Sustainable and Rapid Preparation of the High-Performance MOR Zeolite Membrane for Acetic Acid Dehydration under Fluoride-Free Conditions via a Hydroxyl Radical-Promoted Strategy

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Feng Yu, Yuqin Li, Dengke Cheng, Bowen Chen, Wuwen Si, Yan Wang, Yonghao Li, Xiaowei Wu, Tian Gui, Xiangshu Chen, Hidetoshi Kita
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引用次数: 0

Abstract

The rapid preparation of high-performance MOR zeolite membranes for the dehydration of high-concentration acetic acid under fluoride-free conditions remains a significant challenge. In this study, a hydroxyl radical-promoted strategy was successfully applied to fabricate high-performance MOR zeolite membranes on macroporous mullite supports within only 3 h, under fluoride-free and organic-template-free conditions. The formation process of MOR zeolite membranes in the presence of hydroxyl radicals was systematically investigated. Furthermore, the roles of hydroxyl radicals and hydroxide ions in the synthesis mechanism of MOR zeolite membranes were discussed in detail using characterization methods such as SEM, XRD, EPR, and fluorescence spectroscopy. Compared with the synthesis system without hydroxyl radical participation, the hydroxyl radical-promoted MOR zeolite membranes not only exhibited a significantly shortened crystallization time but also enabled a reduction in the alkalinity of the reaction system. The membrane prepared under optimal conditions demonstrated excellent separation performance in a 90 wt % acetic acid/water mixture at 75 °C, with a permeation flux as high as 1.37 kg m–2 h–1 and a water content in the permeate exceeding 99.4 wt %. Moreover, the MOR zeolite membranes prepared using the hydroxyl radical-promoted strategy showed excellent reproducibility. This hydroxyl radical-promoted approach provides an efficient and environmentally friendly route for the rapid preparation of high-performance zeolite membranes under fluoride-free, template-free, and low-alkalinity conditions.

在无氟条件下羟基自由基促进下可持续快速制备高效醋酸脱水膜的研究
在无氟条件下快速制备高性能MOR沸石膜用于高浓度乙酸脱水仍然是一个重大挑战。在本研究中,在无氟和无有机模板的条件下,羟基自由基促进策略仅在3小时内成功地在大孔莫来石载体上制备了高性能的MOR沸石膜。系统地研究了羟基自由基存在下MOR沸石膜的形成过程。利用SEM、XRD、EPR、荧光光谱等表征手段,详细探讨了羟基自由基和氢氧离子在MOR分子筛膜合成中的作用。与没有羟基自由基参与的合成体系相比,羟基自由基促进的MOR沸石膜不仅明显缩短了结晶时间,而且降低了反应体系的碱度。在最佳条件下制备的膜在75℃条件下,在90%的乙酸/水混合物中表现出良好的分离性能,渗透通量高达1.37 kg m-2 h-1,渗透物含水量超过99.4 wt %。此外,采用羟基自由基促进策略制备的MOR沸石膜具有良好的再现性。这种羟基自由基促进的方法为在无氟、无模板和低碱度条件下快速制备高性能沸石膜提供了一种高效、环保的途径。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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