title: Gas-solid interfacial modification of oxygen activity in layered oxide cathodes for lithium-ion batteries.
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.
authors.affiliation: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences, Zhejiang 315201, China.
authors.forename: Bao
authors.initials: B
authors.lastname: Qiu
authors.affiliation: Department of Nano Engineering, University of California San Diego (UCSD), La Jolla, California 92093, USA.
authors.forename: Minghao
authors.initials: M
authors.lastname: Zhang
authors.affiliation: Department of Condensed Matter Physics and Materials Science, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Lijun
authors.initials: L
authors.lastname: Wu
authors.affiliation: MEET Battery Research Center/Institute of Physical Chemistry, University of Müenster, Corrensstrasse 46, Müenster 48149, Germany.
authors.forename: Jun
authors.initials: J
authors.lastname: Wang
authors.affiliation: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences, Zhejiang 315201, China.
authors.forename: Yonggao
authors.initials: Y
authors.lastname: Xia
authors.affiliation: Department of Nano Engineering, University of California San Diego (UCSD), La Jolla, California 92093, USA.
authors.forename: Danna
authors.initials: D
authors.lastname: Qian
authors.affiliation: Department of Nano Engineering, University of California San Diego (UCSD), La Jolla, California 92093, USA.
authors.forename: Haodong
authors.initials: H
authors.lastname: Liu
authors.affiliation: Department of Nano Engineering, University of California San Diego (UCSD), La Jolla, California 92093, USA.
authors.forename: Sunny
authors.initials: S
authors.lastname: Hy
authors.affiliation: Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, 37830, USA.
authors.forename: Yan
authors.initials: Y
authors.lastname: Chen
authors.affiliation: Chemical and Engineering Materials Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee, 37830, USA.
authors.forename: Ke
authors.initials: K
authors.lastname: An
authors.affiliation: Department of Condensed Matter Physics and Materials Science, Brookhaven National Laboratory, Upton, New York 11973, USA.
authors.forename: Yimei
authors.initials: Y
authors.lastname: Zhu
authors.affiliation: Ningbo Institute of Materials Technology and Engineering (NIMTE), Chinese Academy of Sciences, Zhejiang 315201, China.
authors.forename: Zhaoping
authors.initials: Z
authors.lastname: Liu
authors.affiliation: Department of Nano Engineering, University of California San Diego (UCSD), La Jolla, California 92093, USA.
authors.forename: Ying Shirley
authors.initials: YS
authors.lastname: Meng