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Title: Gas-solid interfacial modification of oxygen activity in layered oxide cathodes for lithium-ion batteries

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 mAh g–1 with initial Coulombic efficiency of 93.2%. After 100 cycles, a reversible capacity of 300 mAh g–1 still remains without any obvious decay in voltage. Lastly, this study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.
 [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [2] ;  [2] ;  [5] ;  [5] ;  [3] ;  [1] ;  [2] ;  [2]
  1. Chinese Academy of Sciences, Zhejiang (China)
  2. Univ. of California, San Diego, La Jolla, CA (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
  4. Univ. of Muenster, Muenster (Germany)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Nature Publishing Group
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States