Regulation of Framework Aluminum Siting and Acid Distribution in H-MCM-22 by Boron Incorporation and Its Effect on the Catalytic Performance in Methanol to Hydrocarbons

催化作用 甲醇 烯烃纤维 布朗斯特德-洛瑞酸碱理论 沸石 选择性 丙烯 化学 酸强度 化学工程 无机化学 有机化学 工程类
作者
Jialing Chen,Tingyu Liang,Junfen Li,Sen Wang,Zhangfeng Qin,Pengfei Wang,Lizhi Huang,Weibin Fan,Jianguo Wang
出处
期刊:ACS Catalysis [American Chemical Society]
卷期号:6 (4): 2299-2313 被引量:131
标识
DOI:10.1021/acscatal.5b02862
摘要

As the process of methanol to hydrocarbons (MTH) is catalyzed by acid sites, the regulation of framework aluminum siting and acid distribution in a zeolite catalyst to enhance its performance in MTH is an important and challenging task. In this work, the regulation of framework aluminum siting in H-MCM-22 was achieved through boron incorporation; the relation between catalytic performance and acid distribution was investigated. The results illustrate that the distribution of framework aluminum and Brönsted acid sites among three types of pores in H-MCM-22 can be regulated through adjusting the content of boron incorporated during synthesis, due to the competitive occupancy of various framework T sites between boron and aluminum, whereas the textural properties and overall acid types and amounts are less influenced by boron incorporation. Incorporating a proper content of boron can concentrate the Brönsted acid sites in the sinusoidal channels rather than in the surface pockets and supercages. The acid sites located in the surface pockets and supercages are prone to carbonaceous deposition, whereas those acid sites in the sinusoidal channels are crucial for MTH in the steady reaction stage. Moreover, the acid sites in the sinusoidal channels are favorable to the olefin-based cycle that produces preferentially higher olefins. As a result, the incorporation of proper content of boron delivers the H-MCM-22 zeolite much greater stability and higher selectivity to higher olefins such as propene and butene in MTH than previously reported. These results help to clarify the relation between the catalytic performance of H-MCM-22 in MTH and its acid distribution and then bring forward an effective approach to develop better MTH catalysts by regulating the acid distribution.
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