Computational NMR investigation of mixed-metal (Al,Sc)-MIL-53 and its phase transitions
Abstract
Compositionally complex metal-organic frameworks (MOFs) have properties that depend on local structure that is often difficult to characterise. In this paper a density functional theory (DFT) computational study of mixed-metal (Al,Sc)-MIL-53, a flexible MOF with several different forms, was used to calculate the relative energetics of these forms and to predict NMR parameters that can be used to evaluate whether solid-state NMR spectroscopy can be used to differentiate, identify and characterise the forms adopted by mixed-metal MOFs of different composition. The NMR parameters can also be correlated with structural features in the different forms, giving fundamental insight into the nature and origin of the interactions that affect nuclear spins. Given the complexity of advanced NMR experiments required, and the potential need for expensive and difficult isotopic enrichment, the computational work is invaluable in predicting which experiments and approaches are likely to give the most information on the disorder, local structure and pore forms of these mixed-metal MOFs.
Citation
Davis , Z H , Borthwick , E A L , Morris , R E & Ashbrook , S E 2023 , ' Computational NMR investigation of mixed-metal (Al,Sc)-MIL-53 and its phase transitions ' , Physical Chemistry Chemical Physics , vol. 25 , no. 39 , pp. 26486-26496 . https://doi.org/10.1039/D3CP04147F
Publication
Physical Chemistry Chemical Physics
Status
Peer reviewed
ISSN
1463-9076Type
Journal article
Description
Funding: The authors would like to thank the ERC (Advanced Grant 787073 ADOR) and the Allan Handsel Postgraduate Research Scholarship for Chemistry for studentship funding for ZHD and EALB, respectively. We also acknowledge support from the Collaborative Computational Project on NMR Crystallography (CCP-NC) funded by EPSRC (EP/T026642/1) and from the UK Materials and Molecular Modelling Hub (Young), which is partially funded by EPSRC (EP/T022213/1, EP/W032260/1 and EP/P020194/1) for which access was obtained via the UKCP consortium and funded by EPSRC (EP/P022561/1).Collections
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