Compositionally complex doping for zero-strain zero-cobalt layered cathodes

Zhang, Rui; Wang, Chunyang; Zou, Peichao; Lin, Ruoqian; Ma, Lu; Yin, Liang; Li, Tianyi; Xu, Wenqian; Jia, Hao; Li, Qiuyan; Sainio, Sami; Kisslinger, Kim; Trask, Stephen E.; Ehrlich, Steven N.; Yang, Yang; Kiss, Andrew M.; Ge, Mingyuan; Polzin, Bryant J.; Lee, Sang Jun; Xu, Wu; Ren, Yang; Xin, Huolin L.

doi:10.1038/s41586-022-05115-z

Compositionally complex doping for zero-strain zero-cobalt layered cathodes

Journal Article · Wed Sep 21 00:00:00 EDT 2022 · Nature (London)

DOI:https://doi.org/10.1038/s41586-022-05115-z· OSTI ID:1893831

Zhang, Rui ^[1]; ^[1]; Zou, Peichao ^[1]; ^[2]; Ma, Lu ^[3]; Yin, Liang ^[4]; Li, Tianyi ^[4]; Xu, Wenqian ^[4]; Jia, Hao ^[5]; ^[5]; Sainio, Sami ^[6]; Kisslinger, Kim ^[2]; ^[4]; Ehrlich, Steven N. ^[3]; Yang, Yang ^[3]; ^[3]; Ge, Mingyuan ^[3]; Polzin, Bryant J. ^[4]; ^[6]; ^[5] more »

University of California, Irvine, CA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Argonne National Lab. (ANL), Lemont, IL (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)

We report 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 industry. 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 batteries. However, current high-Ni cathode materials, without exception, suffer severely from their intrinsic thermal and chemo-mechanical instabilities and insufficient cycle life. Here, in this paper, 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.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Argonne National Laboratory (ANL), Lemont, IL (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

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

Grant/Contract Number:: AC02-06CH11357; AC02-76SF00515; AC05-76RL01830; EE0008444; SC0012704; SC0021204

OSTI ID:: 1893831

Alternate ID(s):: OSTI ID: 1996504

Report Number(s):: PNNL-SA-170190

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7930 Vol. 610; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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