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.
| Original language | English |
|---|---|
| Article number | 1478 |
| Journal | Nature Communications |
| Volume | 16 |
| Issue number | 1 |
| DOIs | |
| State | Published - Dec 2025 |
Funding
The work was supported by the Virginia Tech Department of Chemistry startup funds and National Science Foundation (DMR-1832613) (F.L.). The use of the Spallation Neutron Source at Oak Ridge National Laboratory is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC05-00OR22725. The use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The research used 18-ID of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. This research used Electron Microscopy facility of the Center for Functional Nanomaterials (CFN), which is a U.S. Department of Energy Office of Science User Facility, at Brookhaven National Laboratory under Contract No. DE-SC0012704. H.S. thanks Dr. Dong Hou for the assistance with diffraction analyses.