The most successful and generally applicable MOF used for the CS method is the [((ZnX 2 ) 3 (tpt) 2 • x(solvent)) n ] system, (tpt = 2,4,6-tris(4-pyridyl)-1,3,5-triazine ligand; X = I, Br, Cl). The system has several advantageous properties including large, hydrophobic pores (5 x 8 Å) with electron-deficient binding sites offered by the tpt ligand. The ZnX 2 components and pyridyl protons of the tpt ligands provide hydrogen-bond donor and acceptor sites, respectively, which enables reproducible and long-range ordering of the guests within the MOF pores and absorption of organic and aromatic molecules of a range of sizes. The interpenetrated framework allows for some flexibility and expansion of the pore size to accommodate larger guests. The study of MOFs and host-guest complexes by computational methods is a growing area of research, dominated by studies aiming to model the uptake of gases, drug delivery, and calculation of binding energies and interaction strengths of small molecules in the pores of frameworks by molecular dynamics, Monte Carlo simulations, and DFT methods. There have been fewer studies directed at MOFs containing flexible molecules, and specifically CS structures. There are certain challenges that arise due to the size and complexity of these systems, especially when considering the presence of large guest molecules and solvent(s); however, the development of molecular simulation methods and access to more powerful high performance computing has meant that modelling such systems is more accessible, and has led to an increasing number of MOFs being studied computationally.