Title Cycling mechanism of Li2MnO3: Li-CO2 batteries and commonality on oxygen redox in cathode materials
Authors Zhuo, Zengqing
Dai, Kehua
Qiao, Ruimin
Wang, Rui
Wu, Jinpeng
Liu, Yali
Peng, Jiayue
Chen, Liquan
Chuang, Yi-de
Pan, Feng
Shen, Zhi-xun
Liu, Gao
Li, Hong
Devereaux, Thomas P.
Yang, Wanli
Affiliation Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA
Peking Univ, Sch Adv Mat, Shenzhen Grad Sch, Shenzhen 518055, Peoples R China
Lawrence Berkeley Natl Lab, Energy Storage & Distributed Resources Div, Energy Technol Area, Berkeley, CA 94720 USA
Tianjin Normal Univ, Coll Chem, Tianjin 300387, Peoples R China
Northeastern Univ, Sch Met, Shenyang 110819, Peoples R China
Chinese Acad Sci, Inst Phys, Beijing 100190, Peoples R China
Stanford Inst Mat & Energy Sci, SLAC Natl Accelerator Lab, Menlo Pk, CA 94025 USA
Stanford Univ, Geballe Lab Adv Mat, Stanford, CA 94305 USA
Stanford Univ, Dept Phys & Appl Phys, Stanford, CA 94305 USA
Stanford Univ, Dept Mat Sci & Engn, Stanford, CA 94305 USA
Keywords POSITIVE ELECTRODE MATERIALS
RICH LAYERED OXIDES
LI-ION
ANIONIC REDOX
CHARGE-COMPENSATION
ELECTROCHEMICAL-BEHAVIOR
ANOMALOUS CAPACITY
LATTICE OXYGEN
METAL-OXIDES
THIN-FILM
Issue Date 21-Apr-2021
Publisher JOULE
Abstract A SUMMARY Li2MnO3 has been considered to be a representative Li-rich compound with active debates on oxygen activities. Here, by evaluating the Mn and O states in the bulk and on the surface of Li2MnO3, we clarify that Mn( III/IV) redox dominates the reversible bulk redox in Li2MnO3, while the initial charge plateau is from surface reactions with oxygen release and carbonate decomposition. No lattice oxygen redox is involved at any electrochemical stage. The carbonate formation and decomposition indicate the catalytic property of the Li2MnO3 surface, which inspires Li-CO2/air batteries with Li2MnO3 acting as a superior electrocatalyst. The absence of lattice oxygen redox in Li2MnO3 questions the origin of the oxygen redox in Li-rich compounds, which is found to be of the same nature as that in conventional materials based on spectroscopic comparisons. These findings provide guidelines on understanding and controlling oxygen activities toward high-energy cathodes and suggest opportunities on using alkali-rich materials for catalytic reactions.
URI http://hdl.handle.net/20.500.11897/612971
ISSN 2542-4351
DOI 10.1016/j.joule.2021.02.004
Indexed SCI(E)
Appears in Collections: 新材料学院

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