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等级孔FAU型分子筛的制备及应用的研究进展

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FAU型分子筛因其独特的孔道结构已成为化学工业中应用最广泛、用量最大的催化剂、催化剂载体及吸附剂之一。然而,FAU型分子筛单一的微孔孔道限制了客体分子的扩散,导致其性能严重下降。相比之下,等级孔FAU型分子筛具有微-介/大孔复合的多级孔道结构,能够促进大分子的扩散、提高活性位点的可接近性,进而改善其吸附和催化性能。目前,等级孔分子筛的制备方法主要包括"自下而上"的直接合成法和"自上而下"的后处理法。本文主要介绍了近年来等级孔X型和Y型分子筛制备方法的研究现状,重点总结了等级孔X型和Y型分子筛在吸附、催化等过程中的应用性能,并对等级孔FAU型分子筛的绿色化制备进行展望。
Research progress in the synthesis and application of hierarchical FAU-type zeolites
FAU-type zeolites are an important class of porous aluminosilicate materials with a 3-dimiensional network of accessible micropores(0.74 nm),which primarily encompass X and Y zeolites.Typically,FAU zeolite with a framework SiO2/Al2O3 molar ratio between 2.0 and 3.0 is called X zeolite,and that is greater than 3.0 is classified as Y zeolite.Due to their distinctive structure and pore characteristics,FAU-type zeolites have emerged as one of the most widely used catalysts,catalyst carriers,and adsorbents in the chemical industry.However,the sole microporous channels of the conventional FAU-type zeolites not only make them difficult for the reactions involving bulky molecules to occur within pore channel,leading to insufficient contact between reactants with active sites of the zeolite,but also restrict the diffusion of product within the zeolite,thus affecting the activity and lifetime of the catalyst.Therefore,the key to improving the performance of FAU-type zeolites lies in alleviating the adverse effects of micropore diffusion on mass transfer.Introducing mesopores and/or macropores into microporous zeolites to construct hierarchical zeolites with a multi-modal pore structure is believed to be a promising approach.This modification not only can preserve the active sites from the microporous structure,but also significantly enhances the diffusion rate of guest molecules within the zeolites.Consequently,researchers have concentrated on the preparation and application of hierarchical zeolites.This article focuses on the current research status on the preparation of hierarchical X and Y zeolites based on"bottom-up"direct synthesis and"top-down"post-treatment methods.The direct synthesis method mainly comprises template and template-free methods.In terms of the template method,the pore structure of FAU zeolites can be tailored by altering the nature of the templating agent,synthesis conditions and so on.Differently,the template-free method enables the preparation of hierarchical FAU zeolites without the addition of any template.In particular,hierarchical X and Y zeolites have been successfully synthesized directly from natural aluminosilicate minerals without the use of organic templates,which not only reduces the synthesis cost of hierarchical zeolites from raw materials,but also contributes to environmental protection.This method provides a novel synthetic pathway for the preparation of hierarchical zeolites in a low-cost and green way.On the other hand,post-treatment method based on desilication and dealumination is the main method for the preparation of hierarchical Y zeolite,whereas few researchers have made use of post-treatment method to introduce meso/macroporous structures into X zeolite because of the poor chemical stability of X zeolite.In addition,the article introduces the application performance of hierarchical X and Y zeolites in adsorption,catalysis as well as other reaction processes.Despite the superior diffusion capabilities of hierarchical FAU-type zeolites,there are several problemsincluding high cost of organic templates and pollution emissions from the removal of template in the process of synthesizing hierarchical zeolites based on template method,limiting the industrial application of this method.As a result,designing cheap and recyclable templates is the key to realizing green and low-cost preparation of hierarchical FAU-type zeolite.Furthermore,post-treatment method cannot achieve the regulation of mesoporous size in hierarchical zeolites.Future research should deeply investigate the structure-activity relationship between the pore structure and reaction performance of hierarchical FAU-type zeolites,so as to further open pore channels,and enhance diffusion,thus promoting the development of hierarchical FAU-type zeolites in industrial applications.

hierarchical FAU-type zeolitesdirect synthesispost treatmentadsorptioncatalysis

董鹏、朱琳、骆龙华、李铁森、王廷海、王婵、崔勍焱、施杰、岳源源

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福州大学化工学院,福州 350108

清源创新实验室,泉州 362801

等级孔FAU型分子筛 直接合成 后处理 吸附 催化

国家自然科学基金

22322803

2024

科学通报
中国科学院国家自然科学基金委员会

科学通报

CSTPCD北大核心
影响因子:1.269
ISSN:0023-074X
年,卷(期):2024.69(19)
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