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通过后合成处理对分级β沸石进行合理设计及其应用

Rational Design of Hierarchical Beta Zeolites via Post-Synthesis Treatments and Their Applications.

作者信息

Zieliński Michał, Matysiak Natalia, Janiszewska Ewa

机构信息

Faculty of Chemistry, Adam Mickiewicz University, Uniwersytetu Poznańskiego 8, 61-614 Poznań, Poland.

出版信息

Molecules. 2025 Feb 24;30(5):1030. doi: 10.3390/molecules30051030.

Abstract

Hierarchical zeolites with micro- and mesoporous frameworks can overcome diffusional limitations of microporous systems. This study investigates the post-synthetic modification of Beta zeolite using different porogeneous agents (NaOH, NHOH, NHF) under identical conditions to compare their efficiency in generating mesopores. The effect of treatment time was also examined for NHOH and NHF. The modified materials were characterized using physicochemical techniques and evaluated for catalytic performance in acetic acid esterification with alcohols of different sizes and adsorption of methylene blue. All the modifications increased mesoporosity but reduced acidity. NaOH produced the highest mesoporosity but significantly reduced acidity, while NHF retained the most acidity. Catalytic activity in esterification with methanol depended on acidity, but for larger alcohols (n-butanol, benzyl alcohol), activity was influenced by both acidity and mesoporosity. The NHOH- and NHF-modified materials, with lower mesoporosity but higher acidity, exhibited better performance with larger alcohols. In MB adsorption, the adsorption equilibrium rates increased with mesoporosity. The NaOH-modified sample reached equilibrium the fastest due to its superior mesoporosity, while the NHF-modified sample demonstrated the highest adsorption efficiency owing to its abundant Brønsted acid sites. These findings demonstrate that the choice of modifier affects mesoporosity, acidity, and functional performance, offering insights into tailoring hierarchical zeolites for specific applications.

摘要

具有微孔和介孔框架的分级沸石可以克服微孔系统的扩散限制。本研究调查了在相同条件下使用不同的造孔剂(NaOH、NHOH、NHF)对Beta沸石进行合成后改性,以比较它们产生介孔的效率。还考察了NHOH和NHF的处理时间的影响。使用物理化学技术对改性材料进行了表征,并评估了其在与不同尺寸的醇进行乙酸酯化反应中的催化性能以及对亚甲基蓝的吸附性能。所有改性都增加了介孔率,但降低了酸度。NaOH产生的介孔率最高,但显著降低了酸度,而NHF保留的酸度最多。与甲醇酯化反应的催化活性取决于酸度,但对于较大的醇(正丁醇、苯甲醇),活性受酸度和介孔率两者的影响。具有较低介孔率但较高酸度的NHOH和NHF改性材料在与较大醇反应时表现出更好的性能。在亚甲基蓝吸附中,吸附平衡速率随介孔率增加而增加。由于其优异的介孔率,NaOH改性样品达到平衡最快,而NHF改性样品由于其丰富的布朗斯台德酸位点而表现出最高的吸附效率。这些发现表明,改性剂的选择会影响介孔率、酸度和功能性能,为针对特定应用定制分级沸石提供了见解。

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