title: In Situ Atomic-Scale Observation of Electrochemical Delithiation Induced Structure Evolution of LiCoO2Cathode in a Working All-Solid-State Battery.
abstract: We report a method for in situ atomic-scale observation of electrochemical delithiation in a working all-solid-state battery using a state-of-the-art chip based in situ transmission electron microscopy (TEM) holder and focused ion beam milling to prepare an all-solid-state lithium-ion battery sample. A battery consisting of LiCoO2cathode, LLZO solid state electrolyte and gold anode was constructed, delithiated and observed in an aberration corrected scanning transmission electron microscope at atomic scale. We found that the pristine single crystal LiCoO2became nanosized polycrystal connected by coherent twin boundaries and antiphase domain boundaries after high voltage delithiation. This is different from liquid electrolyte batteries, where a series of phase transitions take place at LiCoO2cathode during delithiation. Both grain boundaries become more energy favorable along with extraction of lithium ions through theoretical calculation. We also proposed a lithium migration pathway before and after polycrystallization. This new methodology could stimulate atomic scale in situ scanning/TEM studies of battery materials and provide important mechanistic insight for designing better all-solid-state battery.
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.|School of Physical Sciences, University of Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Yue
authors.identifier: 0000-0002-5764-3117
authors.initials: Y
authors.lastname: Gong
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Jienan
authors.initials: J
authors.lastname: Zhang
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Liwei
authors.initials: L
authors.lastname: Jiang
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Jin-An
authors.initials: JA
authors.lastname: Shi
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Qinghua
authors.initials: Q
authors.lastname: Zhang
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Zhenzhong
authors.initials: Z
authors.lastname: Yang
authors.affiliation: Department of Mechanical, Materials and Manufacturing Engineering, The University of Nottingham Ningbo China , Ningbo, Zhejiang 315100, China.
authors.forename: Dongli
authors.initials: D
authors.lastname: Zou
authors.affiliation: Department of Physics, Shantou University , Shantou, Guangdong 515063, China.
authors.forename: Jiangyong
authors.initials: J
authors.lastname: Wang
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Xiqian
authors.identifier: 0000-0001-8513-518X
authors.initials: X
authors.lastname: Yu
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Ruijuan
authors.initials: R
authors.lastname: Xiao
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Yong-Sheng
authors.initials: YS
authors.lastname: Hu
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.|Department of Physics, Shantou University , Shantou, Guangdong 515063, China.|Collaborative Innovation Center of Quantum Matter , Beijing 100190, China.|School of Physical Sciences, University of Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Lin
authors.identifier: 0000-0002-7504-031X
authors.initials: L
authors.lastname: Gu
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Hong
authors.initials: H
authors.lastname: Li
authors.affiliation: Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences , Beijing 100190, China.
authors.forename: Liquan
authors.initials: L
authors.lastname: Chen