Quantifying tortuosity in porous Li-ion battery materials

An accurate assessment of liquid-phase mass transport resistances is necessary for understanding and optimizing battery performance using mathematical models. This work combines modeling and experiments to quantify tortuosity in electrolyte-filled porous battery structures (separator and active-material film). Tortuosities of separators were measured by two methods, AC impedance and polarization-interrupt, which produced consistent results. We measured an apparent interfacial resistance at the lithium metal electrodes that contributed to both ohmic and diffusional resistance of the cell. The polarization-interrupt experiment was used similarly to measure effective electrolyte transport in porous films of cathode materials, particularly films containing LiFePO₄. An empirical relationship between porosity and the tortuosity of the porous structures was developed. Our results demonstrate that the tortuosity-dependent mass transport resistance in porous separators and electrodes is significantly higher than that predicted by the oft-used Bruggeman relationship.