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Multi-phase management is crucial for performance and durability of electrochemical cells such as batteries and fuel cells. In this paper we present a generic framework for describing the two-dimensional spatiotemporal evolution of gaseous, liquid and solid phases, as well as their interdependence with interfacial (electro-)chemistry and microstructure in a continuum description. The modeling domain consists of up to seven layers (current collectors, channels, electrodes, separator/membrane), each of which can consist of an arbitrary number of bulk phases (gas, liquid, solid) and connecting interfaces (two-phase or multi-phase boundaries). Bulk and interfacial chemistry is described using global or elementary kinetic reactions. Multi-phase management is coupled to chemistry and to mass and charge transport within bulk phases. The functionality and flexibility of this framework is demonstrated using four application areas in the context of post-lithium-ion batteries and fuel cells, that is, lithium-sulfur (Li-S) cells, lithium-oxygen (Li-O) cells, solid oxide fuel cells (SOFC) and polymer electrolyte membrane fuel cells (PEFC). The results are compared to models available in literature and properties of the generic framework are discussed.
In this paper we present a model of the discharge of a lithium–oxygen battery with aqueous electrolyte. Lithium–oxygen batteries (Li–O2) have recently received great attention due to their large theoretical specific energy. Advantages of the aqueous design include the stability of the electrolyte, the long experience with gas diffusion electrodes (GDEs), and the solubility of the reaction product lithium hydroxide. However, competitive specific energies can only be obtained if the product is allowed to precipitate. Here we present a dynamic one-dimensional model of a Li–O2 battery including a GDE and precipitation of lithium hydroxide. The model is parameterized using experimental data from the literature. We demonstrate that GDEs remove power limitations due to slow oxygen transport in solutions and that lithium hydroxide tends to precipitate on the anode side. We discuss the system architecture to engineer where nucleation and growth predominantly occurs and to optimize for discharge capacity.