Thermal processing to modulate surface chemistry and bulk charge distribution in nickel-rich layered lithium positive electrodes

Huabin Sun, Zhijie Yang, Rupayan Ghosh, Sooyeon Hwang, Anyang Hu, Yuxin Zhang, Jue Liu, Chengjun Sun, Sami Sainio, Dennis Nordlund, Xianghui Xiao and Feng Lin ()
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Huabin Sun: Virginia Tech
Zhijie Yang: Virginia Tech
Rupayan Ghosh: Virginia Tech
Sooyeon Hwang: Brookhaven National Laboratory
Anyang Hu: Virginia Tech
Yuxin Zhang: Virginia Tech
Jue Liu: Oak Ridge National Laboratory
Chengjun Sun: Argonne National Laboratory
Sami Sainio: SLAC National Accelerator Laboratory
Dennis Nordlund: SLAC National Accelerator Laboratory
Xianghui Xiao: Brookhaven National Laboratory
Feng Lin: Virginia Tech

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract The broader application of nickel-rich layered oxides as positive electrode materials for lithium-ion batteries has been hindered by their high manufacturing cost and inferior cycling stability. Thermal processing, which is integral to electrode materials manufacturing and fundamental in materials science, has not been fully utilized to design advanced positive electrode materials. Herein, we demonstrate the capability of using quenching heat treatment to regulate Li distribution and modulate electronic structure near particle surface. The resulting materials exhibit less parasitic reactions with the electrolyte and an improved charge distribution homogeneity in secondary particles, leading to more stable cycling performance at high voltages (4.5 V vs Li/Li+). Our synchrotron X-ray analyses reveal the underlying interplay between surface structure and bulk charge distribution in positive electrode materials particles. While strategies used to stabilize positive electrode materials through compositional control, surface modification, and electrolyte engineering have become mature, thermal processing can be advantageous to further improve positive electrode materials manufacturing.

Date: 2025
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DOI: 10.1038/s41467-025-56075-7

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