Catalytic upgrading of lignite pyrolysis volatiles to light aromatics under methanol atmosphere over Zr and/or Fe modified hollow ZSM-5 zeolites

IF 4.8 3区 材料科学 Q1 CHEMISTRY, APPLIED
Yue-lun Wang , Han-bing Gao , Wei-hua Zhao , Xu Yan , Jing Liang , Yun-Peng Zhao , Jing-pei Cao , Lin-jun Zhu
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Abstract

Fe and Zr modified hollow ZSM-5 zeolites were prepared and their applications in upgrading of lignite pyrolysis volatiles coupling with methanol to light aromatics were investigated. The results demonstrated that hollow zeolites with larger voids and shorter diffusion length favored the production of light aromatics. Adding Fe and Zr into ZSM-5 zeolites further enhanced BTX yields due to the synergism between metals and acid sites for promoting hydrodeoxygenation reactions. Meanwhile, Zr-Fe/HZ-5 catalyst with increasing Lewis acid sites facilitated methylation leading to high selectivity of xylene under methanol atmosphere. Moreover, diffusion behaviors of xylene were quantified. Higher self-diffusion coefficient of molecules in hollow zeolites led to the formation of less coke, while the incorporation of Fe and Zr promoted the formation of catalytic coke due to the increase of alkylation resulting in partial conversion of BTX into PAHs on external surfaces although the total coke yields were further decreased.

Abstract Image

在甲醇气氛下,在 Zr 和/或 Fe 改性空心 ZSM-5 沸石上催化褐煤热解挥发物升级为轻芳烃
制备了铁和锆改性的空心 ZSM-5 沸石,并研究了它们在将褐煤热解挥发物与甲醇偶联升级为轻芳烃中的应用。结果表明,空隙较大、扩散长度较短的空心沸石有利于轻芳烃的生产。在 ZSM-5 沸石中添加 Fe 和 Zr 可进一步提高 BTX 产量,这是因为金属与酸性位点之间的协同作用可促进加氢脱氧反应。同时,增加路易斯酸位点的 Zr-Fe/HZ-5 催化剂可促进甲基化,从而在甲醇气氛下提高二甲苯的选择性。此外,还对二甲苯的扩散行为进行了量化。分子在空心沸石中的自扩散系数越高,形成的焦炭就越少,而铁和锆的加入则促进了催化焦炭的形成,这是因为烷基化作用的增加导致 BTX 部分转化为外表面的多环芳烃,尽管总焦炭产率进一步降低。
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来源期刊
Microporous and Mesoporous Materials
Microporous and Mesoporous Materials 化学-材料科学:综合
CiteScore
10.70
自引率
5.80%
发文量
649
审稿时长
26 days
期刊介绍: Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.
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