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An Inorganic‐Rich Solid Electrolyte Interphase for Advanced Lithium‐Metal Batteries in Carbonate Electrolytes
Author(s) -
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
Publication year - 2021
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.202012005
Subject(s) - electrolyte , ethylene carbonate , faraday efficiency , anode , dimethyl carbonate , inorganic chemistry , chemistry , metal , dissolution , propylene carbonate , carbonate , chemical engineering , materials science , electrode , organic chemistry , catalysis , engineering
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 %.