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

Bak, Seong-Min; Song, Myeongjun; Shadike, Zulipiya; Hunt, Adrian; Waluyo, Iradwikanari; Sadowski, Jerzy T.; Yan, Hanfei; Chu, Yong S.; Yang, Xiao-Qing; Huang, Xiaojing; Shin, Youngho

doi:10.1016/j.nanoen.2024.109644

Title: Understanding improved cycling and thermal stability of compositionally graded Ni-rich layered LiNi_0.6Mn_0.2Co_0.2O₂ cathode materials

Journal Article · Tue Apr 23 00:00:00 UTC 2024 · Nano Energy

DOI: https://doi.org/10.1016/j.nanoen.2024.109644 · OSTI ID:2341831

Bak, Seong-Min ^[1]; Song, Myeongjun ^[1]; Shadike, Zulipiya ^[2]; Hunt, Adrian ^[3]; Waluyo, Iradwikanari ^[3];

^[4]; Yan, Hanfei ^[3]; Chu, Yong S. ^[3]; Yang, Xiao-Qing ^[5]; Huang, Xiaojing ^[3]; Shin, Youngho ^[6]

Yonsei Univ., Seoul (Korea, Republic of)
Shanghai Jiao Tong Univ. (China)
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)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States)

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 LiNi_0.6Mn_0.2Co_0.2O₂ (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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS); Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN); Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012704

OSTI ID:: 2341831

Report Number(s):: BNL--225574-2024-JAAM

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

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References (37)

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Title: Understanding improved cycling and thermal stability of compositionally graded Ni-rich layered LiNi_0.6Mn_0.2Co_0.2O₂ cathode materials