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Designing Cation–Solvent Fully Coordinated Electrolyte for High‐Energy‐Density Lithium–Sulfur Full Cell Based On Solid–Solid Conversion
Author(s) -
Yang Huijun,
Qiao Yu,
Chang Zhi,
He Ping,
Zhou Haoshen
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202106788
Subject(s) - electrolyte , cathode , chemistry , dissolution , inorganic chemistry , anode , polysulfide , lithium (medication) , chemical engineering , solvent , electrode , organic chemistry , medicine , engineering , endocrinology
Sulfur chemistry based on solid–liquid dissolution‐deposition route inevitably encounters shuttle of lithium polysulfides, its parasitic interaction with lithium (Li) anode and flood electrolyte environment. The sulfurized pyrolyzed poly(acrylonitrile) (S@pPAN) cathode favors solid‐solid conversion mechanism in carbonate ester electrolytes but fails to pair high‐capacity Li anode. Herein, we rationally design a cation‐solvent fully coordinated ether electrolyte to simultaneously resolve the problems of both Li anode and S@pPAN cathode. Raman spectroscopy reveals a highly suppressed solvent activity and a cation‐solvent fully coordinated structure (molar ratio 1:1). Consequently, Li electrodeposit evolves into round‐edged morphology, LiF‐rich interphase, and high reversibility. Moreover, S@pPAN cathode inherits a neat solid‐phase redox reaction and fully eliminated the dissolution of lithium polysulfides. Finally, we harvest a long‐life Li‐S@pPAN pouch cell with slight Li metal excessive (0.4 time) and ultra‐lean electrolyte design (1 μL mg S −1 ), delivering 394 Wh kg −1 energy density based on electrodes and electrolyte mass.