Simulating the Self-Assembly of MOF-5 Using Reactive Force Field (ReaxFF)

In this work, we demonstrate the self-assembly of MOF-5 through molecular dynamics simulations by using the reactive force field (ReaxFF). The reactant flux is the major factor considered in the simulations. It is found that well-ordered tetrahedral MOF-5 structures are formed at relatively low fluxes of MOF-5 building units, i.e., Zn4O metal clusters and 1,4-benzenedicarboxylate ligands. However, when the reactant flux becomes sufficiently high, Zn4O metal clusters and 1,4-benzenedicarboxylate ligands aggregate before incorporating into the growing MOF, resulting in amorphous structures with misaligned bonding between metal clusters and ligands. This work shows the possibility of simulating the self-assembly of MOFs using ReaxFF. It also provides insights into the tuning of the MOF structures during assembly processes.