Nat Comput Sci. 2021 Mar;1(3):212-220. doi: 10.1038/s43588-021-00041-y. Epub 2021 Mar 25.
ABSTRACT
Models of the electrical double layer (EDL) at electrode/liquid-electrolyte interfaces no longer hold for all-solid-state electrochemistry. Here we show a more general model for the EDL at a solid-state electrochemical interface based on the Poisson-Fermi-Dirac equation. By combining this model with density functional theory predictions, the interconnected electronic and ionic degrees of freedom in all-solid-state batteries, including the electronic band bending and defect concentration variation in the space-charge layer, are captured self-consistently. Along with a general mathematical solution, the EDL structure is presented in various materials that are thermodynamically stable in contact with a lithium metal anode: the solid electrolyte Li7La3Zr2O12 (LLZO) and the solid interlayer materials LiF, Li2O and Li2CO3. The model further allows design of the optimum interlayer thicknesses to minimize the electrostatic barrier for lithium ion transport at relevant solid-state battery interfaces.
PMID:38183191 | DOI:10.1038/s43588-021-00041-y
