Journal
NATURE COMMUNICATIONS
Volume 7, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms12108
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Funding
- NIMTE from Strategic Priority Research Program of Chinese Academy of Sciences (CAS) [XDA09010101]
- CAS [174433KYSB20150047]
- Department of Energy, USA (CAS-DOE) [174433KYSB20150047]
- Ningbo Science and Technology Innovation Team [2012B82001]
- Assistant Secretary for Energy Efficiency and Renewable Energy, Office of Vehicle Technologies of the U.S. Department of Energy (DOE) under the Advanced Battery Materials Research (BMR) Program [DE-AC02-05CH11231, 7073923]
- U.S. DOE, Office of Basic Energy Science, Division of Materials Science and Engineering [DE-AC02-98CH10886]
- office of Basic Energy Sciences (BES), the Office of Science of the U.S. DOE
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Lattice oxygen can play an intriguing role in electrochemical processes, not only maintaining structural stability, but also influencing electron and ion transport properties in high-capacity oxide cathode materials for Li-ion batteries. Here, we report the design of a gas-solid interface reaction to achieve delicate control of oxygen activity through uniformly creating oxygen vacancies without affecting structural integrity of Li-rich layered oxides. Theoretical calculations and experimental characterizations demonstrate that oxygen vacancies provide a favourable ionic diffusion environment in the bulk and significantly suppress gas release from the surface. The target material is achievable in delivering a discharge capacity as high as 301 mAhg(-1) with initial Coulombic efficiency of 93.2%. After 100 cycles, a reversible capacity of 300 mAhg(-1) still remains without any obvious decay in voltage. This study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.
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