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• W4386866929 abstract "Development of energy storage systems with high energy density is of vital importance for realizing a sustainable society. Although lithium-ion batteries (LIBs) are the state-of-the-art energy storage technology, their energy density is limited in part by the specific capacity of the positive electrode (cathode) materials. For example, conventional cathode materials, i.e. , layered transition-metal oxides LiMO 2 (M = transition metal), deliver a modest capacity of approximately 160 mAh/g, where the dominant mechanism of charge compensation for lithium-ion (de)intercalation is the valence change of the transition metal. Further increase in the cathode capacity requires an additional redox center. Integrating an anionic-redox (or oxygen-redox) capacity with the conventional cationic-redox capacity is a promising strategy for large-capacity battery cathodes exceeding present technical limits. However, most oxygen-redox cathodes exhibit a large charge/discharge voltage hysteresis (> 0.5 V), resulting in poor energy efficiency and impractical implementation. Considering immediate electron transfer (O 2– → O – + e – ) against subsequent structural deformation (O–O dimerization), the overall hypothetical mechanism of the oxygen-redox reactions is described as a square scheme (Figure 1) 1 : if an oxidized oxide ion (O – ) is stable, it directly contributes to a non-polarizing discharge capacity (nonpolarizing O redox). 2 Meanwhile, unstable O – dimerize to form stable peroxo-like O 2 2– , which may be accelerated by cation migration. The O 2 2– dimers provide a polarizing discharge capacity (polarizing O redox) and an unstable reduced dimer (e.g., O 2 4– ) decomposes to O 2– . The O–O dimerization is prone to result in release of O 2 gas (O 2 evolution) by their excessive oxidation. However, experimental verification of the square scheme is limited in part due to complicated structural changes during the oxygen-redox reactions. For example, O3-type Li 1.2 Ni 0.2 Mn 0.6 O 2 (O3: lithium ions occupy octahedral sites between the MO 2 layers, and the packing arrangement of the oxide ions is ABCABC) exhibits irreversible structural degradation such as layered-to-spinel transformation and surface cation densification upon cycling. In this work, we focus on O2-type lithium-rich layered transition-metal oxides that possess structural integrity against the oxygen-redox reactions (O2: lithium ions occupy octahedral sites between the MO 2 layers and the packing arrangement of the oxide ions is ABCBA). O2-type Li 1.12– y Ni 0.17 Mn 0.71 O 2 delivers a large reversible capacity greater than 200 mAh/g with minimal voltage decay and capacity fading upon cycling. Combination of X-ray absorption/emission spectroscopy, magnetic susceptibility measurements, and density functional theory calculations indicates bond-forming 2O – → O 2 2– and bond-cleaving O 2 4– → 2O 2– processes. These results emphasize the importance of suppressing the formation of O 2 2– and maximizing the contribution of the nonpolarizing O 2– /O – redox couple to develop energy-efficient oxygen-redox battery electrodes. Furthermore, based on the electrochemical kinetic analysis, particularly for the 2O 2– → O 2 2– transformation, technical strategies to quantify non-polarizing and energy-efficient oxygen redox will be discussed. References M. Okubo, et al. , Acc. Mater. Res. 2021 , 3, 33–41. A. Tsuchimoto, et al. , Nat. Commun. 2020 , 12, 63. K. Kawai, et al. , Energy Environ. Sci. 2022 , 15, 2591–2600. Figure 1" @default.
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• W4386866929 date "2023-08-28" @default.
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• W4386866929 title "Peroxide Formation for Voltage Hysteresis in O2-Type Lithium-Rich Layered Oxides" @default.
• W4386866929 doi "https://doi.org/10.1149/ma2023-012490mtgabs" @default.
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