Stabilizing the Oxygen Lattice and Reversible Oxygen Redox Chemistry through Structural Dimensionality in Lithium-Rich Cathode Oxides

  • Enyue Zhao
  • , Qinghao Li
  • , Fanqi Meng
  • , Jue Liu
  • , Junyang Wang
  • , Lunhua He
  • , Zheng Jiang
  • , Qinghua Zhang
  • , Xiqian Yu
  • , Lin Gu
  • , Wanli Yang
  • , Hong Li
  • , Fangwei Wang
  • , Xuejie Huang

Research output: Contribution to journalArticlepeer-review

131 Scopus citations

Abstract

Lattice-oxygen redox (l-OR) has become an essential companion to the traditional transition-metal (TM) redox charge compensation to achieve high capacity in Li-rich cathode oxides. However, the understanding of l-OR chemistry remains elusive, and a critical question is the structural effect on the stability of l-OR reactions. Herein, the coupling between l-OR and structure dimensionality is studied. We reveal that the evolution of the oxygen-lattice structure upon l-OR in Li-rich TM oxides which have a three-dimensional (3D)-disordered cation framework is relatively stable, which is in direct contrast to the clearly distorted oxygen-lattice framework in Li-rich oxides which have a two-dimensional (2D)/3D-ordered cation structure. Our results highlight the role of structure dimensionality in stabilizing the oxygen lattice in reversible l-OR, which broadens the horizon for designing high-energy-density Li-rich cathode oxides with stable l-OR chemistry.

Original languageEnglish
Pages (from-to)4323-4327
Number of pages5
JournalAngewandte Chemie - International Edition
Volume58
Issue number13
DOIs
StatePublished - Mar 22 2019

Funding

This work was supported by funding from National Key R&D Program of China (2016YFA0202500), Foundation for Innovative Research Groups of the NSFC (No. 51421002), NSFC (No. 11675255, 51502334, 51822211). This work used resources of the ALS, which is a US DOE Office of Science User Facility, W.Y. acknowledges support from EERE VTO under the Applied Battery Materials Program of the US DOE, both under Contract No. DE-AC02-05CH11231.

Keywords

  • cathodes
  • lattice oxygen redox
  • lithium-ion batteries
  • oxides
  • structural dimensionality

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