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Regulating the Hidden Solvation‐Ion‐Exchange in Concentrated Electrolytes for Stable and Safe Lithium Metal Batteries
Author(s) -
Amine Rachid,
Liu Jianzhao,
Acznik Ilona,
Sheng Tian,
Lota Katarzyna,
Sun Hui,
Sun ChengJun,
Fic Krzysztof,
Zuo Xiaobing,
Ren Yang,
EIHady Deia Abd,
Alshitari Wael,
AlBogami Abdullah S.,
Chen Zonghai,
Amine Khalil,
Xu GuiLiang
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202000901
Subject(s) - electrolyte , polysulfide , materials science , solvation , cathode , inorganic chemistry , dissolution , lithium (medication) , anode , chemical engineering , battery (electricity) , solvent , chemistry , organic chemistry , electrode , medicine , power (physics) , physics , quantum mechanics , engineering , endocrinology
Lithium–sulfur batteries are attractive for automobile and grid applications due to their high theoretical energy density and the abundance of sulfur. Despite the significant progress in cathode development, lithium metal degradation and the polysulfide shuttle remain two critical challenges in the practical application of Li–S batteries. Development of advanced electrolytes has become a promising strategy to simultaneously suppress lithium dendrite formation and prevent polysulfide dissolution. Here, a new class of concentrated siloxane‐based electrolytes, demonstrating significantly improved performance over the widely investigated ether‐based electrolytes are reported in terms of stabilizing the sulfur cathode and Li metal anode as well as minimizing flammability. Through a combination of experimental and computational investigation, it is found that siloxane solvents can effectively regulate a hidden solvation‐ion‐exchange process in the concentrated electrolytes that results from the interactions between cations/anions (e.g., Li + , TFSI − , and S 2− ) and solvents. As a result, it could invoke a quasi‐solid‐solid lithiation and enable reversible Li plating/stripping and robust solid‐electrolyte interphase chemistries. The solvation‐ion‐exchange process in the concentrated electrolytes is a key factor in understanding and designing electrolytes for other high‐energy lithium metal batteries.

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