Mapping nanocrystalline disorder within an amorphous metal-organic framework.
Mapping nanocrystalline disorder within an amorphous metal-organic framework.
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DOI：
10.1038/s42004-023-00891-9
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发表时间：
2023-05-11
影响因子：
5.9
通讯作者：
Collins SM
中科院分区：
文献类型：
--
作者：
Sapnik AF;Sun C;Laulainen JEM;Johnstone DN;Brydson R;Johnson T;Midgley PA;Bennett TD;Collins SM
有意无序的金属有机框架（MOFs）显示出丰富的功能行为。然而，其原子结构的表征仍然具有令人难以置信的挑战性。X射线对分布函数技术在确定它们的平均局部结构方面是关键的，但在很大程度上对结构的空间变化不敏感。Fe-BTC（BTC = 1，3，5-苯三甲酸酯）是一种纳米复合材料MOF，以其催化性能而闻名，包括结晶纳米颗粒和无定形基质。在这里，我们使用扫描电子衍射首先映射的结晶和非晶成分，以评估域的大小，然后进行电子对分布函数分析，以探测空间分离的原子结构的非晶基体。进一步的布拉格散射分析揭示了Fe-BTC纳米晶内的系统取向无序，显示出在单个颗粒上超过10 °的连续晶格旋转。最后，我们确定了晶体成分的候选晶胞。这些独立的结构分析量化了工程复合MOF材料在临界长度尺度下Fe-BTC中的无序。含有非晶和纳米晶相的框架材料的表征具有挑战性，因为它们的平均结构描述符代表性较差，因此通常需要进行微观到纳米级的分析。在这里，扫描电子衍射结合电子对分布函数分析和布拉格散射分析被用来探测金属有机框架Fe-BTC的结构中的空间变化，已知包括结晶纳米颗粒和无定形基质。
Intentionally disordered metal–organic frameworks (MOFs) display rich functional behaviour. However, the characterisation of their atomic structures remains incredibly challenging. X-ray pair distribution function techniques have been pivotal in determining their average local structure but are largely insensitive to spatial variations in the structure. Fe-BTC (BTC = 1,3,5-benzenetricarboxylate) is a nanocomposite MOF, known for its catalytic properties, comprising crystalline nanoparticles and an amorphous matrix. Here, we use scanning electron diffraction to first map the crystalline and amorphous components to evaluate domain size and then to carry out electron pair distribution function analysis to probe the spatially separated atomic structure of the amorphous matrix. Further Bragg scattering analysis reveals systematic orientational disorder within Fe-BTC’s nanocrystallites, showing over 10° of continuous lattice rotation across single particles. Finally, we identify candidate unit cells for the crystalline component. These independent structural analyses quantify disorder in Fe-BTC at the critical length scale for engineering composite MOF materials. Framework materials containing amorphous and nanocrystalline phases are challenging to characterize as they are poorly represented by average structural descriptors, and thus microscopic to nanoscale analysis is often required. Here, scanning electron diffraction combined with electron pair distribution function analysis and Bragg scattering analysis are used to probe spatial variations in the structure of metal–organic framework Fe-BTC, known to comprise crystalline nanoparticles and an amorphous matrix.
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影响因子：
4.3
作者：
Bennett, Thomas D.;Saines, Paul J.;Cheetham, Anthony K.
通讯作者：
Cheetham, Anthony K.
DOI：
10.1098/rspa.1951.0197
发表时间：
1951-01-01
影响因子：
--
作者：
FRANKLIN, RE
通讯作者：
FRANKLIN, RE
影响因子：
8.6
作者：
Bechis, Irene;Sapnik, Adam F.;Tarzia, Andrew;Wolpert, Emma H.;Addicoat, Matthew A.;Keen, David A.;Bennett, Thomas D.;Jelfs, Kim E.
通讯作者：
Jelfs, Kim E.
影响因子：
15
作者：
Ashling, Christopher W.;Johnstone, Duncan N.;Bennett, Thomas D.
通讯作者：
Bennett, Thomas D.
卤化铅钙钛矿和金属有机框架玻璃的液相烧结
影响因子：
56.9
作者：
Hou, Jingwei;Chen, Peng;Bennett, Thomas D.
通讯作者：
Bennett, Thomas D.