Rational Design of Na(Li1/3Mn2/3)O2 Operated by Anionic Redox Reactions for Advanced Sodium‐Ion Batteries |
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| Authors: | Duho Kim Maenghyo Cho Kyeongjae Cho |
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| Affiliation: | 1. Department of Mechanical and Aerospace Engineering, Seoul National University, Gwanak‐gu, Seoul, Republic of Korea;2. Institute of Advanced Machines and Design, Seoul National University, Gwanak‐gu, Seoul, Republic of Korea;3. Department of Materials Science and Engineering and Department of Physics, University of Texas at Dallas, Richardson, TX, USA |
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| Abstract: | In an effort to develop high‐energy‐density cathodes for sodium‐ion batteries (SIBs), low‐cost, high capacity Na(Li1/3Mn2/3)O2 is discovered, which utilizes the labile O 2p‐electron for charge compensation during the intercalation process, inspired by Li2MnO3 redox reactions. Na(Li1/3Mn2/3)O2 is systematically designed by first‐principles calculations considering the Li/Na mixing enthalpy based on the site preference of Na in the Li sites of Li2MnO3. Using the anionic redox reaction (O2?/O?), this Mn‐oxide is predicted to show high redox potentials (≈4.2 V vs Na/Na+) with high charge capacity (190 mAh g?1). Predicted cathode performance is validated by experimental synthesis, characterization, and cyclic performance studies. Through a fundamental understanding of the redox reaction mechanism in Li2MnO3, Na(Li1/3Mn2/3)O2 is designed as an example of a new class of promising cathode materials, Na(Li1/3M2/3)O2 (M: transition metals featuring stabilized M4+), for further advances in SIBs. |
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| Keywords: | anionic redox reactions first principle calculations lone‐pair O manganese oxides sodium‐ion batteries |
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