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

Yang, Chongyin; Suo, Liumin; Borodin, Oleg; Wang, Fei; Sun, Wei; Gao, Tao; Fan, Xiulin; Hou, Singyuk; Ma, Zhaohui; Amine, Khalil; Xu, Kang; Wang, Chunsheng

doi:10.1073/pnas.1703937114

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

Journal Article · Wed May 31 00:00:00 EDT 2017 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1703937114· OSTI ID:1360993

Yang, Chongyin; Suo, Liumin; Borodin, Oleg; Wang, Fei; Sun, Wei; Gao, Tao; ; Hou, Singyuk; Ma, Zhaohui; Amine, Khalil; Xu, Kang; Wang, Chunsheng

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.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Aeronautic and Space Administration (NASA); USDOE Advanced Research Projects Agency - Energy (ARPA-E)

Grant/Contract Number:: AC02-06CH11357; AR0000389

OSTI ID:: 1360993

Alternate ID(s):: OSTI ID: 1406903

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

References (40)

Recent Progress in Aqueous Lithium-Ion Batteries Wang, Yonggang; Yi, Jin; Xia, Yongyao Advanced Energy Materials, Vol. 2, Issue 7 https://doi.org/10.1002/aenm.201200065	journal	June 2012
Recent Advances in Electrolytes for Lithium-Sulfur Batteries Zhang, Shiguo; Ueno, Kazuhide; Dokko, Kaoru Advanced Energy Materials, Vol. 5, Issue 16 https://doi.org/10.1002/aenm.201500117	journal	April 2015
A High Energy Lithium-Sulfur Battery with Ultrahigh-Loading Lithium Polysulfide Cathode and its Failure Mechanism Qie, Long; Zu, Chenxi; Manthiram, Arumugam Advanced Energy Materials, Vol. 6, Issue 7 https://doi.org/10.1002/aenm.201502459	journal	February 2016
Porous Hollow Carbon@Sulfur Composites for High-Power Lithium-Sulfur Batteries Jayaprakash, N.; Shen, J.; Moganty, Surya S. Angewandte Chemie International Edition, Vol. 50, Issue 26, p. 5904-5908 https://doi.org/10.1002/anie.201100637	journal	May 2011
Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte Suo, Liumin; Borodin, Oleg; Sun, Wei Angewandte Chemie International Edition, Vol. 55, Issue 25 https://doi.org/10.1002/anie.201602397	journal	April 2016
High-voltage Zn/LiMn0.8Fe0.2PO4 aqueous rechargeable battery by virtue of “water-in-salt” electrolyte Zhao, Jingwen; Li, Yuqi; Peng, Xuan Electrochemistry Communications, Vol. 69 https://doi.org/10.1016/j.elecom.2016.05.014	journal	August 2016
Methods to obtain excellent capacity retention in LiCoO2 cycled to 4.5 V Chen, Zhaohui; Dahn, J. R. Electrochimica Acta, Vol. 49, Issue 7 https://doi.org/10.1016/j.electacta.2003.10.019	journal	March 2004
Electrochemical properties of TiP2O7 and LiTi2(PO4)3 as anode material for lithium ion battery with aqueous solution electrolyte Wang, Haibo; Huang, Kelong; Zeng, Yuqun Electrochimica Acta, Vol. 52, Issue 9 https://doi.org/10.1016/j.electacta.2006.10.010	journal	February 2007
Improvement of cycle performance of lithium ion cell LiMn2O4/LixV2O5 with aqueous solution electrolyte by polypyrrole coating on anode Wang, Haibo; Zeng, Yuqun; Huang, Kelong Electrochimica Acta, Vol. 52, Issue 15 https://doi.org/10.1016/j.electacta.2007.02.004	journal	April 2007
Systematical electrochemical study on the parasitic shuttle-effect in lithium-sulfur-cells at different temperatures and different rates Busche, Martin Rolf; Adelhelm, Philipp; Sommer, Heino Journal of Power Sources, Vol. 259 https://doi.org/10.1016/j.jpowsour.2014.02.075	journal	August 2014
In Situ Raman Spectroscopy of Sulfur Speciation in Lithium–Sulfur Batteries Wu, Heng-Liang; Huff, Laura A.; Gewirth, Andrew A. ACS Applied Materials & Interfaces, Vol. 7, Issue 3 https://doi.org/10.1021/am5072942	journal	January 2015
Lithium Batteries and Cathode Materials Whittingham, M. Stanley Chemical Reviews, Vol. 104, Issue 10, p. 4271-4302 https://doi.org/10.1021/cr020731c	journal	October 2004
Aqueous Rechargeable Li and Na Ion Batteries Kim, Haegyeom; Hong, Jihyun; Park, Kyu-Young Chemical Reviews, Vol. 114, Issue 23 https://doi.org/10.1021/cr500232y	journal	September 2014
Raman studies of sulfur-containing anions in inorganic polysulfides. Potassium polysulfides Janz, G. J.; Coutts, J. W.; Downey, J. R. Inorganic Chemistry, Vol. 15, Issue 8 https://doi.org/10.1021/ic50162a003	journal	August 1976
Solvent Effect of Room Temperature Ionic Liquids on Electrochemical Reactions in Lithium–Sulfur Batteries Park, Jun-Woo; Yamauchi, Kento; Takashima, Eriko The Journal of Physical Chemistry C, Vol. 117, Issue 9 https://doi.org/10.1021/jp400153m	journal	February 2013
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
Towards greener and more sustainable batteries for electrical energy storage Larcher, D.; Tarascon, J-M. Nature Chemistry, Vol. 7, Issue 1 https://doi.org/10.1038/nchem.2085	journal	November 2014
Raising the cycling stability of aqueous lithium-ion batteries by eliminating oxygen in the electrolyte Luo, Jia-Yan; Cui, Wang-Jun; He, Ping Nature Chemistry, Vol. 2, Issue 9 https://doi.org/10.1038/nchem.763	journal	August 2010
