Construction of stable solid electrolyte interphase on lithium anode for long-cycling solid-state lithium–sulfur batteries

Lithium sulfur batteries (LSBs) are promising next-generation rechargeable batteries due to the high gravimetric energy, low cost, abundance, nontoxicity, and high sustainability of sulfur. However, the dissolution of high-order polysulfide in electrolytes and low Coulombic efficiency of Li anode require excess electrolytes and Li metal, which significantly reduce the energy density of LSBs. Quasi-solid-state LSBs, where sulfur is encapsulated in the micropores of carbon matrix and sealed by solid electrolyte interphase, can operate under lean electrolyte conditions, but a low sulfur loading in carbon matrix (<40 wt %) and low sulfur unitization (<70%) still limit the energy density in a cell level. Here, we significantly increase the sulfur loading in carbon to 60 wt % and sulfur utilization to ∼87% by dispersing sulfur in an oxygen-rich dense carbon host at a molecular level through strong chemical interactions of C–S and O–S. In an all-fluorinated organic lean electrolyte, the C/S cathode experiences a solid-state lithiation/delithiation reaction after the formation of solid electrolyte interphase in the first deep lithiation, completely avoiding the shuttle reaction. The chemically stabilized C/S composite retains a high reversible capacity of 541 mAh⋅g−1(based on the total weight of the C/S composite) for 200 cycles under lean electrolyte conditions, corresponding to a high energy density of 974 Wh⋅kg−1. The superior electrochemical performance of the chemical bonding-stabilized C/S composite renders it a promising cathode material for high-energy and long-cycle-life LSBs.

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High Capacity and Superior Cyclic Performances of All-Solid-State Lithium–Sulfur Batteries Enabled by a High-Conductivity Li10SnP2S12 Solid Electrolyte

ACS Applied Materials & Interfaces ◽

10.1021/acsami.9b12846 ◽

2019 ◽

Vol 11 (40) ◽

pp. 36774-36781 ◽

Cited By ~ 12

Author(s):

Jingguang Yi ◽

Long Chen ◽

Yongchang Liu ◽

Hongxia Geng ◽

Li-Zhen Fan

Keyword(s):

Solid State ◽

Solid Electrolyte ◽

High Capacity ◽

High Conductivity ◽

Lithium Sulfur Batteries ◽

Lithium Sulfur

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Mastering the interface for advanced all-solid-state lithium rechargeable batteries

Proceedings of the National Academy of Sciences ◽

10.1073/pnas.1615912113 ◽

2016 ◽

Vol 113 (47) ◽

pp. 13313-13317 ◽

Cited By ~ 138

Author(s):

Yutao Li ◽

Weidong Zhou ◽

Xi Chen ◽

Xujie Lü ◽

Zhiming Cui ◽

...

Keyword(s):

Solid State ◽

Solid Electrolyte ◽

Solid Electrolyte Interphase ◽

Rechargeable Batteries ◽

Ion Conductivity ◽

Rhombohedral Structure ◽

Interfacial Resistance ◽

Lithium Anode ◽

Metal Anode ◽

Li Ion

A solid electrolyte with a high Li-ion conductivity and a small interfacial resistance against a Li metal anode is a key component in all-solid-state Li metal batteries, but there is no ceramic oxide electrolyte available for this application except the thin-film Li-P oxynitride electrolyte; ceramic electrolytes are either easily reduced by Li metal or penetrated by Li dendrites in a short time. Here, we introduce a solid electrolyte LiZr2(PO4)3 with rhombohedral structure at room temperature that has a bulk Li-ion conductivity σLi = 2 × 10−4 S⋅cm−1 at 25 °C, a high electrochemical stability up to 5.5 V versus Li+/Li, and a small interfacial resistance for Li+ transfer. It reacts with a metallic lithium anode to form a Li+-conducting passivation layer (solid-electrolyte interphase) containing Li3P and Li8ZrO6 that is wet by the lithium anode and also wets the LiZr2(PO4)3 electrolyte. An all-solid-state Li/LiFePO4 cell with a polymer catholyte shows good cyclability and a long cycle life.

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