Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

Yuwei ZHAO; Donghong WANG; Xinliang LI; Qi YANG; Ying GUO; Funian MO; Qing LI; Chengxin PENG; Hongfei LI; Chunyi ZHI

doi:10.1002/adma.202003070

Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

Yuwei ZHAO, Donghong WANG, Xinliang LI, Qi YANG, Ying GUO, Funian MO, Qing LI, Chengxin PENG, Hongfei LI, Chunyi ZHI

Research output: Journal Publications › Journal Article (refereed) › peer-review

104 Citations (Scopus)

Abstract

Sulfur cathodes have been under intensive study in various systems, such as Li/S, Na/S, Mg/S, and Al/S batteries. However, to date, Zn/S chemistry has never been reported. The first reliable aqueous Zn/polysulfide system activated by a “liquid film” comprising 4-(3-butyl-1-imidazolio)-1-butanesulfoni ionic liquid (IL) encapsulated within PEDOT:PSS. CF₃SO₃⁻ anions in the IL operating as Zn²⁺-transfer channels is reported. Moreover, the PEDOT:PSS network retains the IL, which renders Zn²⁺-transfer channels and a polysulfide cathode with enhanced structural stability. The Zn/polysulfide system delivers extraordinary capacity of 1148 mAh g⁻¹ and overwhelming energy density of 724.7 Wh kg⁻¹_cathode at 0.3 Ag⁻¹. During the discharging phase, S₆²⁻ is dominantly reduced by Zn to S²⁻ (S₆ → S²⁻). During the charging phase, these short chains are oxidized to form long-chain Zn_xLi_yS_3-6. A further optimized high-concentrated salt electrolyte is used to improve the reversibility of the battery, demonstrating an extended lifetime over 1600 cycles at 1 Ag⁻¹ with a capacity retention of 204 mAh g⁻¹. This facile approach and the superior performance of the developed aqueous Zn/S chemistry provide a new platform for sulfur-based battery and potentially solve the problems of other metal/sulfur batteries.

Original language	English
Article number	2003070
Number of pages	9
Journal	Advanced Materials
Volume	32
Issue number	32
Early online date	28 Jun 2020
DOIs	https://doi.org/10.1002/adma.202003070
Publication status	Published - 13 Aug 2020
Externally published	Yes

Bibliographical note

This research was supported by the National Key R&D Program of China under Project 2019YFA0705104. The work was also partially sponsored by the National Natural Science Foundation of China (21875141), the Shanghai Pujiang Program (18PJ1409000), the Guangdong Innovative and Entrepreneurial Research Team Program (Grant No. 2016ZT06G578), and a grant from City University of Hong Kong (9667165).

Keywords

aqueous batteries
ionic liquid films
sulfur cathodes
zinc ion batteries
zinc/sulfur batteries

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10.1002/adma.202003070

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title = "Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”",

abstract = "Sulfur cathodes have been under intensive study in various systems, such as Li/S, Na/S, Mg/S, and Al/S batteries. However, to date, Zn/S chemistry has never been reported. The first reliable aqueous Zn/polysulfide system activated by a “liquid film” comprising 4-(3-butyl-1-imidazolio)-1-butanesulfoni ionic liquid (IL) encapsulated within PEDOT:PSS. CF3SO3− anions in the IL operating as Zn2+-transfer channels is reported. Moreover, the PEDOT:PSS network retains the IL, which renders Zn2+-transfer channels and a polysulfide cathode with enhanced structural stability. The Zn/polysulfide system delivers extraordinary capacity of 1148 mAh g−1 and overwhelming energy density of 724.7 Wh kg−1cathode at 0.3 Ag−1. During the discharging phase, S62− is dominantly reduced by Zn to S2− (S6 → S2−). During the charging phase, these short chains are oxidized to form long-chain ZnxLiyS3-6. A further optimized high-concentrated salt electrolyte is used to improve the reversibility of the battery, demonstrating an extended lifetime over 1600 cycles at 1 Ag−1 with a capacity retention of 204 mAh g−1. This facile approach and the superior performance of the developed aqueous Zn/S chemistry provide a new platform for sulfur-based battery and potentially solve the problems of other metal/sulfur batteries. ",

keywords = "aqueous batteries, ionic liquid films, sulfur cathodes, zinc ion batteries, zinc/sulfur batteries",

author = "Yuwei ZHAO and Donghong WANG and Xinliang LI and Qi YANG and Ying GUO and Funian MO and Qing LI and Chengxin PENG and Hongfei LI and Chunyi ZHI",

