Abstract Li–air batteries have potential to be the next generation power sources for various applications, from portable devices to electric vehicles and microgrids, due largely to their significantly higher theoretical energy densities than those of the existing batteries. The commercialization of this technology, however, is hindered by a variety of technical hurdles, including low obtainable capacity, poor energy efficiency, and limited cycle life. Breakthrough to these barriers requires a fundamental understanding of the complex electrochemical and transport behaviors inside the batteries. Mathematical modeling and simulation are imperative in gaining important insight into the mechanisms of these complex phenomena, which is vital to achieving rational designs of better materials for high-performance batteries. In this paper, we present a comprehensive review of the latest advances in modeling and simulation of Li–air batteries and offer our perspectives on new directions of future development. Unlike previous reviews that centered mainly on continuum modeling of non-aqueous Li–air batteries, the present paper focuses on mathematical descriptions of the detailed transport and electrochemical processes in different types of Li–air batteries. We start with a brief introduction to the working principles of Li–air batteries. Then, the governing equations for mass transport and electrochemical reactions in non-aqueous Li–air batteries are formulated, including lithium ion and oxygen transport in the porous air electrode, the formation of solid discharge products, the kinetics of electrode reactions, the evolution of electrode structure, the distribution of active sites, the effect of the side reactions during cycling, the phenomena of the volume change, and the charge process. In addition, the mo\deling and simulations of aqueous and hybrid Li–air batteries are reviewed, highlighting the phenomena that are different from those in the non-aqueous ones. Finally, the challenges facing the modeling and simulation of Li–air batteries are discussed and perspectives for the development of a new generation of Li–air batteries are outlined.

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锂空气电池建模与仿真研究进展

摘要 锂空气电池有潜力成为各种应用的下一代电源，从便携式设备到电动汽车和微电网，主要是因为它们的理论能量密度比现有电池高得多。然而，该技术的商业化受到各种技术障碍的阻碍，包括可用容量低、能源效率低和循环寿命有限。突破这些障碍需要对电池内部复杂的电化学和传输行为有基本的了解。数学建模和仿真对于深入了解这些复杂现象的机制至关重要，这对于为高性能电池合理设计更好的材料至关重要。在本文中，我们全面回顾了锂空气电池建模和仿真的最新进展，并提供了我们对未来发展新方向的看法。与之前的评论主要集中在非水锂空气电池的连续介质建模不同，本文侧重于不同类型锂空气电池中详细传输和电化学过程的数学描述。我们首先简要介绍锂空气电池的工作原理。然后，建立了非水锂空气电池质量传输和电化学反应的控制方程，包括多孔空气电极中锂离子和氧的传输、固体放电产物的形成、电极反应动力学、电极结构，活性位点分布，循环过程中副反应的影响、体积变化现象和充电过程。此外，还回顾了水性和混合锂空气电池的建模和模拟，突出了与非水性电池不同的现象。最后，讨论了锂空气电池建模和仿真面临的挑战，并概述了开发新一代锂空气电池的前景。