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Mixed hierarchical local structure in a disordered metal–organic framework

DOI: 10.1038/s41467-021-22218-9 DOI Help

Authors: Adam F. Sapnik (University of Cambridge) , Irene Bechis (Imperial College London) , Sean M. Collins (University of Cambridge; University of Leeds) , Duncan N. Johnstone (University of Cambridge) , Giorgio Divitini (University of Cambridge) , Andrew J. Smith (Diamond Light Source) , Philip A. Chater (Diamond Light Source) , Matthew A. Addicoat (Nottingham Trent University) , Timothy Johnson (Johnson Matthey Technology Centre) , David A. Keen (Rutherford Appleton Laboratory) , Kim E. Jelfs (Imperial College London) , Thomas D. Bennett (University of Cambridge)
Co-authored by industrial partner: Yes

Type: Journal Paper
Journal: Nature Communications , VOL 12

State: Published (Approved)
Published: April 2021
Diamond Proposal Number(s): 20038 , 24563

Open Access Open Access

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.

Journal Keywords: Atomistic models; Metal–organic frameworks

Subject Areas: Materials, Chemistry

Diamond Offline Facilities: Electron Physical Sciences Imaging Centre (ePSIC)
Instruments: E02-JEM ARM 300CF , I15-1-X-ray Pair Distribution Function (XPDF) , I22-Small angle scattering & Diffraction


Discipline Tags:

Material Sciences Metallurgy Metal-Organic Frameworks Chemistry

Technical Tags:

Microscopy Scattering Electron Microscopy (EM) Small Angle X-ray Scattering (SAXS) Total Scattering Wide Angle X-ray Scattering (WAXS) Transmission Electron Microscopy (TEM)