Improving Lithium-Sulfur Battery Performance under Lean Electrolyte through Nanoscale Confinement in Soft Swellable Gels.

Li-S batteries have been extensively studied using rigid carbon as the host for sulfur encapsulation, but improving the properties with a reduced electrolyte amount remains a significant challenge. This is critical for achieving high energy density. Here, we developed a soft PEO10LiTFSI polymer swellable gel as a nanoscale reservoir to trap the polysulfides under lean electrolyte conditions. The PEO10LiTFSI gel immobilizes the electrolyte and confines polysulfides within the ion conducting phase. The Li-S cell with a much lower electrolyte to sulfur ratio (E/S) of 4 gE/gS (3.3 mLE/gS) could deliver a capacity of 1200 mA h/g, 4.6 mA h/cm2, and good cycle life. The accumulation of polysulfide reduction products, such as Li2S, on the cathode, is identified as the potential mechanism for capacity fading under lean electrolyte conditions.

[1]  Yuyan Shao,et al.  Restricting the Solubility of Polysulfides in Li‐S Batteries Via Electrolyte Salt Selection , 2016 .

[2]  A. Manthiram,et al.  High-Energy-Density Lithium–Sulfur Batteries Based on Blade-Cast Pure Sulfur Electrodes , 2016 .

[3]  Long-Chain Polysulfide Retention at the Cathode of Li–S Batteries , 2016 .

[4]  Feng Li,et al.  3D Graphene‐Foam–Reduced‐Graphene‐Oxide Hybrid Nested Hierarchical Networks for High‐Performance Li–S Batteries , 2016, Advanced materials.

[5]  Xiulin Fan,et al.  Activation of Oxygen‐Stabilized Sulfur for Li and Na Batteries , 2016 .

[6]  Kenville E. Hendrickson,et al.  Enhanced Li-S Batteries Using Amine-Functionalized Carbon Nanotubes in the Cathode. , 2016, ACS nano.

[7]  Sean E. Doris,et al.  Three-Dimensional Growth of Li2S in Lithium-Sulfur Batteries Promoted by a Redox Mediator. , 2016, Nano letters.

[8]  A. Manthiram,et al.  High‐Energy, High‐Rate, Lithium–Sulfur Batteries: Synergetic Effect of Hollow TiO2‐Webbed Carbon Nanotubes and a Dual Functional Carbon‐Paper Interlayer , 2016 .

[9]  Rajeev S. Assary,et al.  Solvent Effects on Polysulfide Redox Kinetics and Ionic Conductivity in Lithium-Sulfur Batteries , 2016 .

[10]  Zhengyuan Tu,et al.  Nanostructured electrolytes for stable lithium electrodeposition in secondary batteries. , 2015, Accounts of chemical research.

[11]  Petr Novák,et al.  Progress Towards Commercially Viable Li–S Battery Cells , 2015 .

[12]  D. Aurbach,et al.  Review on Li‐Sulfur Battery Systems: an Integral Perspective , 2015 .

[13]  Jens Tübke,et al.  Lithium–Sulfur Cells: The Gap between the State‐of‐the‐Art and the Requirements for High Energy Battery Cells , 2015 .

[14]  Wu Xu,et al.  Anodes for Rechargeable Lithium‐Sulfur Batteries , 2015 .

[15]  Jianming Zheng,et al.  High Energy Density Lithium–Sulfur Batteries: Challenges of Thick Sulfur Cathodes , 2015 .

[16]  Shiguo Zhang,et al.  Recent Advances in Electrolytes for Lithium–Sulfur Batteries , 2015 .

[17]  Ying Yu,et al.  In Situ Polymerized PAN-Assisted S/C Nanosphere with Enhanced High-Power Performance as Cathode for Lithium/Sulfur Batteries. , 2015, Nano letters.

[18]  Chunsheng Wang,et al.  Confined Sulfur in Microporous Carbon Renders Superior Cycling Stability in Li/S Batteries , 2015 .

[19]  Seung M. Oh,et al.  Highly Cyclable Lithium-Sulfur Batteries with a Dual-Type Sulfur Cathode and a Lithiated Si/SiOx Nanosphere Anode. , 2015, Nano letters.

[20]  Dongping Lu,et al.  Following the transient reactions in lithium-sulfur batteries using an in situ nuclear magnetic resonance technique. , 2015, Nano letters.

[21]  Yuyan Shao,et al.  Molecular-confinement of polysulfides within mesoscale electrodes for the practical application of lithium sulfur batteries , 2015 .

[22]  A. Manthiram,et al.  A Facile Layer‐by‐Layer Approach for High‐Areal‐Capacity Sulfur Cathodes , 2015, Advanced materials.

[23]  Shaogang Wang,et al.  Rapid communicationA graphene foam electrode with high sulfur loading for flexible and high energy Li-S batteries , 2015 .

[24]  L. Nazar,et al.  Review—The Importance of Chemical Interactions between Sulfur Host Materials and Lithium Polysulfides for Advanced Lithium-Sulfur Batteries , 2015 .

[25]  Kevin G. Gallagher,et al.  Critical Link between Materials Chemistry and Cell-Level Design for High Energy Density and Low Cost Lithium-Sulfur Transportation Battery , 2015 .

[26]  Jun Lu,et al.  Insight into sulfur reactions in Li-S batteries. , 2014, ACS applied materials & interfaces.

