Hyperpolarised xenon MRI and time-resolved X-ray computed tomography studies of structure-transport relationships in hierarchical porous media

•Xenon-129 MRI studies of gas permeation through walls in catalysed diesel particulate filter (DPF) monoliths.•Time-resolved X-ray Computerised Tomography studies of migration of liquid ganglia and menisci during drying of monoliths.•Determination of the contributions from different levels in the hierarchy of porosity to mass transport flux.•Assessment of accessibility, to through gas flow, of catalytically-active sites. Catalysed diesel particulate filter (DPF) monoliths are hierarchical porous solids, as demonstrated by mercury porosimetry. Establishing structure-transport relationships, including assessing the general accessibility of the catalyst, is challenging, and, thus, a comprehensive approach is necessary. Contributions, from each porosity level, to transport have been established using hyperpolarised (hp) xenon-129 magnetic resonance imaging (MRI) of gas dispersion within DPF monoliths at variable water saturation, since X-ray Computerised-Tomography, and 1H and 2H NMR methods, have shown that porosity levels dry out progressively. At high saturation, hp 129Xe MRI showed gas transport between the channels of the monolith is predominantly taking place at channel wall intersections with high macroporosity. The walls themselves make a relatively small contribution to through transport due to the distribution of the micro-/meso-porous washcoat layer away from intersections. Only at low saturation, when the smallest pores are opened, do hp 129Xe MR images became strongly affected by relaxation. This observation indicates accessibility of paramagnetic (catalytic) centres for gases arises only once the smallest pores are open.