Publication date: 10th April 2024
The prediction of charge carrier chemistry and mixed ion-electron transport phenomena in battery electrodes is crucial for battery electrodes. However, conventional theoretical predictions [1-3] often encounter limitations when applied to realistic electrode architectures, which involve multi-phase composites comprising electroactive materials, solid electrolytes, and electronically conductive carbon. Challenges in predicting charge transport kinetics and carrier chemistry stem from the sophisticate electrode microstructure and the presence of heterointerfaces among constituent materials. To address these challenges, we employ the finite element method to establish a charge transport model capable of characterizing the transport kinetics and carrier chemistry of composite electrodes. Through simulations of electrochemical impedance, we identify electrical and chemical transport phenomena in the composites, interpreting them via the generalized transmission line model. We also underscore the critical roles of heterointerfaces' selectivity and the influence of particle size on the transport process. Furthermore, through visualization of concentration propagation during battery discharging, we elucidate the impacts of ionic and electronic networks, as well as the contact issues between each constituent in the composite electrode. Our work paves the way for understanding and predicting the behavior of mixed ion-electron transport in complex electrochemical systems, while also offering guidelines for rationally designing electrode architectures in batteries.
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