MOR-to-MFI interzeolite transformations: Tuning of paired sites content towards the development of efficient MTH catalyst

IF 4.8 3区材料科学 Q1 CHEMISTRY, APPLIED

Microporous and Mesoporous Materials Pub Date : 2024-10-05 DOI:10.1016/j.micromeso.2024.113364

Daniil V. Bruter , Vladimir S. Pavlov , Irina I. Ivanova

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Abstract

Interzeolite transformation is a rapidly developing method of zeolite synthesis, which allows a precise design of the active site structure. We report on the application of MOR to MFI interzeolite transformation (IZT) for the preparation of MFI zeolite with variable content of paired sites and the elucidation of their role in the MTH reaction. IZT procedure involved hydrothermal treatment of the reaction mixture containing mordenite zeolite as a source of silica and alumina, alkali, TPAOH, TPABr and water. Tuning of paired sites was achieved by variation of the content of water and alkali in the reaction mixture and the application of seeding. The results demonstrate that IZT procedure allows to tune paired sites content within 10–65 % without affecting other characteristics of MFI products, such as Si/Al ratio, crystal size, texture, acid sites type, content and strength, as well as the amount of EFAL species and the distribution of aluminum between channels and intersections of the MFI structure. The evaluation of MOR-to-MFI zeolites with different paired sites content in the MTH reaction pointed to significant effect of paired sites on the stability of catalytic activity with time on stream and on the propylene/ethylene selectivity.

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MOR-MFI沸石间转化：调整配对位点含量以开发高效的 MTH 催化剂

沸石间转化是一种快速发展的沸石合成方法，可以精确设计活性位点结构。我们报告了将 MOR 应用于 MFI 沸石间转化（IZT）以制备配对位点含量可变的 MFI 沸石，并阐明其在 MTH 反应中的作用。IZT 过程包括对含有作为二氧化硅和氧化铝来源的莫来石沸石、碱、TPAOH、TPABr 和水的反应混合物进行水热处理。通过改变反应混合物中水和碱的含量以及播种的应用，实现了配对位点的调整。结果表明，IZT 程序可将配对位点的含量调整在 10-65 % 的范围内，而不会影响 MFI 产品的其他特性，如硅/铝比、晶体尺寸、质地、酸位点类型、含量和强度，以及 EFAL 种类的数量和铝在 MFI 结构的通道和交叉点之间的分布。在 MTH 反应中对具有不同配对位点含量的 MOR 转 MFI 沸石进行的评估表明，配对位点对催化活性随时间流的稳定性以及对丙烯/乙烯选择性有显著影响。

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来源期刊

Microporous and Mesoporous Materials 化学-材料科学：综合

CiteScore

10.70

自引率

5.80%

发文量

649

审稿时长

26 days

期刊介绍： Microporous and Mesoporous Materials covers novel and significant aspects of porous solids classified as either microporous (pore size up to 2 nm) or mesoporous (pore size 2 to 50 nm). The porosity should have a specific impact on the material properties or application. Typical examples are zeolites and zeolite-like materials, pillared materials, clathrasils and clathrates, carbon molecular sieves, ordered mesoporous materials, organic/inorganic porous hybrid materials, or porous metal oxides. Both natural and synthetic porous materials are within the scope of the journal. Topics which are particularly of interest include: All aspects of natural microporous and mesoporous solids The synthesis of crystalline or amorphous porous materials The physico-chemical characterization of microporous and mesoporous solids, especially spectroscopic and microscopic The modification of microporous and mesoporous solids, for example by ion exchange or solid-state reactions All topics related to diffusion of mobile species in the pores of microporous and mesoporous materials Adsorption (and other separation techniques) using microporous or mesoporous adsorbents Catalysis by microporous and mesoporous materials Host/guest interactions Theoretical chemistry and modelling of host/guest interactions All topics related to the application of microporous and mesoporous materials in industrial catalysis, separation technology, environmental protection, electrochemistry, membranes, sensors, optical devices, etc.