Abstract
Li-air batteries have attracted interest as energy storage devices due to their high energy and power density. Li-air batteries are expected to revolutionize the automobile industry (for use in electric and hybrid vehicles) and electrochemical energy storage systems by surpassing the energy capacities of conventional Li-ion batteries. However, the practical implementation of Li-air batteries is still hindered by many challenges, such as low cyclic performance and high charging voltage, resulting from oxygen transport limitations, electrolyte degradation, and the formation of irreversible reduction products. Therefore, various methodologies have been attempted to mitigate the issues causing performance degradation of Li-air batteries. Among myriad studies, theoretical and numerical modeling are powerful tools for describing and investigating the chemical reactions, reactive ion transportation, and electrical performance of batteries. Herein, we review the various multi-physics/scale models used to provide mechanistic insights into processes in Li-air batteries and relate these to overall battery performance. First, continuum-based models describing ion transport, pore blocking phenomena, and reduction product precipitation are presented. Next, atomistic modeling-based studies that provide an understanding of the reaction mechanisms in oxygen evolution reaction (OER) and oxygen reduction reaction (ORR), as well as ion–ion interactions in the electrolyte, are described.
Highlights
The highest specific energy storage achieved by state-of-the-art lithium-ion batteries is too low to meet current demands in the automotive industry [1,2]
Chen et al [19] investigated the performance of Li-air batteries with carbon nanotube (CNT) and carbon nanofiber (CNF) cathodes, where the cathode material was modeled as a cylinder
Different film film cathodepore poreshapes, shapes,including including planar, planar, cylindrical, cylindrical, and and spherical resistor models were suggested for each cathode pore shape, and the voltage drop due to the electric resistor models were suggested for each cathode pore shape, and the voltage drop due to the electric passivation passivationwas wasmodeled modeledfor for each each case case as: as:
Summary
The highest specific energy storage achieved by state-of-the-art lithium-ion batteries is too low to meet current demands in the automotive industry [1,2]. Lithium-Air (Li-air) batteries [3,4], which are based on the chemistry of a Li metal anode and air cathode, have extremely high theoretical energy densities, as shown, and have been proposed as alternative systems. Achieving the theoretically predicted energy densities of Li-air batteries depends, in part, on the selection of appropriate electrolytes that allow high cyclability and improve energy density without compromising safety [1]. Another critical issue in Li-air batteries is the selection of a suitable cathode structure along with catalysts to improve efficiency and cycle life. These issues, as aptly summarized in a recent review by Grande et al [5], are related to the overall poor rate capability, high charge overvoltage, and low chemical stability of active materials, leading to a diminished cycle life and the high reactivity of metallic lithium in the anode, which poses a safety threat
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