High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries

Yao, Libing; Zou, Peichao; Wang, Chunyang; Jiang, Jiahao; Ma, Lu; Tan, Sha; Beyer, Kevin A.; Xu, Feng; Hu, Enyuan; Xin, Huolin L.

doi:10.1002/aenm.202201989

High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries

Journal Article · Thu Sep 08 00:00:00 EDT 2022 · Advanced Energy Materials

DOI:https://doi.org/10.1002/aenm.202201989· OSTI ID:1889148

Yao, Libing ^[1]; Zou, Peichao ^[1]; Wang, Chunyang ^[1]; Jiang, Jiahao ^[1]; Ma, Lu ^[2]; Tan, Sha ^[3]; Beyer, Kevin A. ^[4]; Xu, Feng ^[5]; ^[3]; ^[1]

Univ. of California, Irvine, CA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.
Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Southeast Univ., Nanjing (China)

Layered transition metal oxides are appealing cathodes for sodium-ion batteries due to their overall advantages in energy density and cost. But their stabilities are usually compromised by the complicated phase transition and the oxygen redox, particularly when operating at high voltages, leading to poor structural stability and substantial capacity loss. Here, in this study, an integrated strategy combing the high-entropy design with the superlattice-stabilization to extend the cycle life and enhance the rate capability of layered cathodes is reported. It is shown that the as-prepared high-entropy Na_2/3Li_1/6Fe_1/6Co_1/6Ni_1/6Mn_1/3O₂ cathode enables a superlattice structure with Li/transition metal ordering and delivers excellent electrochemical performance that is not affected by the presence of phase transition and oxygen redox. It achieves a high reversible capacity (171.2 mAh g^–1 at 0.1 C), a high energy density (531 Wh kg^–1), extended cycling stability (89.3% capacity retention at 1 C for 90 cycles and 63.7% capacity retention at 5 C after 300 cycles), and excellent fast-charging capability (78 mAh g^–1 at 10 C). This strategy would inspire more rational designs that can be leveraged to improve the reliability of layered cathodes for secondary-ion batteries.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704; AC02-06CH11357; AC02-76SF00515

OSTI ID:: 1889148

Alternate ID(s):: OSTI ID: 1896836

Report Number(s):: BNL-223423-2022-JAAM

Journal Information:: Advanced Energy Materials, Journal Name: Advanced Energy Materials Journal Issue: 41 Vol. 12; ISSN 1614-6832

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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