Promoting the alkylation of toluene to para-xylene over MCM-22 by the steric effects of trimethylsilyl groups

IF 2.8 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY Research on Chemical Intermediates Pub Date : 2024-07-23 DOI:10.1007/s11164-024-05352-z
Bing Yan, Yalan Feng, Zonghui Liu, Bing Xue
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Abstract

Owing to the low energy consumption and few by-products, toluene alkylation is regarded as a promising way to produce p-xylene. The zeolites with the characteristics of 10-MR were usually employed to catalyze the toluene alkylation after being modified. However, the catalyst activity is liable to sharp decrease by common modifying strategies. In this study, the alkylation of toluene with dimethyl carbonate was catalyzed by the MCM-22 zeolites with selective dealumination and silanization treatment. The Al sites on the MCM-22 external surface were first eliminated by oxalic acid, and then trimethylsilyl groups were grafted at the external surface of MCM-22 by bonding with Si–OH formed from dealumination. This modification strategy can not only reduce the Brønsted acid sites on the external surface and narrow the pore entrance size but also retain more internal active sites, leading to improving PX selectivity without a significant decrease in activity. Compared to parent MCM-22, the PX selectivity was doubled, and the toluene conversion only decreased from 39 to 34% over 200-DeMCM-22 catalyst at 400 °C.

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通过三甲基硅基的立体效应促进甲苯在 MCM-22 上烷基化为对二甲苯
由于能耗低、副产品少,甲苯烷基化被认为是生产对二甲苯的一种有前途的方法。具有 10-MR 特性的沸石经过改性后通常被用来催化甲苯烷基化反应。然而,普通的改性策略容易导致催化剂活性急剧下降。在本研究中,MCM-22 沸石经选择性脱铝和硅烷化处理后催化了甲苯与碳酸二甲酯的烷基化反应。首先用草酸消除 MCM-22 外表面的 Al 位点,然后在 MCM-22 外表面接枝三甲基硅基,并与脱烷基形成的 Si-OH 结合。这种改性策略不仅能减少外表面的布氏酸位点,缩小孔隙入口尺寸,还能保留更多的内部活性位点,从而在不显著降低活性的情况下提高 PX 选择性。与母体 MCM-22 相比,200-DeMCM-22 催化剂在 400 °C 下的 PX 选择性提高了一倍,甲苯转化率仅从 39% 降至 34%。
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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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