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Unblocking Oxygen Charge Compensation for Stabilized High-Voltage Structure in P2-Type Sodium-Ion Cathode

  • He Zhu
  • , Zhenpeng Yao
  • , Hekang Zhu
  • , Yalan Huang
  • , Jian Zhang
  • , Cheng Chao Li*
  • , Kamila M. Wiaderek
  • , Yang Ren
  • , Cheng-Jun Sun
  • , Hua Zhou
  • , Longlong Fan
  • , Yanan Chen
  • , Hui Xia
  • , Lin Gu*
  • , Si Lan
  • , Qi Liu*
    • *Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

85   Link opens in a new tab Citations (Scopus)
72 Downloads (CityUHK Scholars)

Abstract

Layered transition-metal (TM) oxides are ideal hosts for Li+ charge carriers largely due to the occurrence of oxygen charge compensation that stabilizes the layered structure at high voltage. Hence, enabling charge compensation in sodium layered oxides is a fascinating task for extending the cycle life of sodium-ion batteries. Herein a Ti/Mg co-doping strategy for a model P2-Na2/3Ni1/3Mn2/3O2 cathode material is put forward to activate charge compensation through highly hybridized O2p-TM3d covalent bonds. In this way, the interlayer O-O electrostatic repulsion is weakened upon deeply charging, which strongly affects the systematic total energy that transforms the striking P2–O2 interlayer contraction into a moderate solid-solution-type evolution. Accordingly, the cycling stability of the codoped cathode material is improved superiorly over the pristine sample. This study starts a perspective way of optimizing the sodium layered cathodes by rational structural design coupling electrochemical reactions, which can be extended to widespread battery researches.
Original languageEnglish
Article number2200498
JournalAdvanced Science
Volume9
Issue number16
Online published28 Mar 2022
DOIs
Publication statusPublished - 3 Jun 2022

Funding

H.Z. and Z.Y. contributed equally to this work. This study was supported by the National Key R&D Program of China (No. 2020YFA0406203), the Shenzhen Science and Technology Innovation Commission (Nos. SGDX2019081623240948 and JCYJ20200109105618137), the ECS scheme (No. CityU 21307019), and the Shenzhen Research Institute, City University of Hong Kong. Dr. Z. Yao is grateful to the support by the US Department of Energy, Office of Science – Chicago under Award No. DE-SC0019300. Computations were performed on the Niagara supercomputer at the SciNet HPC Consortium. SciNet is funded by the Canada Foundation for Innovation; the Government of Ontario, Ontario Research Fund-Research Excellence, and the University of Toronto. This research also 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 No. DE-AC02-06CH11357.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

  1. SDG 7 - Affordable and Clean Energy
    SDG 7 Affordable and Clean Energy

Research Keywords

  • high-voltage structural stability
  • in situ synchrotron characterizations
  • layered transition-metal oxide cathodes
  • oxygen charge compensation
  • sodium-ion battery

Publisher's Copyright Statement

  • This full text is made available under CC-BY 4.0. https://creativecommons.org/licenses/by/4.0/

RGC Funding Information

  • RGC-funded

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