Ammonia is essential for global food production as a component of fertiliser, and a potential energy carrier in the energy transition. Electrochemical ammonia synthesis faces numerous challenges as an alternative to the carbon intensive Haber-Bosch process, including competition from hydrogen evolution, and mass transport limitations. An unconventional cell design with a hydrogen permeable electrode could help to address these problems. The reaction mechanism and performance of ammonia synthesis using hydrogen permeable electrodes was investigated at elevated temperatures and pressures of up to 120 °C and 8 bar. Furthermore, a facile method for enhancing the electrochemical surface area of the electrode was developed and tested. Operation at elevated pressure resulted in a moderate increase in cell performance. However, replenishment of the nitrogen vacancies in the nickel nitride catalyst through dinitrogen adsorption is identified as the elementary step that limits activity and stability. The amount of pre-deposited N is found to significantly influence the ammonia production rate and its stability. Dynamics of ammonia desorption could also play a role in nitride regeneration. In future studies, the presence of a decomposition reaction of the nitride should be investigated. Usage of more stable nitride species or a combination of host nitride and dopants is recommended to improve stability and simultaneously promote dinitrogen activation and hydrogenation to ammonia. These findings expand the understanding of the mechanisms underlying the nitrogen reduction reaction, paving the way for the development of a more efficient green ammonia synthesis process.

The ongoing worldwide energy transition has prompted significant scientific interest in energy storage. Rechargeable lithium-ion batteries have become a standard for energy storage in mobile devices and electric vehicles for their mass-energy density. While industry standard lithium-ion cells are currently based on liquid electrolytes, solid electrolytes promise to bring the next step towards safety, energy density and sustainability. However, there are critical challenges, notably improving the lithium conduction of solid electrolytes. Furthermore, as a relatively new research field it is important to target high recyclability and sustainability for materials early on. Battery modelling facilitates performance comparisons of for example battery materials and geometric properties, and subsequent optimisation. The report treats battery modelling with a specific focus on solid electrolytes. Two solid electrolyte models, based on weak electrolyte theory and a lattice gas model by Landstorfer et al., were implemented in the Multiphase Porous Electrode Theory software (Smith,2017). The former is relevant for glass type electrolytes, while the latter models crystalline materials. The models showed comparable performance, with a constant voltage offset but good mutual agreement in term of behaviour. It is important to verify the results experimentally. The numerical methods used in porous electrode theory were treated with the creation of a standalone porous electrode model, with separate domains for the electrolyte and active cathode particles. This model is stable and functional with the two domains in isolation, while a fault remains in the coupling between the domains. Lastly, a proposal is made for the addition of interface regions in the MPET software. With these domains situated between the bulk electrolyte and active cathode particles, porous electrode models could include a variety of phenomena that are currently impossible to implement. For solid electrolytes in particular, modelling dynamic stress effects and lithium conduction across particle boundaries would be valuable additions.