[27]  K. Edström,et al.  Functional, water-soluble binders for improved capacity and stability of lithium–sulfur batteries , 2014 .

[28]  Jens Tübke,et al.  Cell energy density and electrolyte/sulfur ratio in Li–S cells , 2014 .

[29]  Jou-Hyeon Ahn,et al.  Effect of sulfur loading on energy density of lithium sulfur batteries , 2014 .

[30]  R. Dominko,et al.  Application of in operando UV/Vis spectroscopy in lithium-sulfur batteries. , 2014, ChemSusChem.

[31]  Hua Zhao,et al.  Glymes as Versatile Solvents for Chemical Reactions and Processes: From the Laboratory to Industry , 2014 .

[32]  Arumugam Manthiram,et al.  Rechargeable lithium-sulfur batteries. , 2014, Chemical reviews.

[33]  Shuru Chen,et al.  Bis(2,2,2-trifluoroethyl) ether as an electrolyte co-solvent for mitigating self-discharge in lithium-sulfur batteries. , 2014, ACS applied materials & interfaces.

[34]  Petr Novák,et al.  Importance of ‘unimportant’ experimental parameters in Li–S battery development , 2014 .

[35]  D. Aurbach,et al.  The Use of Redox Mediators for Enhancing Utilization of Li2S Cathodes for Advanced Li-S Battery Systems. , 2014, The journal of physical chemistry letters.

[36]  Xie Kai,et al.  Review of Electrolyte for Lithium Sulfur Battery , 2014 .

[37]  Shuru Chen,et al.  Bis ( 2 , 2 , 2-tri fl uoroethyl ) Ether As an Electrolyte Co-solvent for Mitigating Self-Discharge in Lithium − Sulfur Batteries , 2014 .

[38]  Wolfgang G. Bessler,et al.  Insight into lithium–sulfur batteries: Elementary kinetic modeling and impedance simulation , 2013 .

[39]  Li Li,et al.  Polyethylene-glycol-doped polypyrrole increases the rate performance of the cathode in lithium-sulfur batteries. , 2013, ChemSusChem.

[40]  Robert Dominko,et al.  Li-S battery analyzed by UV/Vis in operando mode. , 2013, ChemSusChem.

[41]  Shengbo Zhang,et al.  Liquid electrolyte lithium/sulfur battery: Fundamental chemistry, problems, and solutions , 2013 .

[42]  Joachim Häcker,et al.  Investigation of Magnesium–Sulfur Batteries using Electrochemical Impedance Spectroscopy , 2013 .

[43]  Shengbo Zhang.  New insight into liquid electrolyte of rechargeable lithium/sulfur battery , 2013 .

[44]  Jianming Zheng,et al.  How to Obtain Reproducible Results for Lithium Sulfur Batteries , 2013 .

[45]  Shengbo Zhang.  A Concept for Making Poly(ethylene oxide) Based Composite Gel Polymer Electrolyte Lithium/Sulfur Battery , 2013 .

[46]  Phillip K. Koech,et al.  Controlled Nucleation and Growth Process of Li2S2/Li2S in Lithium-Sulfur Batteries , 2013 .

[47]  Shengbo Zhang,et al.  Improved Cyclability of Liquid Electrolyte Lithium/Sulfur Batteries by Optimizing Electrolyte/Sulfur Ratio , 2012 .

[48]  Shizhao Xiong,et al.  Insights into Li-S Battery Cathode Capacity Fading Mechanisms: Irreversible Oxidation of Active Mass during Cycling , 2012 .

[49]  Daniel M. Seo,et al.  Electrolyte Solvation and Ionic Association , 2012 .

[50]  M. Watanabe,et al.  Change from Glyme Solutions to Quasi-ionic Liquids for Binary Mixtures Consisting of Lithium Bis(trifluoromethanesulfonyl)amide and Glymes , 2011 .

[51]  S. E. Mochalov,et al.  A study of the electrochemical processes in lithiumsulphur cells by impedance spectroscopy , 2011 .

[52]  Xinping Qiu,et al.  New insight into the discharge process of sulfur cathode by electrochemical impedance spectroscopy , 2009 .

[53]  K. W. Kim,et al.  Electrochemical properties of lithium sulfur cells using PEO polymer electrolytes prepared under three different mixing conditions , 2007 .

[54]  W. Henderson.  Crystallization Kinetics of Glyme-LiX and PEO-LiX Polymer Electrolytes , 2007 .

[55]  Jason R. Wickham,et al.  Lithium environment in dilute poly(ethylene oxide)/lithium triflate polymer electrolyte from REDOR NMR spectroscopy. , 2006, The journal of physical chemistry. B.

[56]  Price,et al.  Structure of liquid PEO-LiTFSI electrolyte , 2000, Physical review letters.

[57]  Peter G. Bruce,et al.  Structure of the polymer electrolyte poly(ethylene oxide)6:LiAsF6 , 1999, Nature.

[58]  Michel Perrier,et al.  Phase Diagrams and Conductivity Behavior of Poly(ethylene oxide)-Molten Salt Rubbery Electrolytes , 1994 .

[59]  P. Bruce,et al.  Crystal Structure of the Polymer Electrolyte Poly(ethylene oxide)3:LiCF3SO3 , 1993, Science.