Aluminum distribution and active site locations in the structures of zeolite ZSM-5 catalysts

IF 44.7 1区综合性期刊 Q1 MULTIDISCIPLINARY SCIENCES

Science Pub Date : 2025-04-24 DOI:10.1126/science.ads7290

Przemyslaw Rzepka, Thomas Huthwelker, Jiri Dedecek, Edyta Tabor, Milan Bernauer, Stepan Sklenak, Kinga Mlekodaj, Jeroen A. van Bokhoven

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Abstract

Zeolites have exceptional catalytic performance in oil refining and chemical synthesis that can be attributed to their well-defined porous structures that host active sites. This study pinpoints the exact locations of aluminum atoms in ZSM-5 structures—a key zeolite catalyst. Aluminum siting governs catalytic efficiency in acid and redox processes. Anomalous x-ray powder diffraction (AXRPD) at the aluminum K-edge probes the long-range order of aluminum atoms within the ZSM-5 frameworks, precisely quantifying both isolated aluminum atoms and Al(-O-Si-O-)_xAl sequences (aluminum pairs). Supported by nuclear magnetic resonance studies, AXRPD unambiguously determines the crystallographic organization of aluminum pairs, recognized spectroscopically as α, β, and γ sites, linking their distribution to superior catalytic activity in propene oligomerization. This combined approach provides essential insights for optimizing zeolite catalysts and enhancing their performance.

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ZSM-5沸石催化剂结构中铝的分布及活性位点

沸石在炼油和化学合成中具有特殊的催化性能，这可归因于其具有活性位点的明确的多孔结构。这项研究确定了ZSM-5结构中铝原子的确切位置，这是一种关键的沸石催化剂。铝的定位决定了酸和氧化还原过程的催化效率。在铝k边的异常x射线粉末衍射（AXRPD）探测了ZSM-5框架内铝原子的长程顺序，精确量化了分离的铝原子和Al(- o - si - o -) x Al序列（铝对）。在核磁共振研究的支持下，AXRPD明确地确定了铝对的晶体组织，在光谱上被识别为α、β和γ位点，将它们的分布与丙烯低聚化的优越催化活性联系起来。这种结合的方法为优化沸石催化剂和提高其性能提供了重要的见解。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Science 综合性期刊-综合性期刊

CiteScore

61.10

自引率

0.90%

发文量

审稿时长

2.1 months

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