Process intensification of catalytic fixed-bed reactors is of vital interest and can be conducted on different length scales, ranging from the molecular scale to the pellet scale to the plant scale. Particle-resolved computational fluid dynamics (CFD) is used to characterize different reactor designs regarding optimized heat transport characteristics on the pellet scale. Packings of cylinders, Raschig rings, four-hole cylinders, and spheres were investigated regarding their impact on bed morphology, fluid dynamics, and heat transport, whereby for the latter particle shape, the influence of macroscopic wall structures on the radial heat transport was also studied. Key performance indicators such as the global heat transfer coefficient and the specific pressure drop were evaluated to compare the thermal performance of the different designs. For plant-scale intensification, effective transport parameters that are needed for simplified pseudo-homogeneous two-dimensional plug flow models were determined from the CFD results, and the accuracy of the simplified modeling approach was judged.

The classical continuum modeling of evaporation in capillary porous media is revisited from pore network simulations of the evaporation process. The computed moisture diffusivity is characterized by a minimum corresponding to the transition between liquid and vapor transport mechanisms confirming previous interpretations. Also the study suggests an explanation for the scattering generally observed in the moisture diffusivity obtained from experimental data. The pore network simulations indicate a noticeable nonlocal equilibrium effect leading to a new interpretation of the vapor pressure‐saturation relationship classically introduced to obtain the one‐equation continuum model of evaporation. The latter should not be understood as a desorption isotherm as classically considered but rather as a signature of a nonlocal equilibrium effect. The main outcome of this study is therefore that nonlocal equilibrium two‐equation model must be considered for improving the continuum modeling of evaporation.

We study the velocity field in the liquid phase during the drying of a porous medium in the capillarity-dominated regime with evaporation from the top surface. A simple mass balance in the continuum framework leads to a linear variation of the filtration velocity across the sample. By contrast, the instantaneous slice-averaged velocity field determined from pore network simulations leads to step velocity profiles. The vertical velocity profile is almost constant near the evaporative top surface and zero close to the bottom of the sample. The relative extent of the two regions with constant velocity is dictated by the position of the most unstable meniscus. It is shown that the continuum and pore network results can be reconciled by averaging the velocity field obtained from the pore network simulations over time. This opens up interesting prospects regarding the transport of dissolved species during drying. Also, the study reveals the existence of an edge effect, which is not taken into account in the classical continuum models of drying.

Activity of ammonia synthesis catalyst in the Haber-Bosch process is studied for the case of feeding the process with intermittent and impurity containing hydrogen stream from water electrolysis. Hydrogen deficiency due to low availability of renewable energy is offset by increased flow rate of nitrogen, argon, or ammonia, leading to off-design operation of the Haber-Bosch process. Catalyst poisoning by ppm levels of water and oxygen is considered as the main deactivation mechanism and is evaluated with a microkinetic model. Simulation results show that catalyst activity changes considerably with feed gas composition, even at exceptionally low water contents below $10ppm$. A decreased hydrogen content always leads to lower poisoning of the catalyst. It is shown that ammonia offers less flexibility to the operation of Haber-Bosch process under fluctuating hydrogen production compared to nitrogen and argon. Transient and significant changes of catalyst activity are expected in electrolysis coupled Haber-Bosch process.