note = "This research was supported by the National Key R&D Program of China under Project 2019YFA0705104. The work was also partially sponsored by the National Natural Science Foundation of China (21875141), the Shanghai Pujiang Program (18PJ1409000), the Guangdong Innovative and Entrepreneurial Research Team Program (Grant No. 2016ZT06G578), and a grant from City University of Hong Kong (9667165).",

year = "2020",

month = aug,

day = "13",

doi = "10.1002/adma.202003070",

language = "English",

volume = "32",

journal = "Advanced Materials",

issn = "0935-9648",

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TY - JOUR

T1 - Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

AU - ZHAO, Yuwei

AU - WANG, Donghong

AU - LI, Xinliang

AU - YANG, Qi

AU - GUO, Ying

AU - MO, Funian

AU - LI, Qing

AU - PENG, Chengxin

AU - LI, Hongfei

AU - ZHI, Chunyi

N1 - This research was supported by the National Key R&D Program of China under Project 2019YFA0705104. The work was also partially sponsored by the National Natural Science Foundation of China (21875141), the Shanghai Pujiang Program (18PJ1409000), the Guangdong Innovative and Entrepreneurial Research Team Program (Grant No. 2016ZT06G578), and a grant from City University of Hong Kong (9667165).

PY - 2020/8/13

Y1 - 2020/8/13

N2 - Sulfur cathodes have been under intensive study in various systems, such as Li/S, Na/S, Mg/S, and Al/S batteries. However, to date, Zn/S chemistry has never been reported. The first reliable aqueous Zn/polysulfide system activated by a “liquid film” comprising 4-(3-butyl-1-imidazolio)-1-butanesulfoni ionic liquid (IL) encapsulated within PEDOT:PSS. CF3SO3− anions in the IL operating as Zn2+-transfer channels is reported. Moreover, the PEDOT:PSS network retains the IL, which renders Zn2+-transfer channels and a polysulfide cathode with enhanced structural stability. The Zn/polysulfide system delivers extraordinary capacity of 1148 mAh g−1 and overwhelming energy density of 724.7 Wh kg−1cathode at 0.3 Ag−1. During the discharging phase, S62− is dominantly reduced by Zn to S2− (S6 → S2−). During the charging phase, these short chains are oxidized to form long-chain ZnxLiyS3-6. A further optimized high-concentrated salt electrolyte is used to improve the reversibility of the battery, demonstrating an extended lifetime over 1600 cycles at 1 Ag−1 with a capacity retention of 204 mAh g−1. This facile approach and the superior performance of the developed aqueous Zn/S chemistry provide a new platform for sulfur-based battery and potentially solve the problems of other metal/sulfur batteries.

AB - Sulfur cathodes have been under intensive study in various systems, such as Li/S, Na/S, Mg/S, and Al/S batteries. However, to date, Zn/S chemistry has never been reported. The first reliable aqueous Zn/polysulfide system activated by a “liquid film” comprising 4-(3-butyl-1-imidazolio)-1-butanesulfoni ionic liquid (IL) encapsulated within PEDOT:PSS. CF3SO3− anions in the IL operating as Zn2+-transfer channels is reported. Moreover, the PEDOT:PSS network retains the IL, which renders Zn2+-transfer channels and a polysulfide cathode with enhanced structural stability. The Zn/polysulfide system delivers extraordinary capacity of 1148 mAh g−1 and overwhelming energy density of 724.7 Wh kg−1cathode at 0.3 Ag−1. During the discharging phase, S62− is dominantly reduced by Zn to S2− (S6 → S2−). During the charging phase, these short chains are oxidized to form long-chain ZnxLiyS3-6. A further optimized high-concentrated salt electrolyte is used to improve the reversibility of the battery, demonstrating an extended lifetime over 1600 cycles at 1 Ag−1 with a capacity retention of 204 mAh g−1. This facile approach and the superior performance of the developed aqueous Zn/S chemistry provide a new platform for sulfur-based battery and potentially solve the problems of other metal/sulfur batteries.

KW - aqueous batteries

KW - ionic liquid films

KW - sulfur cathodes

KW - zinc ion batteries

KW - zinc/sulfur batteries

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U2 - 10.1002/adma.202003070

DO - 10.1002/adma.202003070

M3 - Journal Article (refereed)

AN - SCOPUS:85087219429

SN - 0935-9648

VL - 32

JO - Advanced Materials

JF - Advanced Materials

IS - 32

M1 - 2003070

ER -

Initiating a Reversible Aqueous Zn/Sulfur Battery through a “Liquid Film”

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