期刊
CHEMISTRY OF MATERIALS
卷 28, 期 4, 页码 1058-1065出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.5b04289
关键词
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资金
- Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan
- Elemental Strategy Initiative for Catalysis and Batteries (ESICB)
- Hattori Hokokai Foundation
- [15H05701]
- Grants-in-Aid for Scientific Research [14J11134, 15K13798, 15H05701] Funding Source: KAKEN
Raising the operating potential of the cathode materials in sodium-ion batteries is a crucial challenge if they are to outperform state-of-the-art lithium-ion batteries. Although the layered transition metal oxides, NaMO2 (M: transition metal), are the most promising cathode materials owing to their high theoretical capacity with much more stable nature than Li1-xMO2 system, factors influencing the redox potential have not yet been fully understood. Here, we identify redox potential paradox, E(Ni3+/Ni2+) > E(Ni4+/Ni3+), in an identical structural framework, namely, NaTi0.54+Ni0.52+O2 and NaFe0.53+Ni0.53+O2, which is induced by transition of the oxides from Mott-Hubbard to negative charge-transfer regimes. The origin of the unusually low E(Ni4+/Ni3+) is the surprisingly large contribution (over 80%) of oxygen orbital to the redox reaction, of which the primary effect on the electrochemical property is demonstrated for the first time, providing a firm platform to design better cathodes for advanced sodium-ion batteries.
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