Publication date: 10th April 2024
Space charge effects at heterojunctions are essential in solid-state ionic devices. A comprehensive understanding of the behavior of charge carriers at contacts is imperative for elucidating the interfacial effects that govern charge storage and electrical transport in energy applications. While considerable studies have investigated the space charge effects in mixed conductors, they are limited to the specific cases without providing a general treatment for various types of heterojunctions comprising mixed conductors. More importantly, the mixed conductors used in energy applications generally involve remarkable stoichiometric variation in the bulk phase. Yet, the fundamental relation of the coupling between bulk and interfacial effects in mixed conductors remains a vital but unclear question.
This contribution develops a generalized treatment describing the behaviors of charge carriers at the junctions composed of mixed conductors. The model considers the defect chemical equilibrium and, more crucially, allows for unifying the bulk and interfacial effects in mixed conductors, providing a comprehensive understanding on the doping and size effects of nanostructured electrodes. The developed model is demonstrated by simulating the interface of electroactive material Ni0.8Mn0.1Co0.1O2 and solid electrolyte Al-doped Li7La3Zr2O12, where the distributions of the charged species are examined to highlight the critical role of interfacial storage and transport processes in solid-state batteries. The findings of this study sheds light on offering a pertinent methodology to investigate the interfacial phenomena on storage, transport, and reaction kinetics in a variety of electrochemical systems.
The work is sponsored by National Science and Technology Council, Taiwan.
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