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Electrolyte Structure of Lithium Polysulfides with Anti‐Reductive Solvent Shells for Practical Lithium–Sulfur Batteries
Author(s) -
Zhang XueQiang,
Jin Qi,
Nan YiLing,
Hou LiPeng,
Li BoQuan,
Chen Xiang,
Jin ZheHui,
Zhang XiTian,
Huang JiaQi,
Zhang Qiang
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.202103470
Subject(s) - polysulfide , electrolyte , chemistry , lithium (medication) , solvent , reactivity (psychology) , battery (electricity) , anode , diglyme , ether , inorganic chemistry , chemical engineering , organic chemistry , electrode , medicine , power (physics) , physics , alternative medicine , pathology , quantum mechanics , endocrinology , engineering
The lithium–sulfur (Li–S) battery is regarded as a promising secondary battery. However, constant parasitic reactions between the Li anode and soluble polysulfide (PS) intermediates significantly deteriorate the working Li anode. The rational design to inhibit the parasitic reactions is plagued by the inability to understand and regulate the electrolyte structure of PSs. Herein, the electrolyte structure of PSs with anti‐reductive solvent shells was unveiled by molecular dynamics simulations and nuclear magnetic resonance. The reduction resistance of the solvent shell is proven to be a key reason for the decreased reactivity of PSs towards Li. With isopropyl ether (DIPE) as a cosolvent, DIPE molecules tend to distribute in the outer solvent shell due to poor solvating power. Furthermore, DIPE is more stable than conventional ether solvents against Li metal. The reactivity of PSs is suppressed by encapsulating PSs into anti‐reductive solvent shells. Consequently, the cycling performance of working Li–S batteries was significantly improved and a pouch cell of 300 Wh kg −1 was demonstrated. The fundamental understanding in this work provides an unprecedented ground to understand the electrolyte structure of PSs and the rational electrolyte design in Li–S batteries.