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Direct Atomic-Level Imaging of Zeolites: Oxygen, Sodium in Na-LTA and Iron in Fe-MFI.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-06-16 , DOI: 10.1002/anie.202006122
Alvaro Mayoral 1, 2 , Qing Zhang 1 , Yi Zhou 3 , Pengyu Chen 4 , Yanhang Ma 1 , Taro Monji 5 , Pit Losch 6 , Wolfgang Schmidt 6 , Ferdi Schüth 6 , Hajime Hirao 7 , Jihong Yu 8 , Osamu Terasaki 1, 9
Affiliation  

Zeolites are becoming more versatile in their chemical functions through rational design of their frameworks. Therefore, direct imaging of all atoms at the atomic scale, basic units (Si, Al, and O), heteroatoms in the framework, and extra‐framework cations, is needed. TEM provides local information at the atomic level, but the serious problem of electron‐beam damage needs to be overcome. Herein, all framework atoms, including oxygen and most of the extra‐framework Na cations, are successfully observed in one of the most electron‐beam‐sensitive and lowest framework density zeolites, Na‐LTA. Zeolite performance, for instance in catalysis, is highly dependent on the location of incorporated heteroatoms. Fe single atomic sites in the MFI framework have been imaged for the first time. The approach presented here, combining image analysis, electron diffraction, and DFT calculations, can provide essential structural keys for tuning catalytically active sites at the atomic level.

中文翻译:

沸石的直接原子级成像:氧气,Na-LTA中的钠和Fe-MFI中的铁。

通过合理设计骨架,沸石的化学功能变得越来越通用。因此,需要在原子尺度上直接成像所有原子,基本单元(Si,Al和O),框架中的杂原子以及框架外阳离子。TEM提供了原子级的本地信息,但是需要克服严重的电子束损坏问题。本文中,在最电子束敏感和最低骨架密度的沸石之一Na- LTA中成功观察到了所有骨架原子,包括氧和大多数骨架外Na阳离子。沸石的性能,例如在催化中的性能,高度依赖于结合的杂原子的位置。MFI中的Fe单原子位点框架是第一次成像。此处介绍的方法结合了图像分析,电子衍射和DFT计算,可以为调节原子级催化活性位提供必要的结构关键。
更新日期:2020-06-16
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