4.6 Article

Bifunctional Interphase-Enabled Li10GeP2S12 Electrolytes for Lithium-Sulfur Battery

期刊

ACS ENERGY LETTERS
卷 6, 期 3, 页码 862-868

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c02617

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资金

  1. National Science Foundation [1805159]
  2. U.S. Department of Energy EERE [DE-EE0008856]
  3. Div Of Chem, Bioeng, Env, & Transp Sys
  4. Directorate For Engineering [1805159] Funding Source: National Science Foundation

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By forming a lithiophilic-lithiophobic gradient interlayer interphase layer at the LGPS/Li interface, the instability of LGPS against Li and Li dendrite growth can be addressed. This rational design enhances the performance of all-solid-state lithium batteries, enabling them to exhibit high reversible capacity.
Li10GeP2S12 (LGPS) has a high ionic conductivity and compatibility with sulfur cathodes; however, the instability of LGPS against Li and Li dendrite growth still remains unsolved. Here, we solved these two challenges by forming a lithiophilic-lithiophobic gradient interlayer interphase layer between Li and LGPS through the sequential reduction of salts and solvent in Mg(TFSI)(2)-LiTFSI-DME liquid electrolyte at the LGPS/Li interface (TFSI = bis(trifluoromethanesulfonyl)imide; DME = dimethoxyethane). Mg(TFSI)(2)-LiTFSI is first reduced, forming a lithiophilic LixMg alloy-rich layer on the lithium surface and a lithiophobic LiF-rich layer on top of LixMg due to the lithiophobicity difference. The later reduced DME solvent forms a flexible organic polymer between the LiF-rich layer and LGPS. After evaporation of DME solvent, the Li/LGPS/Ni-Li2S-LiTiS2 all-solid-state battery shows a reversible capacity of 699.7 mAh g(-1) (1.07 mAh cm(-2)) based on the mass of Ni-Li2S-LiTiS2 at 100 mA g(-1) (0.26 mA cm(-2)). The rational design of a solid electrolyte interface between a Li anode and LGPS electrolyte opens a new opportunity to develop high-performance all-solid-state lithium batteries.

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