Highly para-selective alkylation of toluene with methanol over modified superfine nano-ZSM-5 aggregates

IF 3.5 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Xiaotong Mi, Yongheng Li, Peipei Zhang, Sixuan Li, Jing Xin, Zhanggui Hou
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Abstract

Alkylation between toluene and methanol is a promising route to produce para-xylene (PX). ZSM-5 zeolite commonly used as a catalyst in toluene alkylation with methanol, has been paid extensive attention. In this study, synthesis of superfine nano-ZSM-5 aggregates with fast mass transfer and controllable acid properties were realized before modification in an simple way. Firstly, nano-ZSM-5 aggregates with fast mass transfer was synthesized combined with a dual-silica source and a low-temperature crystallization method. The acid properties, such as W/S and LASs/BASs, were adjusted during low-temperature crystallization. Secondly, the mass transfer ability was further enhanced by introducing more irregular pore structures via alkali treatment method, meanwhile, the acid properties were further optimized to obtain increased W/S and LAS/BAS ratios, which had positive on the catalytic performance. After SiO2 modification, the obtained Si/AH-NTZ-130 catalyst displayed excellent performance with the PX selectivity approaching 80%. Moreover, the optimized Si/P-AH-NTZ-130 was stable for 120 h, with a PX selectivity of nearly 100%.

Abstract Image

Abstract Image

改性超细纳米zsm -5聚集体上甲苯与甲醇的高度准选择性烷基化
甲苯与甲醇的烷基化反应是制备对二甲苯(PX)的一条很有前途的途径。ZSM-5沸石是甲苯与甲醇烷基化反应中常用的催化剂,受到了广泛的关注。在本研究中,通过简单的改性前,实现了快速传质、酸性质可控的超细纳米zsm -5聚集体的合成。首先,结合双硅源和低温结晶法合成了具有快速传质性能的纳米zsm -5聚集体;在低温结晶过程中调整了W/S和LASs/BASs等酸性质。其次,通过碱处理方法引入更多的不规则孔隙结构,进一步增强了传质能力,同时进一步优化了酸性能,提高了W/S和LAS/BAS比,这对催化性能有积极的影响。SiO2改性后的Si/AH-NTZ-130催化剂表现出优异的性能,对PX的选择性接近80%。优化后的Si/P-AH-NTZ-130在120 h内稳定存在,对PX的选择性接近100%。
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来源期刊
CiteScore
5.70
自引率
18.20%
发文量
229
审稿时长
2.6 months
期刊介绍: Research on Chemical Intermediates publishes current research articles and concise dynamic reviews on the properties, structures and reactivities of intermediate species in all the various domains of chemistry. The journal also contains articles in related disciplines such as spectroscopy, molecular biology and biochemistry, atmospheric and environmental sciences, catalysis, photochemistry and photophysics. In addition, special issues dedicated to specific topics in the field are regularly published.
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