cm0c01737_si_004.cif (147.84 kB)
Ab Initio Prediction of Metal-Organic Framework Structures
dataset
posted on 2020-06-16, 21:44 authored by James
P. Darby, Mihails Arhangelskis, Athanassios D. Katsenis, Joseph M. Marrett, Tomislav Friščić, Andrew J. MorrisMetal-organic
frameworks (MOFs) have emerged as highly versatile
materials with applications in gas storage and separation, solar light
energy harvesting and photocatalysis. The design of new MOFs, however,
has been hampered by the lack of computational methods for ab initio MOF structure prediction, which could be used
to inspire and direct experimental synthesis. Here, we report the
first ab initio method for the prediction of MOF
structures and test it against a diverse set of known MOFs that were
chosen for their differences in topology, metal coordination geometry,
and ligand binding sites. In all cases, our calculations produced
structures that match experiment using only the target composition
and ligand molecular structure, proving the versatility of our procedure.
The herein presented methodology utilizes the point group symmetry
of ligands to enable, for the first time, prediction of MOF structures
from first principles, without having to resort to empirical guidelines
based on rigid connectivity of nodes and linkers, or to previously
determined crystal structures and topologies of known MOFs. This advance
provides the first tool to change MOF design from an empirically based
process that is based on chemistʼs intuition rooted in literature-
or database-established knowledge of node-and-linker connectivity
to a more general and theory-driven materials development. This ab initio MOF structure prediction approach, which is here
validated on a range of known MOF classes, provides a unique opportunity
to explore the phase landscape of MOFs computationally and enables
MOF research and development even in case of limited access to laboratory
resources, as for example in case of a global pandemic.
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ab initio methodchemist ʼs intuitiontheory-driven materials developmentlight energy harvestingMOF structuresMetal-Organic Framework Structures Metal-organic frameworksab initio MOF structure prediction approachpoint group symmetryAb Initio Predictionchange MOF designmetal coordination geometryab initio MOF structure predictionligand binding sites