A zwitterionic gel electrolyte for efficient solid-state supercapacitors Peng, Xu; Liu, Huili; Yin, Qin Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms11782	journal	May 2016
Sulphur–TiO₂ yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries Wei Seh, Zhi; Li, Weiyang; Cha, Judy J. Nature Communications, Vol. 4, Article No. 1331 https://doi.org/10.1038/ncomms2327	journal	January 2013
Two-dimensional vanadyl phosphate ultrathin nanosheets for high energy density and flexible pseudocapacitors Wu, Changzheng; Lu, Xiuli; Peng, Lele Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3431	journal	September 2013
A strategic approach to recharging lithium-sulphur batteries for long cycle life Su, Yu-Sheng; Fu, Yongzhu; Cochell, Thomas Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3985	journal	December 2013
Surface-enhanced redox chemistry of polysulphides on a metallic and polar host for lithium-sulphur batteries Pang, Quan; Kundu, Dipan; Cuisinier, Marine Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5759	journal	August 2014
Two-dimensional layered transition metal disulphides for effective encapsulation of high-capacity lithium sulphide cathodes Seh, Zhi Wei; Yu, Jung Ho; Li, Weiyang Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6017	journal	September 2014
Hydrate-melt electrolytes for high-energy-density aqueous batteries Yamada, Yuki; Usui, Kenji; Sodeyama, Keitaro Nature Energy, Vol. 1, Issue 10 https://doi.org/10.1038/nenergy.2016.129	journal	August 2016
A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries Ji, Xiulei; Lee, Kyu Tae; Nazar, Linda F. Nature Materials, Vol. 8, Issue 6, p. 500-506 https://doi.org/10.1038/nmat2460	journal	May 2009
Li–O₂ and Li–S batteries with high energy storage Bruce, Peter G.; Freunberger, Stefan A.; Hardwick, Laurence J. Nature Materials, Vol. 11, Issue 1, p. 19-29 https://doi.org/10.1038/nmat3191	journal	January 2012
Single step transformation of sulphur to Li2S2/Li2S in Li-S batteries Helen, M.; Reddy, M. Anji; Diemant, Thomas Scientific Reports, Vol. 5, Issue 1 https://doi.org/10.1038/srep12146	journal	July 2015
Unique behaviour of nonsolvents for polysulphides in lithium–sulphur batteries Cuisinier, M.; Cabelguen, P. -E.; Adams, B. D. Energy Environ. Sci., Vol. 7, Issue 8 https://doi.org/10.1039/C4EE00372A	journal	January 2014
An aqueous dissolved polysulfide cathode for lithium–sulfur batteries Li, Na; Weng, Zhe; Wang, Yarong Energy Environ. Sci., Vol. 7, Issue 10 https://doi.org/10.1039/C4EE01717J	journal	January 2014
An aqueous electrolyte rechargeable Li-ion/polysulfide battery Demir-Cakan, Rezan; Morcrette, Mathieu; Leriche, Jean-Bernard J. Mater. Chem. A, Vol. 2, Issue 24 https://doi.org/10.1039/C4TA01308E	journal	January 2014
Sol–gel encapsulated lithium polysulfide catholyte and its application in lithium–sulfur batteries Smith, Leland C.; Malati, Peter; Fang, Jonathan Materials Horizons, Vol. 3, Issue 2 https://doi.org/10.1039/C5MH00228A	journal	January 2016
Exploiting XPS for the identification of sulfides and polysulfides Fantauzzi, Marzia; Elsener, Bernhard; Atzei, Davide RSC Advances, Vol. 5, Issue 93 https://doi.org/10.1039/C5RA14915K	journal	January 2015
Advances in Li–S batteries Ji, Xiulei; Nazar, Linda F. Journal of Materials Chemistry, Vol. 20, Issue 44, p. 9821-9826 https://doi.org/10.1039/b925751a	journal	January 2010
Rechargeable Lithium Batteries with Aqueous Electrolytes Li, W.; Dahn, J. R.; Wainwright, D. S. Science, Vol. 264, Issue 5162, p. 1115-1118 https://doi.org/10.1126/science.264.5162.1115	journal	May 1994
"Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries Suo, L.; Borodin, O.; Gao, T. Science, Vol. 350, Issue 6263 https://doi.org/10.1126/science.aab1595	journal	November 2015
Polysulfide Shuttle Study in the Li/S Battery System Mikhaylik, Yuriy V.; Akridge, James R. Journal of The Electrochemical Society, Vol. 151, Issue 11, p. A1969-A1976 https://doi.org/10.1149/1.1806394	journal	January 2004
Aqueous Solubilities, Solubility Products and Standard Oxidation-Reduction Potentials of the Metal Sulfides Licht, Stuart Journal of The Electrochemical Society, Vol. 135, Issue 12 https://doi.org/10.1149/1.2095471	journal	January 1988
Lithium Sulfur Battery: Oxidation/Reduction Mechanisms of Polysulfides in THF Solutions Yamin, H.; Gorenshtein, A.; Penciner, J. Journal of The Electrochemical Society, Vol. 135, Issue 5, p. 1045-1048 https://doi.org/10.1149/1.2095868	journal	January 1988
Raman Spectroscopic and X-ray Diffraction Studies of Sulfur Composite Electrodes during Discharge and Charge Yeon, Jin-Tak; Jang, Jun-Young; Han, Jung-Gu Journal of The Electrochemical Society, Vol. 159, Issue 8 https://doi.org/10.1149/2.080208jes	journal	January 2012

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