Mixed hierarchical local structure in a disordered metal–organic framework

Sapnik, AF, Bechis, I, Collins, SM, Johnstone, DN, Divitini, G, Smith, AJ, Chater, PA, Addicoat, MA ORCID: https://orcid.org/0000-0002-5406-7927, Johnson, T, Keen, DA, Jelfs, KE and Bennett, TD, 2021. Mixed hierarchical local structure in a disordered metal–organic framework. Nature Communications, 12: 2062. ISSN 2041-1723

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Abstract

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.

Item Type:	Journal article
Publication Title:	Nature Communications
Creators:	Sapnik, A.F., Bechis, I., Collins, S.M., Johnstone, D.N., Divitini, G., Smith, A.J., Chater, P.A., Addicoat, M.A., Johnson, T., Keen, D.A., Jelfs, K.E. and Bennett, T.D.
Publisher:	Springer Science and Business Media LLC
Date:	6 April 2021
Volume:	12
ISSN:	2041-1723
Identifiers:	Number Type 10.1038/s41467-021-22218-9 DOI 1430151 Other
Rights:	© The Author(s) 2021 This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
Divisions:	Schools > School of Science and Technology
Record created by:	Jeremy Silvester
Date Added:	09 Apr 2021 09:28
Last Modified:	31 May 2021 15:04
URI:	https://irep.ntu.ac.uk/id/eprint/42678

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