Superhigh Coulombic Efficiency Lithium–Sulfur Batteries Enabled by In Situ Coating Lithium Sulfide with Polymerizable Electrolyte Additive

The polysulfide shuttling and electrode structure destruction caused by heterogeneous conversion reactions are the fundamental causes of the poor reversibility of high‐energy‐density lithium–sulfur (Li–S) batteries. The most direct manifestation is the unsatisfactory low Coulombic efficiency (CE). H...

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Bibliographic Details
Published in:Advanced energy materials 2023-04, Vol.13 (15), p.n/a
Main Authors: Geng, Chuannan, Qu, Wenjia, Han, Zhiyuan, Wang, Li, Lv, Wei, Yang, Quan‐Hong
Format: Article
Language:English
Subjects:
Additives
catalysis
Cathodes
Coating
Cycles
Electrolytes
Electrolytic cells
interfacial coating
Li 2S cathodes
Lithium
Lithium sulfur batteries
organosulfides
Polymerization
Polysulfides
Sulfur
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Summary:The polysulfide shuttling and electrode structure destruction caused by heterogeneous conversion reactions are the fundamental causes of the poor reversibility of high‐energy‐density lithium–sulfur (Li–S) batteries. The most direct manifestation is the unsatisfactory low Coulombic efficiency (CE). Herein the importance of CE in evaluating Li–S batteries is highlighted and a remedy is presented for such low efficiencies by in situ coating lithium sulfide (Li2S), as the cathode, with polymerizable electrolyte additives, where trithiocyanuric acid trilithium salt (TTCA‐Li) is employed for a typical demonstration. The involved reaction catalytically decreases the initial overpotential of Li2S, and the produced coating confines the shuttling of lithium polysulfides, thus inhibiting the redistribution of sulfur species and active sulfur loss upon cycling. The prototype full cell where the coated Li2S cathode couples with the Li anode has an extremely high CE of over 99.5%, while, in a Li‐free cell, the Li2S cathode well matches the lithiated silicon anode in a low N/P ratio of 1.2. This approach shows its practicality and generality through a pouch cell demonstration with a practically high Li2S loading and the extension to elemental sulfur‐based batteries by injecting the TTCA‐Li additives into cycling cells. An electrolyte modification strategy is proposed to achieve high Coulombic efficiency sulfur‐based cathodes by interfacially coating lithium sulfide with organosulfides as in situ polymerized additives. The involved reaction catalytically decreases the initial overpotential of Li2S, and the produced coating confines the shuttling of lithium polysulfides, thus inhibiting the redistribution of sulfur species and active sulfur loss upon cycling.
ISSN:1614-6832
1614-6840
DOI:10.1002/aenm.202204246