Hierarchical nickel valence gradient stabilizes high-nickel content layered cathode materials

Ruoqian Lin, Seong Min Bak, Youngho Shin, Rui Zhang, Chunyang Wang, Kim Kisslinger, Mingyuan Ge, Xiaojing Huang, Zulipiya Shadike, Ajith Pattammattel, Hanfei Yan, Yong Chu, Jinpeng Wu, Wanli Yang, M. Stanley Whittingham, Huolin L. Xin, Xiao Qing Yang

Research output: Contribution to journalArticlepeer-review

70 Citations (Scopus)


High-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials’ thermal and cycling stability. Even though promising, the fundamental mechanism of the nickel concentration gradient’s stabilization effect remains elusive because it is inseparable from nickel’s valence gradient effect. To isolate nickel’s valence gradient effect and understand its fundamental stabilization mechanism, we design and synthesize a LiNi0.8Mn0.1Co0.1O2 material that is compositionally uniform and has a hierarchical valence gradient. The nickel valence gradient material shows superior cycling and thermal stability than the conventional one. The result suggests creating an oxidation state gradient that hides the more capacitive but less stable Ni3+ away from the secondary particle surfaces is a viable principle towards the optimization of high-nickel content cathode materials.

Original languageEnglish
Article number2350
JournalNature communications
Issue number1
Publication statusPublished - 2021 Dec 1

Bibliographical note

Publisher Copyright:
© 2021, The Author(s).

All Science Journal Classification (ASJC) codes

  • General Chemistry
  • General Biochemistry,Genetics and Molecular Biology
  • General Physics and Astronomy


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