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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.
The durability of polymer electrolyte membrane fuel cells (PEMFC) is governed by a nonlinear coupling between system demand, component behavior, and physicochemical degradation mechanisms, occurring on timescales from the sub-second to the thousand-hour. We present a simulation methodology for assessing performance and durability of a PEMFC under automotive driving cycles. The simulation framework consists of (a) a fuel cell car model converting velocity to cell power demand, (b) a 2D multiphysics cell model, (c) a flexible degradation library template that can accommodate physically-based component-wise degradation mechanisms, and (d) a time-upscaling methodology for extrapolating degradation during a representative load cycle to multiple cycles. The computational framework describes three different time scales, (1) sub-second timescale of electrochemistry, (2) minute-timescale of driving cycles, and (3) thousand-hour-timescale of cell ageing. We demonstrate an exemplary PEMFC durability analysis due to membrane degradation under a highly transient loading of the New European Driving Cycle (NEDC).
The DMFC is a promising option for backup power systems and for the power supply of portable devices. However, from the modeling point of view liquid-feed DMFC are challenging systems due to the complex electrochemistry, the inherent two-phase transport and the effect of methanol crossover. In this paper we present a physical 1D cell model to describe the relevant processes for DMFC performance ranging from electrochemistry on the surface of the catalyst up to transport on the cell level. A two-phase flow model is implemented describing the transport in gas diffusion layer and catalyst layer at the anode side. Electrochemistry is described by elementary steps for the reactions occurring at anode and cathode, including adsorbed intermediate species on the platinum and ruthenium surfaces. Furthermore, a detailed membrane model including methanol crossover is employed. The model is validated using polarization curves, methanol crossover measurements and impedance spectra. It permits to analyze both steady-state and transient behavior with a high level of predictive capabilities. Steady-state simulations are used to investigate the open circuit voltage as well as the overpotentials of anode, cathode and electrolyte. Finally, the transient behavior after current interruption is studied in detail.
Seven cell design concepts for aqueous (alkaline) lithium–oxygen batteries are investigated using a multi-physics continuum model for predicting cell behavior and performance in terms of the specific energy and specific power. Two different silver-based cathode designs (a gas diffusion electrode and a flooded cathode) and three different separator designs (a porous separator, a stirred separator chamber, and a redox-flow separator) are compared. Cathode and separator thicknesses are varied over a wide range (50 μm–20 mm) in order to identify optimum configurations. All designs show a considerable capacity-rate effect due to spatiotemporally inhomogeneous precipitation of solid discharge product LiOH·H2O. In addition, a cell design with flooded cathode and redox-flow separator including oxygen uptake within the external tank is suggested. For this design, the model predicts specific power up to 33 W/kg and specific energy up to 570 Wh/kg (gravimetric values of discharged cell including all cell components and catholyte except housing and piping).
Cell lifetime diagnostics and system be-havior of stationary LFP/graphite lithium-ion batteries
(2018)
Lithium-oxygen cells with organic electrolyte suffer high overpotentials during charge, indicating asymmetric charge/discharge reaction mechanisms. We present a multi-physics dynamic modeling and simulation study of the Li/O2 cell cycling behavior. We present three different multi-step mechanisms of the 2 Li + O2 ⇄ Li2O2 cell reaction, (A) a reversible 5-step mechanism, (B) a partially irreversible 6-step mechanism, and (C) a partially irreversible 8-step mechanism that includes reactions of a redox mediator. Model predictions are compared to experimental galvanostatic cycling data of Swagelok cells without and with 2,2,6,6-tetramethylpiperidinyloxyl (TEMPO) as redox mediator. All mechanisms are able to predict the discharge behavior in good agreement to the experimental results. The experimentally observed high charge overpotentials as well as their reduction by using a redox mediator can be qualitatively reproduced with the irreversible reaction mechanisms. However, the particular shape of the experimental charge curve with continuously increasing charge overpotential cannot be reproduced with the present mechanisms.
Mass transfer phenomena in membrane fuel cells are complex and diversified because of the presence of complex transport pathways including porous media of very different pore sizes and possible formation of liquid water. Electrochemical impedance spectroscopy, although allowing valuable information on ohmic phenomena, charge transfer and mass transfer phenomena, may nevertheless appear insufficient below 1 Hz. Use of another variable, that is, back pressure, as an excitation variable for electrochemical pressure impedance spectroscopy is shown here a promising tool for investigations and diagnosis of fuel cells.
The lifetime and performance of solid-oxide fuel cells (SOFC) and electrolyzer cells (SOEC) can be significantly degraded by oxidation of nickel within the electrode and support structures. This paper documents a detailed computational model describing nickel oxide (NiO) formation as a growing film layer on top of the nickel phase in Ni/YSZ composite electrodes. The model assumes that the oxidation rate is controlled by transport of ions across the film (Wagner's theory). The computational model, which is implemented in a two-dimensional continuum framework, facilitates the investigation of alternative chemical reaction and transport mechanisms. Model predictions agree well with a literature experimental measurement of oxidation-layer growth. In addition to providing insight in interpreting experimental observations, the model provides a quantitative predictive capability for improving electrode design and controlling operating conditions.