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 () and Xiao-Qing Yang ()
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Ruoqian Lin: Brookhaven National Laboratory
Seong-Min Bak: Brookhaven National Laboratory
Youngho Shin: Argonne National Laboratory
Rui Zhang: University of California
Chunyang Wang: University of California
Kim Kisslinger: Brookhaven National Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Xiaojing Huang: Brookhaven National Laboratory
Zulipiya Shadike: Brookhaven National Laboratory
Ajith Pattammattel: Brookhaven National Laboratory
Hanfei Yan: Brookhaven National Laboratory
Yong Chu: Brookhaven National Laboratory
Jinpeng Wu: Lawrence Berkeley National Laboratory
Wanli Yang: Lawrence Berkeley National Laboratory
M. Stanley Whittingham: Binghamton University
Huolin L. Xin: University of California
Xiao-Qing Yang: Brookhaven National Laboratory

Nature Communications, 2021, vol. 12, issue 1, 1-10

Abstract: Abstract 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.

Date: 2021
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DOI: 10.1038/s41467-021-22635-w

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