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

Journal Article · · Advanced Materials
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  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)
+ Show Author Affiliations

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
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
Grant/Contract Number:
AC02-06CH11357; JQ19003; 51622202; 21603009; 21875007; 2018YFB0104302
OSTI ID:
1779193
Alternate ID(s):
OSTI ID: 1804220
Journal Information:
Advanced Materials, Vol. 33, Issue 2; ISSN 0935-9648
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
Li-ion batteries
electrochemical stress
full concentration gradient
lithium-rich layered oxides
voltage decay