局部有序如何导致无序材料的形状选择性:以FAU-FER分子筛间转化中间体为例

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-03-04 DOI:10.1021/acscatal.4c07182
Julia Telles de Souza, Alexandre Ferreira Young, Eduardo F. Sousa-Aguiar, Pedro N. Romano, Javier García-Martínez, João M. A. R. De Almeida
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引用次数: 0

摘要

本研究提出了一系列源自fe - fer相互转化的沸石间转化中间体(ITIs)。这些杂化材料是通过精确控制相互转化过程获得的,具有大介孔和FER拓扑型孔约束,尽管其结构在远距离上无序,但转化率高,形状选择性显著。我们在三个不同的催化测试中展示了这种独特的性能组合。这些结构内部的局部顺序足以产生孔隙限制,这不仅产生了显著的形状选择性,而且通过增加可及性来提高转化。具体来说,与商业铁酸盐相比,其Friedel-Crafts烷基化活性增加了10倍,三异丙苯(TiPBz)裂解活性增加了16倍,甲醇脱水成二甲醚(DME)的活性增加了两倍,同时保持了FER的选择性。这些结果突出了fav - fer i作为高性能催化剂的潜力,它结合了无序结构的可及性和通常与有序沸石相关的选择性,为基于沸石的催化开辟了道路。
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How Local Order Leads to Shape Selectivity in Disordered Materials: The Case of FAU-FER Interzeolite Transformation Intermediates
This study presents a series of Interzeolite Transformation Intermediates (ITIs) derived from FAU-to-FER interconversion. These hybrid materials, obtained through precise control of the interconversion process, exhibit both large mesoporosity and FER topology-type pore confinement, resulting in high conversion and remarkable shape selectivity despite their disordered structure at the long range. We demonstrated this unique combination of properties in three different catalytic tests. The local order within these ITIs is sufficient to create pore confinement, which not only produces remarkable shape selectivity but also enhances conversion by increasing accessibility. Specifically, the ITIs show a 10-fold increase in activity for Friedel–Crafts alkylation, a 16-fold increase in activity for triisopropylbenzene (TiPBz) cracking, and a two-fold increase in methanol dehydration to dimethyl ether (DME) compared to commercial ferrierite all while maintaining the selectivity of FER. These results highlight the potential of FAU-to-FER ITIs as high-performance catalysts that combine the accessibility of disordered structures with the selectivity typically associated with well-ordered zeolites, opening avenues in zeolite-based catalysis.
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来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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