An Inorganic-Rich Solid Electrolyte Interphase for Advanced Lithium-Metal Batteries in Carbonate Electrolytes

Liu, Sufu; Ji, Xiao; Piao, Nan; Chen, Ji; Eidson, Nico; Xu, Jijian; Wang, Pengfei; Chen, Long; Zhang, Jiaxun; Deng, Tao; Hou, Singyuk; Jin, Ting; Wan, Hongli; Li, Jingru; Tu, Jiangping; Wang, Chunsheng

doi:10.1002/anie.202012005

An Inorganic-Rich Solid Electrolyte Interphase for Advanced Lithium-Metal Batteries in Carbonate Electrolytes

Journal Article · Mon Nov 09 00:00:00 EST 2020 · Angewandte Chemie (International Edition)

DOI:https://doi.org/10.1002/anie.202012005· OSTI ID:1848706

Liu, Sufu ^[1]; Ji, Xiao ^[2]; Piao, Nan ^[2]; Chen, Ji ^[2]; Eidson, Nico ^[2]; Xu, Jijian ^[2]; Wang, Pengfei ^[2]; Chen, Long ^[2]; Zhang, Jiaxun ^[2]; Deng, Tao ^[2]; Hou, Singyuk ^[2]; Jin, Ting ^[2]; Wan, Hongli ^[2]; Li, Jingru ^[3]; Tu, Jiangping ^[3]; ^[2]

University of Maryland, College Park, MD (United States); University of Maryland
University of Maryland, College Park, MD (United States)
Zhejiang University, Hangzhou (China)

In carbonate electrolytes, the organic-inorganic solid electrolyte interphase (SEI) formed on the lithium (Li) metal anode surface is strongly bonded to Li and experiences the same volume change as Li, thus it undergoes continuous cracking/reformation during plating/stripping cycles. Here we report, an inorganic-rich SEI is designed on a Li metal surface to reduce its bonding energy with Li metal by dissolving 4 M concentrated LiNO₃ in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene carbonate (FEC) based electrolyte. Due to the aggregate structure of NO₃^- ions and its participation in the primary Li⁺ solvation sheath, abundant Li₂O, Li₃N, and LiN_xO_y grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF₆^- ions. The inorganic-rich SEI’s weak bonding (high interface energy) to Li can effectively promote Li diffusion along the SEI/Li interface and prevent Li dendrite penetration into the SEI. As a result, our designed carbonate electrolyte enables a Li anode to achieve a high Li plating/stripping CE of 99.55% (1 mA cm^-2, 1.0 mAh cm^-2) and the electrolyte also enables a Li||LiNi_0.8Co_0.1Mn_0.1O₂(NMC811) full cell (2.5 mAh cm^-2) to retain 75%of its initial capacity after 200 cycles with an outstanding CE of 99.83%.

View Accepted Manuscript (DOE)

Research Organization:: University of Maryland, College Park, MD (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0008202

OSTI ID:: 1848706

Alternate ID(s):: OSTI ID: 1786166
OSTI ID: 22982342

Journal Information:: Angewandte Chemie (International Edition), Journal Name: Angewandte Chemie (International Edition) Journal Issue: 7 Vol. 60; ISSN 1433-7851

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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An Inorganic-Rich Solid Electrolyte Interphase for Advanced Lithium-Metal Batteries in Carbonate Electrolytes

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