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

Gao, Yue; Zhao, Yuming; Li, Yuguang C.; Huang, Qingquan; Mallouk, Thomas E.; Wang, Donghai

doi:10.1021/jacs.7b06437

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

Journal Article · Fri Oct 06 00:00:00 EDT 2017 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.7b06437· OSTI ID:1435966

^[1]; Zhao, Yuming ^[2];

^[1]; Huang, Qingquan ^[2];

^[1];

^[2]

Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemistry
Pennsylvania State Univ., University Park, PA (United States). Dept. of Mechanical and Nuclear Engineering

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_0.3O₂ 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.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)

Grant/Contract Number:: EE0007795; DMR-1306938

OSTI ID:: 1435966

Alternate ID(s):: OSTI ID: 1430271

Report Number(s):: DOE-PENNSTATE-0007795; PII:974

Journal Information:: Journal of the American Chemical Society, Vol. 139, Issue 43; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 218 works

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Robust Pinhole-free Li ₃ N Solid Electrolyte Grown from Molten Lithium Li, Yanbin; Sun, Yongming; Pei, Allen ACS Central Science, Vol. 4, Issue 1 https://doi.org/10.1021/acscentsci.7b00480	journal	December 2017

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