Journal
ADVANCED MATERIALS
Volume 29, Issue 33, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.201701788
Keywords
anionic redox reactions; first principle calculations; lone-pair O; manganese oxides; sodium-ion batteries
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Funding
- National Research Foundation of Korea (NRF) - Korean government (MSIP), Republic of Korea [2012R1A3A2048841]
- New & Renewable Energy Core Technology Program of the Korea Institute of Energy Technology Evaluation and Planning (KETEP) from Ministry of Trade, Industry & Energy, Republic of Korea [20152020105420]
- Korea Evaluation Institute of Industrial Technology (KEIT) [20152020105420] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
- National Research Foundation of Korea [2012R1A3A2048841] Funding Source: Korea Institute of Science & Technology Information (KISTI), National Science & Technology Information Service (NTIS)
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In an effort to develop high-energy-density cathodes for sodium-ion batteries (SIBs), low-cost, high capacity Na(Li1/3Mn2/3)O-2 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)O-2 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 (approximate to 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)O-2 is designed as an example of a new class of promising cathode materials, Na(Li1/3M2/3)O-2 (M: transition metals featuring stabilized M4+), for further advances in SIBs.
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