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Electrochemical impedance spectroscopy (EIS) is a widely-used diagnostic technique to characterize electrochemical processes. It is based on the dynamic analysis of two electrical observables, that is, current and voltage. Electrochemical cells with gaseous reactants or products (e.g., fuel cells, metal/air cells, electrolyzers) offer an additional observable, that is, the gas pressure. The dynamic coupling of current and/or voltage with gas pressure gives rise to a number of additional impedance definitions, for which we have introduced the term electrochemical pressure impedance spectroscopy (EPIS) [1,2]. EPIS shows a particular sensitivity towards transport processes of gas-phase or dissolved species, in particular, diffusion coefficients and transport pathway lengths. It is as such complementary to standard EIS, which is mainly sensitive towards electrochemical processes. This sensitivity can be exploited for model parameterization and validation. A general analysis of EPIS is presented, which shows the necessity of model-based interpretation of the complex EPIS shapes in the Nyquist plot (cf. Figure). We then present EPIS simulations for two different electrochemical cells: (1) a sodium/oxygen battery cell and (2) a hydrogen/air fuel cell. We use 1D or 2D electrochemical and transport models to simulate current excitation/pressure detection or pressure excitation/voltage detection. The results are compared to first EPIS experimental data available in literature [2,3].
Practical bottlenecks associated with commercialization of Lithium-air cells include capacity limitation and low cycling efficiency. The origin of such losses can be traced to complex electrochemical side reactions and reactant mass transport losses[1]. The efforts to minimize such losses include exploration of various electrolytes with additives[2], and cell component geometry and material design. Given the wide range of options for such materials, it is almost impractical to experimentally setup and characterize all those cells. Consequently, modeling and simulation studies are efficient alternatives to analyze spatially and temporally resolved cell behavior for various combinations of materials[3]. In this study, with the help of a two-dimensional multi physics model, we have focused on the effect of electrode and electrolyte interaction (electrochemistry), choice of electrolyte (species transport), and electrode geometry (electrode design) on the performance of a lithium-air button cell. Figure1a shows the schematics of the 2D axisymmetric computational domain. A comparative analysis of five different electrolytes was performed while focusing on the 2D distribution of local current density and the concentration of electro-chemically active species in the cell, that is, O2and Li+. Using two different cathode configurations, namely, flooded electrode and gas diffusion electrode (GDE)[4] at different cathode thickness, the effect of cell geometry and electrolyte saturation on cell performance was explored. Further, a detailed discussion on electrode volume utilization (cf. Figure1b) is presented via changes in the active volume of cathode that produces 90% of the total current with the cell current density for different combinations of electrolyte saturations and cathode thickness.