In order to improve clarity of assignments and provide a more complete picture of dynamic behaviour, variable temperature NMR experiments were attempted. However, the complex system within the NMR rotor for CO 2 capture materials -including chemisorbed, physisorbed and free head-space gaseous CO 2 -presents a multi-component equilibrium system that is itself affected by temperature changes. This resulted (Fig. ) in alterations of the NMR spectrum that are not simply due to dynamic effects but also driven by shifts in equilibrium position with temperature (e.g. increased CO 2 (g) adsorption with decreasing temperature). This experimental limitation further justified MLFF-MD modelling as a crucial tool for providing insight into the effects of dynamics in the NMR spectroscopy of CO 2 capture systems.