Compositionally complex doping for zero-strain zero-cobalt layered cathodes
Rui Zhang,
Chunyang Wang,
Peichao Zou,
Ruoqian Lin,
Lu Ma,
Liang Yin,
Tianyi Li,
Wenqian Xu,
Hao Jia,
Qiuyan Li,
Sami Sainio,
Kim Kisslinger,
Stephen E. Trask,
Steven N. Ehrlich,
Yang Yang,
Andrew M. Kiss,
Mingyuan Ge,
Bryant J. Polzin,
Sang Jun Lee,
Wu Xu,
Yang Ren and
Huolin L. Xin ()
Additional contact information
Rui Zhang: University of California
Chunyang Wang: University of California
Peichao Zou: University of California
Ruoqian Lin: Brookhaven National Laboratory
Lu Ma: Brookhaven National Laboratory
Liang Yin: Argonne National Laboratory
Tianyi Li: Argonne National Laboratory
Wenqian Xu: Argonne National Laboratory
Hao Jia: Pacific Northwest National Laboratory
Qiuyan Li: Pacific Northwest National Laboratory
Sami Sainio: SLAC National Accelerator Laboratory
Kim Kisslinger: Brookhaven National Laboratory
Stephen E. Trask: Argonne National Laboratory
Steven N. Ehrlich: Brookhaven National Laboratory
Yang Yang: Brookhaven National Laboratory
Andrew M. Kiss: Brookhaven National Laboratory
Mingyuan Ge: Brookhaven National Laboratory
Bryant J. Polzin: Argonne National Laboratory
Sang Jun Lee: SLAC National Accelerator Laboratory
Wu Xu: Pacific Northwest National Laboratory
Yang Ren: Argonne National Laboratory
Huolin L. Xin: University of California
Nature, 2022, vol. 610, issue 7930, 67-73
Abstract:
Abstract The high volatility of the price of cobalt and the geopolitical limitations of cobalt mining have made the elimination of Co a pressing need for the automotive industry1. Owing to their high energy density and low-cost advantages, high-Ni and low-Co or Co-free (zero-Co) layered cathodes have become the most promising cathodes for next-generation lithium-ion batteries2,3. However, current high-Ni cathode materials, without exception, suffer severely from their intrinsic thermal and chemo-mechanical instabilities and insufficient cycle life. Here, by using a new compositionally complex (high-entropy) doping strategy, we successfully fabricate a high-Ni, zero-Co layered cathode that has extremely high thermal and cycling stability. Combining X-ray diffraction, transmission electron microscopy and nanotomography, we find that the cathode exhibits nearly zero volumetric change over a wide electrochemical window, resulting in greatly reduced lattice defects and local strain-induced cracks. In-situ heating experiments reveal that the thermal stability of the new cathode is significantly improved, reaching the level of the ultra-stable NMC-532. Owing to the considerably increased thermal stability and the zero volumetric change, it exhibits greatly improved capacity retention. This work, by resolving the long-standing safety and stability concerns for high-Ni, zero-Co cathode materials, offers a commercially viable cathode for safe, long-life lithium-ion batteries and a universal strategy for suppressing strain and phase transformation in intercalation electrodes.
Date: 2022
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DOI: 10.1038/s41586-022-05115-z
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