Experimentally-validated ab initio crystal structure prediction of novel metal-organic framework materials

28 June 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


First-principles crystal structure prediction (CSP) is the most powerful approach for materials discovery, enabling the prediction and evaluation of properties of new solid phases based only on a diagram of their underlying components. Here, we present the first CSP-based discovery of metal-organic frameworks (MOFs), offering a broader alternative to conventional techniques which rely on geometry, intuition and experimental screening. Phase landscapes were calculated for three systems involving flexible Cu(II) nodes, which could adopt a potentially limitless number of network topologies and are not amenable to conventional MOF design. The CSP procedure was validated experimentally, through synthesis of materials whose structures perfectly matched those found among the lowest energy calculated structures, and whose relevant properties, such as combustion energies, could immediately be evaluated from CSP-derived structures.


crystal structure prediction
metal-organic frameworks
ab initio materials design

Supplementary materials

Supplementary information for: Experimentally-validated ab initio crystal structure prediction of novel metal-organic framework materials
Details of the computational and experimental methods; energies and crystallographic parameters of the predicted structures; crystallographic data of experimentally-determined strucutres; powder X-ray diffraction patterns; DSC and TGA measurements; SEM measurements


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