The Progress of Li-S Batteries-Understanding of the Sulfur Redox Mechanism: Dissolved Polysulfide Ions in the Electrolytes

Zheng, Dong; Wang, Gongwei; Liu, Dan; Si, Jingyu; Ding, Tianyao; Qu, Deyu; Yang, Xiaoqing; Qu, Deyang

doi:10.1002/admt.201700233

Title: The Progress of Li-S Batteries-Understanding of the Sulfur Redox Mechanism: Dissolved Polysulfide Ions in the Electrolytes

Journal Article · 18 June 2018 · Advanced Materials Technologies

DOI: https://doi.org/10.1002/admt.201700233 · OSTI ID:1476765

Zheng, Dong ^[1]; Wang, Gongwei ^[1]; Liu, Dan ^[2]; Si, Jingyu ^[1]; Ding, Tianyao ^[1]; Qu, Deyu ^[2];

^[3];

^[1]

Univ. of Wisconsin Milwaukee, Milwaukee, WI (United States)
Wuhan Univ. of Technology, Wuhan (People's Republic of China)
Brookhaven National Lab. (BNL), Upton, NY (United States)

Rechargeable lithium–sulfur batteries have aroused great attention in recent years. Thousands of research articles are published, and among these publications, the majority are dedicated to improving the battery's performance through chemically and physically modifying the sulfur electrode, electrolytes, separator, and lithium anode. However, the single most important aspect, understanding the sulfur redox mechanism, is sparse and overwhelmed by the huge volume of work done on improving the battery's performance. Besides the intrinsic complexity of the sulfur redox chemistry, the most challenging task is to find an effective analytical technique for the quantitative and qualitative determination of the dissolved and solid polysulfides, including elemental sulfur. In this paper, the recent important research aiming to understand the redox mechanism of the sulfur electrode is reviewed in light of the unique analytical techniques used in the research. The review re–affirms the complexity of the sulfur redox chemistry and lays the background for the future mechanistic research for Li–S batteries.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE; USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: SC0012704

OSTI ID:: 1476765

Report Number(s):: BNL-209155-2018-JAAM

Journal Information:: Advanced Materials Technologies, Journal Name: Advanced Materials Technologies Journal Issue: 9 Vol. 3; ISSN 2365-709X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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In-Situ Raman Investigation of Polysulfide Formation in Li-S Cells Hagen, M.; Schiffels, P.; Hammer, M. Journal of The Electrochemical Society, Vol. 160, Issue 8 https://doi.org/10.1149/2.045308jes	journal	January 2013
Analysis of Polysulfide Dissolved in Electrolyte in Discharge-Charge Process of Li-S Battery Diao, Yan; Xie, Kai; Xiong, Shizhao Journal of The Electrochemical Society, Vol. 159, Issue 4, p. A421-A425 https://doi.org/10.1149/2.060204jes	journal	January 2012
Understanding the Charging Mechanism of Lithium-Sulfur Batteries Using Spatially Resolved Operando X-Ray Absorption Spectroscopy Gorlin, Yelena; Patel, Manu U. M.; Freiberg, Anna Journal of The Electrochemical Society, Vol. 163, Issue 6 https://doi.org/10.1149/2.0631606jes	journal	January 2016
Fingerprinting Lithium-Sulfur Battery Reaction Products by X-ray Absorption Spectroscopy Wujcik, Kevin H.; Velasco-Velez, Juan; Wu, Cheng Hao Journal of The Electrochemical Society, Vol. 161, Issue 6 https://doi.org/10.1149/2.078406jes	journal	January 2014
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
Direct Observation of Sulfur Radicals as Reaction Media in Lithium Sulfur Batteries Wang, Qiang; Zheng, Jianming; Walter, Eric Journal of The Electrochemical Society, Vol. 162, Issue 3 https://doi.org/10.1149/2.0851503jes	journal	December 2014
Quantitative Chromatographic Determination of Dissolved Elemental Sulfur in the Non-Aqueous Electrolyte for Lithium-Sulfur Batteries Zheng, Dong; Zhang, Xuran; Li, Chao Journal of The Electrochemical Society, Vol. 162, Issue 1 https://doi.org/10.1149/2.1011501jes	journal	November 2014
Chromatographic Separation of Polysulfide Species in Non-Aqueous Electrolytes – Revisited Zheng, Dong; Qu, Deyang Journal of The Electrochemical Society, Vol. 161, Issue 6 https://doi.org/10.1149/2.114406jes	journal	January 2014
In Situ X-ray Absorption Spectroscopy Studies of Discharge Reactions in a Thick Cathode of a Lithium Sulfur Battery Wujcik, Kevin H.; Wang, Dunyang Rita; Pascal, Tod A. Journal of The Electrochemical Society, Vol. 164, Issue 2 https://doi.org/10.1149/2.1441614jes	journal	December 2016
A Novel Optical Diagnostic for In Situ Measurements of Lithium Polysulfides in Battery Electrolytes Saqib, Najmus; Silva, Cody J.; Maupin, C. Mark Applied Spectroscopy, Vol. 71, Issue 7 https://doi.org/10.1177/0003702816684638	journal	February 2017
Sulphured Polyacrylonitrile Composite Analysed by in operando UV-Visible Spectroscopy and 4-electrode Swagelok Cell Dominko, Robert; Patel, Manu U. M.; Bele, Marjan Acta Chimica Slovenica https://doi.org/10.17344/acsi.2016.2366	journal	September 2016
Recent Research Progress on Non-aqueous Lithium-Air Batteries from Argonne National Laboratory Lu, Jun; Amine, Khalil Energies, Vol. 6, Issue 11 https://doi.org/10.3390/en6116016	journal	November 2013

