Structure and Interface Design Enable Stable Li-Rich Cathode
Abstract
Li-rich layered-oxide cathodes have the highest theoretical energy density among all the intercalated cathodes, which have attracted intense interests for high energy Li-ion batteries. However, O3-structured layered-oxide cathodes suffer from a low initial Coulombic efficiency (CE), severe voltage fade, and poor cycling stability because of the continuous oxygen release, structural rearrangements due to irreversible transition-metal migration, and serious side reactions between the delithiated cathode and electrolyte. In this work, we report that these challenges are migrated by using a stable O2-structured Li1.2Ni0.13Co0.13Mn0.54O2 (O2-LR-NCM) and all-fluorinated electrolyte. The O2-LR-NCM can restrict the transition metals migrating into the Li layer and the in situ formed fluorinated cathode electrolyte interphase (CEI) on the surface of the O2-LR-NCM from the decomposition of all-fluorinated electrolyte during initial cycles effectively restrains the structure transition, suppresses the O2 release, and thereby safeguards the transition metal redox couples, enabling a highly reversible and stable oxygen redox reaction. O2-LR-NCM in all fluorinated electrolytes achieves a high initial CE of 99.82 % and cycling CE of and cycling CE of >99.9%, high reversible capacity of 278 mAh/g, and high capacity retention of 83.3% after 100 cycles. The synergic design of electrolyte and cathode structure represents a promising direction to stabilizemore »
- Authors:
-
- Univ. of Maryland, College Park, MD (United States)
- Zhejiang Univ., Hangzhou (China)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); national Science Foundation (NSF)
- OSTI Identifier:
- 1616447
- Report Number(s):
- BNL-215884-2020-JAAM
Journal ID: ISSN 0002-7863
- Grant/Contract Number:
- SC0012704; EE0008200
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of the American Chemical Society
- Additional Journal Information:
- Journal Volume: 142; Journal Issue: 19; Journal ID: ISSN 0002-7863
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; Li-rich cathodes; O2-structure; fluorinated CEI; high initial Columbic efficiency; little voltage fade
Citation Formats
Cui, Chunyu, Fan, Xiulin, Zhou, Xiuquan, Chen, Ji, Wang, Qinchao, Ma, Lu, Yang, Chongyin, Hu, Enyuan, Yang, Xiao-Qing, and Wang, Chunsheng. Structure and Interface Design Enable Stable Li-Rich Cathode. United States: N. p., 2020.
Web. doi:10.1021/jacs.0c02302.
Cui, Chunyu, Fan, Xiulin, Zhou, Xiuquan, Chen, Ji, Wang, Qinchao, Ma, Lu, Yang, Chongyin, Hu, Enyuan, Yang, Xiao-Qing, & Wang, Chunsheng. Structure and Interface Design Enable Stable Li-Rich Cathode. United States. https://doi.org/10.1021/jacs.0c02302
Cui, Chunyu, Fan, Xiulin, Zhou, Xiuquan, Chen, Ji, Wang, Qinchao, Ma, Lu, Yang, Chongyin, Hu, Enyuan, Yang, Xiao-Qing, and Wang, Chunsheng. Wed .
"Structure and Interface Design Enable Stable Li-Rich Cathode". United States. https://doi.org/10.1021/jacs.0c02302. https://www.osti.gov/servlets/purl/1616447.
@article{osti_1616447,
title = {Structure and Interface Design Enable Stable Li-Rich Cathode},
author = {Cui, Chunyu and Fan, Xiulin and Zhou, Xiuquan and Chen, Ji and Wang, Qinchao and Ma, Lu and Yang, Chongyin and Hu, Enyuan and Yang, Xiao-Qing and Wang, Chunsheng},
abstractNote = {Li-rich layered-oxide cathodes have the highest theoretical energy density among all the intercalated cathodes, which have attracted intense interests for high energy Li-ion batteries. However, O3-structured layered-oxide cathodes suffer from a low initial Coulombic efficiency (CE), severe voltage fade, and poor cycling stability because of the continuous oxygen release, structural rearrangements due to irreversible transition-metal migration, and serious side reactions between the delithiated cathode and electrolyte. In this work, we report that these challenges are migrated by using a stable O2-structured Li1.2Ni0.13Co0.13Mn0.54O2 (O2-LR-NCM) and all-fluorinated electrolyte. The O2-LR-NCM can restrict the transition metals migrating into the Li layer and the in situ formed fluorinated cathode electrolyte interphase (CEI) on the surface of the O2-LR-NCM from the decomposition of all-fluorinated electrolyte during initial cycles effectively restrains the structure transition, suppresses the O2 release, and thereby safeguards the transition metal redox couples, enabling a highly reversible and stable oxygen redox reaction. O2-LR-NCM in all fluorinated electrolytes achieves a high initial CE of 99.82 % and cycling CE of and cycling CE of >99.9%, high reversible capacity of 278 mAh/g, and high capacity retention of 83.3% after 100 cycles. The synergic design of electrolyte and cathode structure represents a promising direction to stabilize high-energy cathodes.},
doi = {10.1021/jacs.0c02302},
journal = {Journal of the American Chemical Society},
number = 19,
volume = 142,
place = {United States},
year = {Wed Apr 22 00:00:00 EDT 2020},
month = {Wed Apr 22 00:00:00 EDT 2020}
}
Web of Science
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