 王森,李志凯,秦张峰,董梅,李俊汾,樊卫斌,王建国. H-ZSM-5分子筛不同孔道处的酸位在甲醇制烯烃反应中的催化作用[J]. 催化学报, 2021, 42(7): 1126-1136,中插21-中插24. DOI: 10.1016/S1872-2067(20)63732-9 |
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| 作者姓名： | 王森 李志凯 秦张峰 董梅 李俊汾 樊卫斌 王建国 |
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| 作者单位： | 中国科学院山西煤炭化学研究所, 煤转化国家重点实验室, 山西太原030001;中国科学院山西煤炭化学研究所, 煤转化国家重点实验室, 山西太原030001;中国科学院大学, 北京100049 |
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| 基金项目： | This work was supported by the National Key R&D Program of China ;山西省优秀博士生;the Natural Science Foundation of Shanxi Province of China ;山西省自然科学基金;煤转化国家重点实验室自主研究项目;国家重点研发计划;and the Independent Research Project of State Key Laboratory of Coal Con-version, Institute of Coal Chemistry, CAS ;国家自然科学基金;the National Natural Science Foundation of China ;Excellent Doctoral Student Award and Subsidy Program of Shanxi Province |
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| 摘 要： | 甲醇制烯烃(MTO)作为一条由煤、天然气和生物质等含碳资源制备重要有机化学品的非石油路线,近年来备受关注.作为MTO催化剂,分子筛的骨架拓扑结构和酸性质对于其催化活性、反应路径和产物分布等具有重要的影响.H-ZSM-5分子筛是一种典型的MTO反应催化剂,酸位可以分布在MFI拓扑结构的直孔道、正弦孔道和交叉位点处.虽然目...
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| 关 键 词： | 甲醇制烯烃 H-ZSM-5分子筛 酸位分布 密度泛函理论计算 分子动力学模拟 |
Catalytic roles of the acid sites in different pore channels of H-ZSM-5 zeolite for methanol-to-olefins conversion |
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| Sen Wang,Zhikai Li,Zhangfeng Qin,Mei Dong,Junfen Li,Weibin Fan,Jianguo Wang. Catalytic roles of the acid sites in different pore channels of H-ZSM-5 zeolite for methanol-to-olefins conversion[J]. Chinese Journal of Catalysis, 2021, 42(7): 1126-1136,中插21-中插24. DOI: 10.1016/S1872-2067(20)63732-9 |
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| Authors: | Sen Wang Zhikai Li Zhangfeng Qin Mei Dong Junfen Li Weibin Fan Jianguo Wang |
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| Affiliation: | (State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,Shanxi,China;University of the Chinese Academy of Sciences,Beijing 100049,China) |
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| Abstract: | H-ZSM-5 zeolite is a typical catalyst for methanol-to-olefins (MTO) conversion. Although the per-formance of zeolite catalysts for MTO conversion is related to the actual location of acid sites in the zeolite framework, the catalytic roles of the acid sites in different pore channels of the H-ZSM-5 zeolite are not well understood. In this study, the MTO reaction network, involving the aromatic cycle, alkene cycle, and aromatization process, and also the diffusion behavior of methanol feed-stock and olefin and aromatic products at different acid sites in the straight channel, sinusoidal channel, and intersection cavity of H-ZSM-5 zeolite was comparatively investigated using density functional theory calculations and molecular dynamic simulations. The results indicated that the aromatic cycle and aromatization process occurred preferentially at the acid sites in the intersection cavities with a much lower energy barrier than that at the acid sites in the straight and sinusoidal channels. In contrast, the formation of polymethylbenzenes was significantly suppressed at the acid sites in the sinusoidal and straight channels, whereas the alkene cycle can occur at all three types of acid sites with similar energy barriers and probabilities. Consequently, the catalytic performance of H-ZSM-5 zeolite for MTO conversion, including activity and product selectivity, can be regulated properly through the purposive alteration of the acid site distribution, viz., the location of Al in the zeolite framework. This study helps to elucidate the relation between the catalytic performance of different acid sites in the H-ZSM-5 zeolite framework for MTO conversion, which should greatly benefit the design of efficient catalyst for methanol conversion. |
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| Keywords: | Methanol-to-olefins H-ZSM-5 zeolite Acid site distribution Density functional theory calculation Molecular dynamic simulation |
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