Mixed hierarchical local structure in a disordered metal-organic framework.
Mixed hierarchical local structure in a disordered metal-organic framework.
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DOI：
10.1038/s41467-021-22218-9
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发表时间：
2021-04-06
影响因子：
16.6
通讯作者：
Bennett TD
中科院分区：
文献类型：
--
作者：
Sapnik AF;Bechis I;Collins SM;Johnstone DN;Divitini G;Smith AJ;Chater PA;Addicoat MA;Johnson T;Keen DA;Jelfs KE;Bennett TD
无定形金属有机框架（MOFs）是一类新兴的材料。然而，它们的结构表征是一个重大挑战。Fe-BTC和商业等同物Basolite® F300是具有令人难以置信的多种催化能力的MOFs，但它们的无序结构仍然知之甚少。在这里，我们使用先进的电子显微镜，以确定纳米晶结构的Fe-BTC的纳米晶域嵌入在一个非晶基体中，而同步辐射全散射测量揭示了Fe-BTC内的局部原子秩序的程度。我们使用基于聚合的算法来生成Fe-BTC的原子结构，这是该方法应用于充分研究的沸石咪唑酯框架家族之外的无定形MOF领域的第一个例子。这证明了这种计算方法对其他无定形M0 F系统的建模的适用性，其具有对所有M0 F化学和连接性的潜在通用性。我们发现，Fe-BTC和Basolite® F300的结构可以由包含短程和中程有序的混合物的模型表示，Basolite® F300中的中程有序比例大于Fe-BTC。最后，我们讨论我们的方法如何可以允许高通量的计算发现功能，无定形的MOFs。无定形MOFs的结构是具有挑战性的。在这里，作者使用电子显微镜和对分布函数方法，再加上基于聚合的算法来确定Fe-BTC的原子结构，证明了这种计算方法的强大功能。
Amorphous metal–organic frameworks (MOFs) are an emerging class of materials. However, their structural characterisation represents a significant challenge. Fe-BTC, and the commercial equivalent Basolite® F300, are MOFs with incredibly diverse catalytic ability, yet their disordered structures remain poorly understood. Here, we use advanced electron microscopy to identify a nanocomposite structure of Fe-BTC where nanocrystalline domains are embedded within an amorphous matrix, whilst synchrotron total scattering measurements reveal the extent of local atomic order within Fe-BTC. We use a polymerisation-based algorithm to generate an atomistic structure for Fe-BTC, the first example of this methodology applied to the amorphous MOF field outside the well-studied zeolitic imidazolate framework family. This demonstrates the applicability of this computational approach towards the modelling of other amorphous MOF systems with potential generality towards all MOF chemistries and connectivities. We find that the structures of Fe-BTC and Basolite® F300 can be represented by models containing a mixture of short- and medium-range order with a greater proportion of medium-range order in Basolite® F300 than in Fe-BTC. We conclude by discussing how our approach may allow for high-throughput computational discovery of functional, amorphous MOFs. The structures of amorphous MOFs are challenging to characterise. Here the authors use electron microscopy and pair distribution function methods, coupled with a polymerisation-based algorithm to determine the atomic structure of Fe-BTC, demonstrating the power of this computational approach.
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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.
影响因子：
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作者：
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Goodwin, Andrew L.
影响因子：
16.6
作者：
Bennett TD;Tan JC;Yue Y;Baxter E;Ducati C;Terrill NJ;Yeung HH;Zhou Z;Chen W;Henke S;Cheetham AK;Greaves GN
通讯作者：
Greaves GN
影响因子：
3.8
作者：
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通讯作者：
Sanchez-Sanchez, Manuel
影响因子：
8.6
作者：
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通讯作者：
Snurr, Randall Q.