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Title: Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries

Abstract

Abstract Lithium‐rich layered oxides (LLOs) are prospective cathode materials for next‐generation lithium‐ion batteries (LIBs), but severe voltage decay and energy attenuation with cycling still hinder their practical applications. Herein, a series of full concentration gradient‐tailored agglomerated‐sphere LLOs are designed with linearly decreasing Mn and linearly increasing Ni and Co from the particle center to the surface. The gradient‐tailored LLOs exhibit noticeably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. Without any material modifications or electrolyte optimizations, the gradient‐tailored LLO with medium‐slope shows the best electrochemical performance, with a very low average voltage decay of 0.8 mV per cycle as well as a capacity retention of 88.4% within 200 cycles at 200 mA g −1 . These excellent findings are due to spinel structure suppression, electrochemical stress optimization, and Jahn‐Teller effect inhibition. Further investigation shows that the gradient‐tailored LLO reduces the thermal release percentage by as much as about 41% when the battery is charged to 4.4 V. This study provides an effective method to suppress the voltage decay of LLOs for further practical utilization in LIBs and also puts forward a bulk‐structure design strategy to prepare better electrode materials for different rechargeable batteries.

Authors:
 [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [3];  [2];  [4];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Beijing University of Technology (China)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  4. Univ. of Western Ontario, London, ON (Canada)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Beijing Natural Science Foundation; National Natural Science Foundation of China (NSFC); National Key Research and Development Program of China
OSTI Identifier:
1779193
Alternate Identifier(s):
OSTI ID: 1804220
Grant/Contract Number:  
AC02-06CH11357; JQ19003; 51622202; 21603009; 21875007; 2018YFB0104302
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 33; Journal Issue: 2; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Li-ion batteries; electrochemical stress; full concentration gradient; lithium-rich layered oxides; voltage decay

Citation Formats

Wu, Tianhao, Liu, Xiang, Zhang, Xu, Lu, Yue, Wang, Boya, Deng, Qingsong, Yang, Yubo, Wang, Errui, Lyu, Zhongtian, Li, Yaoqian, Wang, Yongtao, Lyu, Yan, He, Cunfu, Ren, Yang, Xu, Guiliang, Sun, Xueliang, Amine, Khalil, and Yu, Haijun. Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries. United States: N. p., 2020. Web. doi:10.1002/adma.202001358.
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Wu, Tianhao, Liu, Xiang, Zhang, Xu, Lu, Yue, Wang, Boya, Deng, Qingsong, Yang, Yubo, Wang, Errui, Lyu, Zhongtian, Li, Yaoqian, Wang, Yongtao, Lyu, Yan, He, Cunfu, Ren, Yang, Xu, Guiliang, Sun, Xueliang, Amine, Khalil, & Yu, Haijun. Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries. United States. https://doi.org/10.1002/adma.202001358
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Wu, Tianhao, Liu, Xiang, Zhang, Xu, Lu, Yue, Wang, Boya, Deng, Qingsong, Yang, Yubo, Wang, Errui, Lyu, Zhongtian, Li, Yaoqian, Wang, Yongtao, Lyu, Yan, He, Cunfu, Ren, Yang, Xu, Guiliang, Sun, Xueliang, Amine, Khalil, and Yu, Haijun. Mon . "Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries". United States. https://doi.org/10.1002/adma.202001358. https://www.osti.gov/servlets/purl/1779193.
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@article{osti_1779193,
title = {Full Concentration Gradient-Tailored Li-Rich Layered Oxides for High-Energy Lithium-Ion Batteries},
author = {Wu, Tianhao and Liu, Xiang and Zhang, Xu and Lu, Yue and Wang, Boya and Deng, Qingsong and Yang, Yubo and Wang, Errui and Lyu, Zhongtian and Li, Yaoqian and Wang, Yongtao and Lyu, Yan and He, Cunfu and Ren, Yang and Xu, Guiliang and Sun, Xueliang and Amine, Khalil and Yu, Haijun},
abstractNote = {Abstract Lithium‐rich layered oxides (LLOs) are prospective cathode materials for next‐generation lithium‐ion batteries (LIBs), but severe voltage decay and energy attenuation with cycling still hinder their practical applications. Herein, a series of full concentration gradient‐tailored agglomerated‐sphere LLOs are designed with linearly decreasing Mn and linearly increasing Ni and Co from the particle center to the surface. The gradient‐tailored LLOs exhibit noticeably reduced voltage decay, enhanced rate performance, improved cycle stability, and thermal stability. Without any material modifications or electrolyte optimizations, the gradient‐tailored LLO with medium‐slope shows the best electrochemical performance, with a very low average voltage decay of 0.8 mV per cycle as well as a capacity retention of 88.4% within 200 cycles at 200 mA g −1 . These excellent findings are due to spinel structure suppression, electrochemical stress optimization, and Jahn‐Teller effect inhibition. Further investigation shows that the gradient‐tailored LLO reduces the thermal release percentage by as much as about 41% when the battery is charged to 4.4 V. This study provides an effective method to suppress the voltage decay of LLOs for further practical utilization in LIBs and also puts forward a bulk‐structure design strategy to prepare better electrode materials for different rechargeable batteries.},
doi = {10.1002/adma.202001358},
journal = {Advanced Materials},
number = 2,
volume = 33,
place = {United States},
year = {Mon Nov 30 00:00:00 EST 2020},
month = {Mon Nov 30 00:00:00 EST 2020}
}
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