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

Bao Qiu, Minghao Zhang, Lijun Wu, Jun Wang, Yonggao Xia (), Danna Qian, Haodong Liu, Sunny Hy, Yan Chen, Ke An, Yimei Zhu, Zhaoping Liu () and Ying Shirley Meng ()
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Bao Qiu: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences
Minghao Zhang: University of California San Diego (UCSD)
Lijun Wu: Brookhaven National Laboratory
Jun Wang: MEET Battery Research Center/Institute of Physical Chemistry, University of Müenster
Yonggao Xia: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences
Danna Qian: University of California San Diego (UCSD)
Haodong Liu: University of California San Diego (UCSD)
Sunny Hy: University of California San Diego (UCSD)
Yan Chen: Oak Ridge National Laboratory
Ke An: Oak Ridge National Laboratory
Yimei Zhu: Brookhaven National Laboratory
Zhaoping Liu: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences
Ying Shirley Meng: University of California San Diego (UCSD)

Nature Communications, 2016, vol. 7, issue 1, 1-10

Abstract: Abstract 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. This study sheds light on the comprehensive design and control of oxygen activity in transition-metal-oxide systems for next-generation Li-ion batteries.

Date: 2016
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DOI: 10.1038/ncomms12108

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