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Unexpected li displacement and suppressed phase transition enabling highly stabilized oxygen redox in P3-type Na layered oxide cathode

引用

Journal of Energy Chemistry 2023年第10期85卷 144-153,I0006页

作者： Myungeun Choi Hobin Ahn Hyunyoung Park Yongseok Lee Jinho Ahn Bonyoung Ku Junseong Kim Wonseok Ko Jungmin Kang Jung-Keun Yoo Duho Kim Jongsoon Kim Department of Energy Science Sungkyunkwan UniversitySuwon 16419Republic of Korea SKKU Institute of Energy Science and Technology(SIEST) Sungkyunkwan UniversitySuwon 16419Republic of Korea Carbon Composites Department Korea Institute of Materials Science(KIMS)Changwon 51508Republic of Korea Department of Mechanical Engineering(Integrated Engineering Program) Kyung Hee University1732Deogyeong-daeroGiheung-guYongin-siGyeonggi-do 17104Republic of Korea Department of KHU-KIST Convergence Science and Technology Kyung Hee University23Kyunghee-daero Dongdaemun-guSeoul 02447Republic of Korea

Oxygen redox is considered a new paradigm for increasing the practical capacity and energy density of the layered oxide cathodes for Na-ion batteries. However, severe local structural changes and phase transitions during anionic redox reactions lead to poor electrochemical performance with sluggish ***, we propose a synergy of li-Cu cations in harnessing the full potential of oxygen redox, through li displacement and suppressed phase transition in P3-type layered oxide cathode. P3-type Na_(0.7)[li_(0.1)Cu_(0.2)Mn_(0.7)]O_(2) cathode delivers a large specific capacity of ~212 mA h g^(-1)at 15 mA g^(-1). The discharge capacity is maintained up to ~90% of the initial capacity after 100 cycles, with stable occurrence of the oxygen redox in the high-voltage region. Through advanced experimental analyses and first-principles calculations, it is confirmed that a stepwise redox reaction based on Cu and O ions occurs for the charge-compensation mechanism upon charging. Based on a concrete understanding of the reaction mechanism, the li displacement by the synergy of li-Cu cations plays a crucial role in suppressing the structural change of the P3-type layered material under the oxygen redox reaction, and it is expected to be an effective strategy for stabilizing the oxygen redox in the layered oxides of Na-ion batteries.

关键词： Layered oxide cathode Oxygen redox reaction Structural stability li displacement No phase transition

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