Carbon dioxide (CO2) sequestration in the sub-surface is a potential mitigation technique for global climate change caused by greenhouse gas emissions. In order to evaluate the feasibility of this technique, understanding the behaviour of CO2 stored in geological rock formations over a range of length- and time-scales is crucial. The work presented in this dissertation contributes to the knowledge in this field by investigating the two-phase flow and entrapment processes of CO2, as well as other relevant fluids, in porous media at the pore- and centimetre-scales using a combination of lab-based nuclear magnetic resonance (NMR) experimental techniques and lattice Boltzmann (LB) numerical simulation techniques.

Pulsed field gradient (PFG) NMR techniques were used to acquire displacement distributions (propagators) of brine flow through a model porous medium (100 µm glass bead packing) before and after the capillary (residual) trapping of gas-phase CO2 in the pore space. The acquired propagators were compared quantitatively with the corresponding LB simulations. In addition, magnetic resonance imaging (MRI) techniques were used to characterise the extent of CO2 trapping in the bead pack. The acquired NMR propagators were compared to LB simulations applied to various CO2 entrapment scenarios in order to investigate the pore morphology in which CO2 becomes entrapped. Subsequently, MRI drop shape analysis techniques were used to identify a pair of analogue fluids which matched certain key physical properties (specifically interfacial tension) of the supercritical CO2/water system in order to extend the work to conditions more relevant to CO2 sequestration in the sub-surface, where CO2 is likely to be present in the supercritical phase. As before, NMR propagator measurements and MRI techniques, along with LB simulations, were used to characterise the capillary trapping of the CO2 analogue phase in glass bead packs, as well as two different types of rock core plugs – relatively homogeneous Bentheimer sandstone, and heterogeneous Portland carbonate.

In addition to capillary trapping, the effect of vertical permeability heterogeneity, such as is often present in underground rock formations, was investigated for the flow of miscible (water/brine) gravity currents in model porous media (glass bead packs), using MRI techniques such as 2D spin-echo imaging and phase-shift velocity imaging. Finally, a preliminary investigation was made into the effect of particle- and pore-size distributions on the gas/liquid (air/water) interface for porous media consisting of glass bead and sand packs of different average particle size using quantitative MRI techniques.