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Title: Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility

Abstract

Leveraging the most recent success in expanding the electrochemical stability window of aqueous electrolytes, in this work we create a unique Li-ion/sulfur chemistry of both high energy density and safety. We show that in the superconcentrated aqueous electrolyte, lithiation of sulfur experiences phase change from a high-order polysulfide to low-order polysulfides through solid–liquid two-phase reaction pathway, where the liquid polysulfide phase in the sulfide electrode is thermodynamically phase-separated from the superconcentrated aqueous electrolyte. The sulfur with solid–liquid two-phase exhibits a reversible capacity of 1,327 mAh/(g of S), along with fast reaction kinetics and negligible polysulfide dissolution. By coupling a sulfur anode with different Li-ion cathode materials, the aqueous Li-ion/sulfur full cell delivers record-high energy densities up to 200 Wh/(kg of total electrode mass) for >1,000 cycles at ~100% coulombic efficiency. These performances already approach that of commercial lithium-ion batteries (LIBs) using a nonaqueous electrolyte, along with intrinsic safety not possessed by the latter. We conclude the excellent performance of this aqueous battery chemistry significantly promotes the practical possibility of aqueous LIBs in large-format applications.

Authors:
; ; ; ; ; ; ORCiD logo; ; ; ; ;
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); National Aeronautics and Space Administration (NASA)
OSTI Identifier:
1360993
Alternate Identifier(s):
OSTI ID: 1406903
Grant/Contract Number:  
AC02-06CH11357; AR0000389
Resource Type:
Journal Article: Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; water-in-salt; rechargeable aqueous battery; aqueous sulfur battery; gel polymer electrolyte; phase separation

Citation Formats

Yang, Chongyin, Suo, Liumin, Borodin, Oleg, Wang, Fei, Sun, Wei, Gao, Tao, Fan, Xiulin, Hou, Singyuk, Ma, Zhaohui, Amine, Khalil, Xu, Kang, and Wang, Chunsheng. Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility. United States: N. p., 2017. Web. doi:10.1073/pnas.1703937114.
Yang, Chongyin, Suo, Liumin, Borodin, Oleg, Wang, Fei, Sun, Wei, Gao, Tao, Fan, Xiulin, Hou, Singyuk, Ma, Zhaohui, Amine, Khalil, Xu, Kang, & Wang, Chunsheng. Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility. United States. https://doi.org/10.1073/pnas.1703937114
Yang, Chongyin, Suo, Liumin, Borodin, Oleg, Wang, Fei, Sun, Wei, Gao, Tao, Fan, Xiulin, Hou, Singyuk, Ma, Zhaohui, Amine, Khalil, Xu, Kang, and Wang, Chunsheng. 2017. "Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility". United States. https://doi.org/10.1073/pnas.1703937114.
@article{osti_1360993,
title = {Unique aqueous Li-ion/sulfur chemistry with high energy density and reversibility},
author = {Yang, Chongyin and Suo, Liumin and Borodin, Oleg and Wang, Fei and Sun, Wei and Gao, Tao and Fan, Xiulin and Hou, Singyuk and Ma, Zhaohui and Amine, Khalil and Xu, Kang and Wang, Chunsheng},
abstractNote = {Leveraging the most recent success in expanding the electrochemical stability window of aqueous electrolytes, in this work we create a unique Li-ion/sulfur chemistry of both high energy density and safety. We show that in the superconcentrated aqueous electrolyte, lithiation of sulfur experiences phase change from a high-order polysulfide to low-order polysulfides through solid–liquid two-phase reaction pathway, where the liquid polysulfide phase in the sulfide electrode is thermodynamically phase-separated from the superconcentrated aqueous electrolyte. The sulfur with solid–liquid two-phase exhibits a reversible capacity of 1,327 mAh/(g of S), along with fast reaction kinetics and negligible polysulfide dissolution. By coupling a sulfur anode with different Li-ion cathode materials, the aqueous Li-ion/sulfur full cell delivers record-high energy densities up to 200 Wh/(kg of total electrode mass) for >1,000 cycles at ~100% coulombic efficiency. These performances already approach that of commercial lithium-ion batteries (LIBs) using a nonaqueous electrolyte, along with intrinsic safety not possessed by the latter. We conclude the excellent performance of this aqueous battery chemistry significantly promotes the practical possibility of aqueous LIBs in large-format applications.},
doi = {10.1073/pnas.1703937114},
url = {https://www.osti.gov/biblio/1360993}, journal = {Proceedings of the National Academy of Sciences of the United States of America},
issn = {0027-8424},
number = ,
volume = ,
place = {United States},
year = {Wed May 31 00:00:00 EDT 2017},
month = {Wed May 31 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at https://doi.org/10.1073/pnas.1703937114

Citation Metrics:
Cited by: 137 works
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