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金光与暗影——β沸石入门

Lights and Shadows of Gold Introduction into Beta Zeolite.

机构信息

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

出版信息

Molecules. 2020 Dec 8;25(24):5781. doi: 10.3390/molecules25245781.

Abstract

Four different methods for gold deposition on Beta zeolite, namely impregnation, ion-exchange, deposition-reduction, and grafting on (3-aminopropyl)trimethoxysilane functionalized support, were applied to investigate their influence on textural/structural changes in the zeolite support and its surface acidity. The as-prepared materials were fully characterized by XRD, N physisorption, ICP-OES, XPS, TEM, and pyridine adsorption. The obtained results indicated that bifunctional redox-acidic materials prepared within this work were characterized not only by different gold loading and gold particle size, but also different textural parameters and acidity. All these features were strongly affected by the procedure applied for gold deposition. The introduction of Au into Beta zeolite by ion exchange caused a significant decrease in the Si/Al ratio in the zeolite framework. The size of Au particles determined the textural parameters of the zeolite and the number of Lewis acid sites (LAS). The Brønsted acid sites (BAS) number was decreased if (3-aminopropyl)trimethoxysilane or NaBH were used in the procedure of gold deposition. The highest BAS/LAS ratio was achieved for the sample prepared by ion exchange in the ammonium form of Beta zeolite. The presented results permit making a proper choice of the gold modification procedure for the preparation of bifunctional (redox-acidic) materials, addressed to a desired application.

摘要

四种不同的方法被应用于将金沉积到 Beta 沸石上,包括浸渍、离子交换、沉积-还原和接枝到(3-氨丙基)三甲氧基硅烷功能化的载体上,以研究它们对沸石载体的结构和表面酸度的影响。所制备的材料通过 XRD、N 物理吸附、ICP-OES、XPS、TEM 和吡啶吸附进行了充分的表征。结果表明,在这项工作中制备的双功能氧化-酸性材料不仅具有不同的金负载量和金颗粒尺寸,而且具有不同的结构参数和酸度。所有这些特征都强烈受到金沉积程序的影响。通过离子交换将 Au 引入 Beta 沸石中会导致沸石骨架中的 Si/Al 比显著降低。Au 颗粒的大小决定了沸石的结构参数和路易斯酸位(LAS)的数量。如果在金沉积过程中使用(3-氨丙基)三甲氧基硅烷或 NaBH,则Brønsted 酸位(BAS)的数量会减少。在铵形式的 Beta 沸石中通过离子交换制备的样品具有最高的 BAS/LAS 比。所呈现的结果允许为制备针对特定应用的双功能(氧化-酸性)材料选择适当的金修饰程序。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/2747/7762595/e92ef22f96e3/molecules-25-05781-g001.jpg

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