Cation configuration in transition-metal layered oxides

Yubo Yang, Zihe Zhang, Shiqi Liu, Boya Wang, Jue Liu, Yang Ren, Xu Zhang, Shu Zhao, Danmin Liu, Haijun Yu

Research output: Contribution to journalArticlepeer-review

31 Scopus citations

Abstract

The cation configuration of transition-metal (TM) layered oxides used as cathode materials for batteries, which significantly affects their intrinsic performance, is extremely important for understanding their electrochemical behavior and remained unclear until now. Herein, the local cation configuration of a series of Mn-based Li-rich layered oxides (Mn-LLOs) was revealed thoroughly by statistical methods, and the influence of the cation configuration on the cationic/anionic redox was also elucidated. Using neutron and synchrotron X-ray pair distribution function combined with Monte Carlo simulation, the existence of Li2MnO3 rather than Li2MnO3-like crystal domain in all Mn-LLOs is revealed strongly, showing each Li atom in the TM layer is surrounded by six Mn atoms with no Ni atom to form a LiMn6 unit, and the reversibility of oxygen redox is closely related with those local structure environments. This work provides insights for the cation configuration investigation of oxide materials and also sheds light on the understanding of the local structure-activity relationship.

Original languageEnglish
Pages (from-to)3869-3882
Number of pages14
JournalMatter
Volume5
Issue number11
DOIs
StatePublished - Nov 2 2022

Funding

This work was funded by the Beijing Natural Science Foundation ( JQ19003 ), Youth Beijing Scholar program ( PXM2021_014204_000023 ), and National Natural Science Foundation of China (grant nos. 21975006 , 22075007 , and 22002004 ). Neutron total scattering measurements were conducted at the NOMAD beamline at the Spallation Neutron Source, Oak Ridge National Laboratory, which is sponsored by the Scientific User Facilities Division, Office of Basic Sciences, U.S. Department of Energy. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science user facility operated for the DOE Office of Science by Argonne National Laboratory under contract DE-AC02-06CH11357.

Keywords

  • LiMn local structure
  • LiMnO crystal domain
  • MAP1: Discovery
  • Mn-LLOs
  • cation configuration
  • oxygen redox reversibility
  • transition-metal-based oxide cathode

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