Long-Cycling Lithium-Sulfur Batteries Enabled by Reactivating Inactive Lithium

Li Ling Su; Mu Xuan Wu; Shu Yu Sun; Chen Xi Bi; Zhao Zheng; Meng Zhao; Bo Quan Li; Xue Qiang Zhang; Jia Qi Huang

doi:10.1021/acsenergylett.4c03177

Long-Cycling Lithium-Sulfur Batteries Enabled by Reactivating Inactive Lithium

Li Ling Su, Mu Xuan Wu, Shu Yu Sun, Chen Xi Bi, Zhao Zheng, Meng Zhao, Bo Quan Li, Xue Qiang Zhang^*, Jia Qi Huang

^*Corresponding author for this work

Advanced Research Institute of Multidisciplinary Science

Research output: Contribution to journal › Article › peer-review

Abstract

High-energy-density lithium-sulfur (Li-S) batteries are attractive but hindered by short cycle life. The formation and accumulation of inactive Li deteriorate the battery stability. Herein, a phenethylamine (PEA) additive is proposed to reactivate inactive Li in Li-S batteries with encapsulating lithium-polysulfide electrolytes (EPSE) without sacrificing the battery Coulombic efficiency (CE). PEA undergoes reactions with inactive Li to form organic polysulfide R-LiPEA in a reduction state at the anode side and subsequently reacts with the S cathode to generate O-LiPEA in an oxidation state. R-LiPEA and O-LiPEA engage in redox cycles to reactivate inactive Li that accumulates in batteries. Compared with 122 cycles based on EPSE without PEA, Li-S batteries with PEA additive in EPSE achieve 185 cycles under demanding conditions and maintain higher CE of 96% with PEA than 93% without PEA. This work elucidates the ingenious modification of amino-based additives to reactivate inactive Li by an organic polysulfide redox mechanism for advanced Li-S batteries.

Original language	English
Pages (from-to)	313-319
Number of pages	7
Journal	ACS Energy Letters
Volume	10
Issue number	1
DOIs	https://doi.org/10.1021/acsenergylett.4c03177
Publication status	Published - 10 Jan 2025

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10.1021/acsenergylett.4c03177

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@article{02c8dd8fdda9422486ef6b93c50a3f9a,

title = "Long-Cycling Lithium-Sulfur Batteries Enabled by Reactivating Inactive Lithium",

abstract = "High-energy-density lithium-sulfur (Li-S) batteries are attractive but hindered by short cycle life. The formation and accumulation of inactive Li deteriorate the battery stability. Herein, a phenethylamine (PEA) additive is proposed to reactivate inactive Li in Li-S batteries with encapsulating lithium-polysulfide electrolytes (EPSE) without sacrificing the battery Coulombic efficiency (CE). PEA undergoes reactions with inactive Li to form organic polysulfide R-LiPEA in a reduction state at the anode side and subsequently reacts with the S cathode to generate O-LiPEA in an oxidation state. R-LiPEA and O-LiPEA engage in redox cycles to reactivate inactive Li that accumulates in batteries. Compared with 122 cycles based on EPSE without PEA, Li-S batteries with PEA additive in EPSE achieve 185 cycles under demanding conditions and maintain higher CE of 96% with PEA than 93% without PEA. This work elucidates the ingenious modification of amino-based additives to reactivate inactive Li by an organic polysulfide redox mechanism for advanced Li-S batteries.",

author = "Su, {Li Ling} and Wu, {Mu Xuan} and Sun, {Shu Yu} and Bi, {Chen Xi} and Zhao Zheng and Meng Zhao and Li, {Bo Quan} and Zhang, {Xue Qiang} and Huang, {Jia Qi}",

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doi = "10.1021/acsenergylett.4c03177",

language = "English",

volume = "10",

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T1 - Long-Cycling Lithium-Sulfur Batteries Enabled by Reactivating Inactive Lithium

AU - Su, Li Ling

AU - Wu, Mu Xuan

AU - Sun, Shu Yu

AU - Bi, Chen Xi

AU - Zheng, Zhao

AU - Zhao, Meng

AU - Li, Bo Quan

AU - Zhang, Xue Qiang

AU - Huang, Jia Qi

PY - 2025/1/10

Y1 - 2025/1/10

N2 - High-energy-density lithium-sulfur (Li-S) batteries are attractive but hindered by short cycle life. The formation and accumulation of inactive Li deteriorate the battery stability. Herein, a phenethylamine (PEA) additive is proposed to reactivate inactive Li in Li-S batteries with encapsulating lithium-polysulfide electrolytes (EPSE) without sacrificing the battery Coulombic efficiency (CE). PEA undergoes reactions with inactive Li to form organic polysulfide R-LiPEA in a reduction state at the anode side and subsequently reacts with the S cathode to generate O-LiPEA in an oxidation state. R-LiPEA and O-LiPEA engage in redox cycles to reactivate inactive Li that accumulates in batteries. Compared with 122 cycles based on EPSE without PEA, Li-S batteries with PEA additive in EPSE achieve 185 cycles under demanding conditions and maintain higher CE of 96% with PEA than 93% without PEA. This work elucidates the ingenious modification of amino-based additives to reactivate inactive Li by an organic polysulfide redox mechanism for advanced Li-S batteries.

AB - High-energy-density lithium-sulfur (Li-S) batteries are attractive but hindered by short cycle life. The formation and accumulation of inactive Li deteriorate the battery stability. Herein, a phenethylamine (PEA) additive is proposed to reactivate inactive Li in Li-S batteries with encapsulating lithium-polysulfide electrolytes (EPSE) without sacrificing the battery Coulombic efficiency (CE). PEA undergoes reactions with inactive Li to form organic polysulfide R-LiPEA in a reduction state at the anode side and subsequently reacts with the S cathode to generate O-LiPEA in an oxidation state. R-LiPEA and O-LiPEA engage in redox cycles to reactivate inactive Li that accumulates in batteries. Compared with 122 cycles based on EPSE without PEA, Li-S batteries with PEA additive in EPSE achieve 185 cycles under demanding conditions and maintain higher CE of 96% with PEA than 93% without PEA. This work elucidates the ingenious modification of amino-based additives to reactivate inactive Li by an organic polysulfide redox mechanism for advanced Li-S batteries.

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DO - 10.1021/acsenergylett.4c03177

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EP - 319

JO - ACS Energy Letters

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IS - 1

ER -

Long-Cycling Lithium-Sulfur Batteries Enabled by Reactivating Inactive Lithium

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