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Title: Understanding improved cycling and thermal stability of compositionally graded Ni-rich layered LiNi0.6Mn0.2Co0.2O2 cathode materials

Journal Article · · Nano Energy
 [1];  [1];  [2];  [3];  [3]; ORCiD logo [4];  [3];  [3];  [5];  [3];  [6]
  1. Yonsei Univ., Seoul (Korea, Republic of)
  2. Shanghai Jiao Tong Univ. (China)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  6. Argonne National Laboratory (ANL), Argonne, IL (United States)
+ Show Author Affiliations

The concentration gradient is a strategic design, adjusting the distribution of Ni, typically with a higher Ni content in the core and a higher Mn content toward the surface. This design leverages the pivotal role of the Ni/Mn ratio, seeking to optimize cathode performance by balancing Ni's high capacity with Mn's stabilizing effects, particularly at the surface where degradation commonly occurs during cycling. Here, our study delves into the intricate structural and chemical transformations within concentration gradient cathode materials during electrochemical cycling. Utilizing advanced synchrotron X-ray techniques, including hard and soft X-ray absorption spectroscopy (hXAS, sXAS), and nanoscale X-ray imaging, we investigate buried changes in concentration gradient LiNi0.6Mn0.2Co0.2O2 (CG NMC622). Contrary to conventional assumptions, our findings challenge the notion that cycling stability relies solely on Mn stability. Unraveling the roles of Ni and Mn, we uncover how their individual and collective contributions impact the cathode's overall performance. This investigation transcends established paradigms, shedding light on the crucial mechanisms governing the enhanced cycling stability of Nirich layered cathode materials.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)
Grant/Contract Number:
SC0012704; AC02-06CH11357
OSTI ID:
2341831
Report Number(s):
BNL--225574-2024-JAAM; {"","Journal ID: ISSN 2211-2855"}
Journal Information:
Nano Energy, Journal Name: Nano Energy Vol. 126; ISSN 2211-2855
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Ni-rich layered oxide
concentration gradient cathode
long cycling
thermal stability
synchrotron x-ray characterizations