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/ange.202012005

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

Journal Article · Wed Dec 16 00:00:00 EST 2020 · Angewandte Chemie

DOI:https://doi.org/10.1002/ange.202012005· OSTI ID:1786223

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

Department of Chemical and Biomolecular Engineering University of Maryland College Park MD 20740 USA
State Key Laboratory of Silicon Materials Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province School of Materials Science&, Engineering Zhejiang University Hangzhou 310027 China

Abstract

In carbonate electrolytes, the organic–inorganic solid electrolyte interphase (SEI) formed on the 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, an inorganic‐rich SEI is designed on a Li‐metal surface to reduce its bonding energy with Li metal by dissolving 4 m concentrated LiNO ₃ in dimethyl sulfoxide (DMSO) as an additive for a fluoroethylene‐carbonate (FEC)‐based electrolyte. Due to the aggregate structure of NO ₃ ⁻ ions and their participation in the primary Li ⁺ solvation sheath, abundant Li ₂ O, Li ₃ N, and LiN _x O _y grains are formed in the resulting SEI, in addition to the uniform LiF distribution from the reduction of PF ₆ ⁻ ions. The weak bonding of the SEI (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 Coulombic efficiency of 99.55 % (1 mA cm ⁻² , 1.0 mAh cm ⁻² ) and the electrolyte also enables a Li||LiNi _0.8 Co _0.1 Mn _0.1 O ₂ (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 (Publisher)

Sponsoring Organization:: USDOE

OSTI ID:: 1786223

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 7 Vol. 133; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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