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Title: Interfacial Chemistry Regulation via a Skin-Grafting Strategy Enables High-Performance Lithium-Metal Batteries

The lithium (Li) metal anode suffers severe interfacial instability from its high reactivity toward liquid electrolytes, especially carbonate-based electrolytes, resulting in poor electrochemical performance of batteries that use 4 V high-capacity cathodes. In this paper, we report a new skin-grafting strategy that stabilizes the Li metal–liquid electrolyte interface by coating the Li metal surface with poly((N-2,2-dimethyl-1,3-dioxolane-4-methyl)-5-norbornene-exo-2,3-dicarboximide), a chemically and electrochemically active polymer layer. This layer, composed of cyclic ether groups with a stiff polycyclic main chain, serves as a grafted polymer skin on the Li metal anode not only to incorporate ether-based polymeric components into the solid-electrolyte interphase (SEI) but also to accommodate Li deposition/dissolution under the skin in a dendrite/moss-free manner. Consequently, a Li-metal battery employing a Li metal anode with the grafted skin paired with LiNi 0.5Co 0.2Mn 0.3O 2 cathode has a 90.0% capacity retention after 400 charge/discharge cycles and a capacity of 1.2 mAh/cm 2 in a carbonate-based electrolyte. Finally, this proof-of-concept study provides a new direction for regulating the interfacial chemistry of Li metal anodes and for enabling high-performance Li-metal batteries.
Authors:
ORCiD logo [1] ;  [2] ; ORCiD logo [1] ;  [2] ; ORCiD logo [1] ; ORCiD logo [2]
  1. Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemistry
  2. Pennsylvania State Univ., University Park, PA (United States). Dept. of Mechanical and Nuclear Engineering
Publication Date:
Report Number(s):
DOE-PENNSTATE-0007795
Journal ID: ISSN 0002-7863; PII:974
Grant/Contract Number:
EE0007795; DMR-1306938
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 139; Journal Issue: 43; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 42 ENGINEERING; Li-metal batteries; Li metal anodes; solid-electrolyte interphase
OSTI Identifier:
1435966

Gao, Yue, Zhao, Yuming, Li, Yuguang C., Huang, Qingquan, Mallouk, Thomas E., and Wang, Donghai. Interfacial Chemistry Regulation via a Skin-Grafting Strategy Enables High-Performance Lithium-Metal Batteries. United States: N. p., Web. doi:10.1021/jacs.7b06437.
Gao, Yue, Zhao, Yuming, Li, Yuguang C., Huang, Qingquan, Mallouk, Thomas E., & Wang, Donghai. Interfacial Chemistry Regulation via a Skin-Grafting Strategy Enables High-Performance Lithium-Metal Batteries. United States. doi:10.1021/jacs.7b06437.
Gao, Yue, Zhao, Yuming, Li, Yuguang C., Huang, Qingquan, Mallouk, Thomas E., and Wang, Donghai. 2017. "Interfacial Chemistry Regulation via a Skin-Grafting Strategy Enables High-Performance Lithium-Metal Batteries". United States. doi:10.1021/jacs.7b06437. https://www.osti.gov/servlets/purl/1435966.
@article{osti_1435966,
title = {Interfacial Chemistry Regulation via a Skin-Grafting Strategy Enables High-Performance Lithium-Metal Batteries},
author = {Gao, Yue and Zhao, Yuming and Li, Yuguang C. and Huang, Qingquan and Mallouk, Thomas E. and Wang, Donghai},
abstractNote = {The lithium (Li) metal anode suffers severe interfacial instability from its high reactivity toward liquid electrolytes, especially carbonate-based electrolytes, resulting in poor electrochemical performance of batteries that use 4 V high-capacity cathodes. In this paper, we report a new skin-grafting strategy that stabilizes the Li metal–liquid electrolyte interface by coating the Li metal surface with poly((N-2,2-dimethyl-1,3-dioxolane-4-methyl)-5-norbornene-exo-2,3-dicarboximide), a chemically and electrochemically active polymer layer. This layer, composed of cyclic ether groups with a stiff polycyclic main chain, serves as a grafted polymer skin on the Li metal anode not only to incorporate ether-based polymeric components into the solid-electrolyte interphase (SEI) but also to accommodate Li deposition/dissolution under the skin in a dendrite/moss-free manner. Consequently, a Li-metal battery employing a Li metal anode with the grafted skin paired with LiNi0.5Co0.2Mn0.3O2 cathode has a 90.0% capacity retention after 400 charge/discharge cycles and a capacity of 1.2 mAh/cm2 in a carbonate-based electrolyte. Finally, this proof-of-concept study provides a new direction for regulating the interfacial chemistry of Li metal anodes and for enabling high-performance Li-metal batteries.},
doi = {10.1021/jacs.7b06437},
journal = {Journal of the American Chemical Society},
number = 43,
volume = 139,
place = {United States},
year = {2017},
month = {10}
}