Model-Based Performance Evaluation of Hybrid Solid-State Batteries: Impact of Laser-Ablated Geometrical Structures

Abstract

Due to challenges in manufacturing composite cathodes with oxide solid electrolytes, new cell concepts are emerging in which the infiltration of solid-polymer electrolyte (SPE) into 3D cathode pore structures improves capacity retention and cycling stability. However, the performance limitation and the resulting practical relevance of such a hybrid concept have not yet been analyzed and discussed. This study investigates the impact of laser-ablated geometric structures on the performance of hybrid solid-state batteries (SSBs). A Doyle–Fuller–Newman modeling approach is developed and parameterized for structured hybrid SSBs that incorporate a PEO/LiTFSI SPE and an LLZO ceramic separator, as well as NMC-811 and Li-metal for the positive- and negative-electrode active materials. Comparison between structured and planar cell designs reveals significant rate capability improvements in structured designs due to reduced diffusion and interfacial charge transfer polarization. A sensitivity analysis of geometric structure parameters shows further potential for performance improvement in terms of specific capacity and energy density. However, current constriction effects in the LLZO separator can deteriorate the rate capability. A more general perspective is then taken by analyzing the impact of changing SPE parameters. An energy density of 128 Wh kg−1 at 1C, and 220 Wh kg−1 at 1C with improved SPE parameters is achieved in the best case, approaching the target of 250 Wh kg−1 , which is currently achieved for conventional Li-ion batteries.