Urea-induced platelike ZSM-5 zeolites with Si zoning for efficient alkylation of toluene with ethanol to para-ethyltoluene†

IF 6.4 1区 化学 Q1 CHEMISTRY, INORGANIC & NUCLEAR Inorganic Chemistry Frontiers Pub Date : 2025-03-25 DOI:10.1039/D5QI00100E
Jialin Tan, Lei Miao, Yang Liu, Shujing Chen, Zhe Hong, Lihua Deng, Qun Yang, Xianlong Gao, Fangtao Huang and Zhirong Zhu
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Abstract

Platelike zeolites with a short diffusion pathway are promising catalysts due to mass transfer advantages. Herein, platelike ZSM-5 with a reduced b-axis thickness (∼90 nm) was synthesized using a urea-assisted crystallization strategy. We disclose the significant application of this platelike catalyst in the toluene alkylation reaction with ethanol to produce para-ethyltoluene (p-ET). The reaction results demonstrate that this platelike ZSM-5 exhibits a higher toluene conversion (58.3%) and ET selectivity (88.7%) than conventional ZSM-5. This improvement is primarily due to the shortened straight channels of platelike ZSM-5, which facilitate mass transport and increase the accessibility to acid sites. Nevertheless, the shortened b-axis of platelike ZSM-5 seems to have no significant positive impact on para-selectivity for p-ET. Hence, we constructed a Si-zoned external surface on the platelike ZSM-5 by means of the surface modification strategy to accurately passivate the surface acid sites, thereby inhibiting the isomerization reaction, and achieving higher selectivity for p-ET (>95%) and extended catalytic stability (>100 h) in the reaction of toluene alkylation with ethanol.

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具有硅区带的尿素诱导板状ZSM-5分子筛用于甲苯与乙醇的高效烷基化生成对乙基甲苯
具有短扩散路径的板状沸石具有传质优势,是一种很有前途的催化剂。本文采用尿素辅助结晶策略合成了b轴厚度缩短(~90 nm)的片状ZSM-5。我们揭示了这种板状催化剂在甲苯与乙醇烷基化反应中产生对乙基甲苯(p-ET)的重要应用。实验结果表明,与传统的ZSM-5相比,这种片状ZSM-5具有更高的甲苯转化率(58.3%)和ET选择性(88.7%)。这种改善主要是由于片状ZSM-5缩短了直道,方便了物质的运输,增加了酸位的可达性。然而,片状ZSM-5的b轴缩短似乎对p-ET的准选择性没有显著的积极影响。因此,我们通过表面修饰策略在类似板的ZSM-5上构建了一个硅带外表面,以精确钝化表面酸位,从而抑制异构化反应,并获得更高的p-ET (>;95%),甲苯与乙醇烷基化反应具有良好的催化稳定性(>100 h)。
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来源期刊
Inorganic Chemistry Frontiers
Inorganic Chemistry Frontiers CHEMISTRY, INORGANIC & NUCLEAR-
CiteScore
10.40
自引率
7.10%
发文量
587
审稿时长
1.2 months
期刊介绍: The international, high quality journal for interdisciplinary research between inorganic chemistry and related subjects
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