Ultrastable cathodes enabled by compositional and structural dual-gradient design

Liu, Tongchao; Yu, Lei; Liu, Junxiang; Dai, Alvin; Zhou, Tao; Wang, Jing; Huang, Weiyuan; Li, Luxi; Li, Matthew; Li, Tianyi; Huang, Xiaojing; Xiao, Xianghui; Ge, Mingyuan; Ma, Lu; Zhuo, Zengqing; Amine, Rachid; Chu, Yong S.; Lee, Wah-Keat; Wen, Jianguo; Amine, Khalil

doi:10.1038/s41560-024-01605-8

Ultrastable cathodes enabled by compositional and structural dual-gradient design

Journal Article · Fri Aug 02 04:00:00 EDT 2024 · Nature Energy

DOI:https://doi.org/10.1038/s41560-024-01605-8· OSTI ID:2440575

^[1]; Yu, Lei ^[2]; ^[1]; Dai, Alvin ^[1]; ^[2]; Wang, Jing ^[1]; ^[1]; ^[3]; ^[1]; ^[3]; ^[4]; ^[4]; ^[4]; Ma, Lu ^[4]; ^[5]; Amine, Rachid ^[1]; Chu, Yong S. ^[4]; Lee, Wah-Keat ^[4]; ^[2]; ^[1]

Argonne National Laboratory (ANL), Argonne, IL (United States)
Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)

Cathodes for next-generation batteries are pressed for higher voltage operation (≥4.5 V) to achieve high capacity with long cyclability and thermal tolerance. Current cathodes fail to meet these requirements owing to structural and electrochemical strains at high voltages, leading to fast capacity fading. Here, in this work, we present a cathode with a coherent architecture ranging from ordered to disordered frameworks with concentration gradient and controllable Ni oxidation activities, which can overcome voltage ceilings imposed by existing cathodes. This design enables simultaneous high-capacity and high-voltage operation at 4.5 V without capacity fading, and up to 4.7 V with negligible capacity decay. Multiscale diffraction and imaging techniques reveal the disordered surface is electrochemically and structurally indestructible, preventing surface parasitic reactions and phase transitions. Structural coherence from ordering to disordering limits lattice parameter changes, mitigating lattice strain and enhancing morphological integrity. The dual-gradient design also notably improves thermal stability, driving the advancement of high-performance cathode materials.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); 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:: 2440575

Report Number(s):: BNL--226019-2024-JAAM

Journal Information:: Nature Energy, Journal Name: Nature Energy Journal Issue: 10 Vol. 9; ISSN 2058-7546

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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