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“Brain‐Coral‐Like” Mesoporous Hollow CoS ₂ @N‐Doped Graphitic Carbon Nanoshells as Efficient Sulfur Reservoirs for Lithium–Sulfur Batteries Seo, Seung‐Deok; Park, Dongjoo; Park, Sangbaek Advanced Functional Materials, Vol. 29, Issue 38 https://doi.org/10.1002/adfm.201903712	journal	July 2019
Single Nickel Atoms on Nitrogen‐Doped Graphene Enabling Enhanced Kinetics of Lithium–Sulfur Batteries Zhang, Linlin; Liu, Daobin; Muhammad, Zahir Advanced Materials, Vol. 31, Issue 40 https://doi.org/10.1002/adma.201903955	journal	August 2019
Sulfur Redox Reactions at Working Interfaces in Lithium-Sulfur Batteries: A Perspective Yuan, Hong; Peng, Hong-Jie; Huang, Jia-Qi Advanced Materials Interfaces, Vol. 6, Issue 4 https://doi.org/10.1002/admi.201802046	journal	January 2019
Efficient Charging of Lithium-Sulfur Batteries by Triboelectric Nanogenerator Based on Pulse Current Yin, Yingying; Zhang, Xiuling; Du, Xinyu Advanced Materials Technologies, Vol. 4, Issue 2 https://doi.org/10.1002/admt.201800326	journal	October 2018
Multiple Nanosheets Assembled Nanoflower‐like MnO 2 to Anchor Polysulfides for Improving Electrochemical Performance in Lithium Sulfur Batteries Wang, Jianing; Li, Yanpei; Li, Wenwen ChemistrySelect, Vol. 4, Issue 24 https://doi.org/10.1002/slct.201901499	journal	June 2019
A Highly Conductive MOF of Graphene Analogue Ni ₃ (HITP) ₂ as a Sulfur Host for High‐Performance Lithium–Sulfur Batteries Cai, Dong; Lu, Mengjie; Li, La Small, Vol. 15, Issue 44 https://doi.org/10.1002/smll.201902605	journal	September 2019
The role of polysulfide dianions and radical anions in the chemical, physical and biological sciences, including sulfur-based batteries Steudel, Ralf; Chivers, Tristram Chemical Society Reviews, Vol. 48, Issue 12 https://doi.org/10.1039/c8cs00826d	journal	January 2019
Metal-based nanostructured materials for advanced lithium–sulfur batteries Balach, Juan; Linnemann, Julia; Jaumann, Tony Journal of Materials Chemistry A, Vol. 6, Issue 46 https://doi.org/10.1039/c8ta07220e	journal	January 2018
Catenated and spirocyclic polychalcogenides from potassium carbonate and elemental chalcogens Liebing, Phil; Kühling, Marcel; Swanson, Claudia Chemical Communications, Vol. 55, Issue 99 https://doi.org/10.1039/c9cc08347b	journal	January 2019
ZnS spheres wrapped by an ultrathin wrinkled carbon film as a multifunctional interlayer for long-life Li–S batteries Yang, Jin-Lin; Zhao, Shi-Xi; Lu, Yi-Ming Journal of Materials Chemistry A, Vol. 8, Issue 1 https://doi.org/10.1039/c9ta10560c	journal	January 2020
Unraveling the Correlation between Solvent Properties and Sulfur Redox Behavior in Lithium-Sulfur Batteries He, Qi; Gorlin, Yelena; Patel, Manu U. M. Journal of The Electrochemical Society, Vol. 165, Issue 16 https://doi.org/10.1149/2.0991816jes	journal	January 2018

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