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

Abstract

Abstract 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 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 2/3 Li 1/6 Fe 1/6 Co 1/6 Ni 1/6 Mn 1/3 O 2 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.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4];  [5]; ORCiD logo [3]; ORCiD logo [1]
  1. Univ. of California, Irvine, CA (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  5. Southeast Univ., Nanjing (China)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
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)
OSTI Identifier:
1889148
Alternate Identifier(s):
OSTI ID: 1896836
Report Number(s):
BNL-223423-2022-JAAM
Journal ID: ISSN 1614-6832
Grant/Contract Number:  
SC0012704; DMR-2011967; CHE-1338173; AC02-06CH11357; AC02-76SF00515; DE‐SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 12; Journal Issue: 41; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; high-entropy oxides; layered materials; sodium-ion cathodes; superlattice

Citation Formats

Yao, Libing, Zou, Peichao, Wang, Chunyang, Jiang, Jiahao, Ma, Lu, Tan, Sha, Beyer, Kevin A., Xu, Feng, Hu, Enyuan, and Xin, Huolin L. High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries. United States: N. p., 2022. Web. doi:10.1002/aenm.202201989.
Yao, Libing, Zou, Peichao, Wang, Chunyang, Jiang, Jiahao, Ma, Lu, Tan, Sha, Beyer, Kevin A., Xu, Feng, Hu, Enyuan, & Xin, Huolin L. High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries. United States. https://doi.org/10.1002/aenm.202201989
Yao, Libing, Zou, Peichao, Wang, Chunyang, Jiang, Jiahao, Ma, Lu, Tan, Sha, Beyer, Kevin A., Xu, Feng, Hu, Enyuan, and Xin, Huolin L. Thu . "High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries". United States. https://doi.org/10.1002/aenm.202201989. https://www.osti.gov/servlets/purl/1889148.
@article{osti_1889148,
title = {High-Entropy and Superstructure-Stabilized Layered Oxide Cathodes for Sodium-Ion Batteries},
author = {Yao, Libing and Zou, Peichao and Wang, Chunyang and Jiang, Jiahao and Ma, Lu and Tan, Sha and Beyer, Kevin A. and Xu, Feng and Hu, Enyuan and Xin, Huolin L.},
abstractNote = {Abstract 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 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 2/3 Li 1/6 Fe 1/6 Co 1/6 Ni 1/6 Mn 1/3 O 2 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.},
doi = {10.1002/aenm.202201989},
journal = {Advanced Energy Materials},
number = 41,
volume = 12,
place = {United States},
year = {Thu Sep 08 00:00:00 EDT 2022},
month = {Thu Sep 08 00:00:00 EDT 2022}
}

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