CFD modelling of a membrane reactor for hydrogen production from ammonia

Despite the growing use of hydrogen (H2) as a transport fuel, one of the major barriers still remaining is efficient and inexpensive fuel distribution and storage. Current approaches, such as compression, liquefaction or metal hydride formation, incur a significant energy penalty. Ammonia (NH3) has long been considered a prospective H2 medium, exhibiting a higher volumetric H2 density than liquid H2, through liquid-phase storage at mild pressure. Decomposition of NH3 into H2 and N2 can be achieved via use of catalytic reactors and fuel-cell-grade H2 can be produced using metal membranes at H2 distribution sites.In this study, a 3-Dimensional (3D) Computational Fluid Dynamics (CFD) model has been developed to understand the performance of the H2 separation process in gas mixtures derived from an NH3-cracking reaction. The reactor consists of 19 tubular membrane tubes, each 470 mm long, inside a tubular shell with an inner diameter of 130 mm. Standard transport and energy equations governing a 3D, pressure-based, steady-state model were derived from the laws of conservation of mass, momentum and energy. The governing equations were solved using commercial CFD software ANSYS Fluent 18.0. Gas flow and mixing were modelled by the two-equation standard k-epsilon model for closure. Coupled solver was used for pressure-velocity coupling, enabling a pseudo-transient option with pseudo time steps of 0.01 s. To estimate H2 permeation through the metal membrane, a constant H2 permeability of 3.0E–07 mol.m−1 s−1 Pa−0.5 derived from series of experiments tested under a range of industrial conditions, was used. Model simulations were conducted for an adiabatic temperature of 300 °C, a feed-side pressure of 7.8 bara and a permeate side pressure of 0.1 bara. A parametric analysis was carried out to explore the effects of variation in total feed-gas flow and effects of changes in NH3-cracking efficiency on H2 production rates and H2 yields. The model estimated that 4.6–11.6 kg H2/day can be produced from a 30-70 L min−1 NH3 inlet flow with 80-90% NH3-cracking efficiency. At lower NH3 inlet flow rates, higher H2 yields can be obtained within a shorter distance of the membrane tubes due to relatively slower velocities and longer residence times. At high inlet flow rates, H2 yields were significantly lower due to their faster velocities and shorter resident times, but high yields (>95%) were still observed at the membrane reactor outlet. A sensitivity analysis of the model showed that even if metal membranes functioned at only 50% of the maximum permeability, a high H2 yield similar to that estimated using 100% permeability can still be achieved at the H2 outlets.