Rational Design of Statically and Dynamically Stable Lithium–Sulfur Batteries with High Sulfur Loading and Low Electrolyte/Sulfur Ratio

The primary challenge with lithium-sulfur battery research is the design of sulfur cathodes that exhibit high electrochemical efficiency and stability while keeping the sulfur content and loading high and the electrolyte/sulfur ratio low. With a systematic investigation, a novel graphene/cotton-carbon cathode is presented here that enables sulfur loading and content as high as 46 mg cm-2 and 70 wt% with an electrolyte/sulfur ratio of as low as only 5. The graphene/cotton-carbon cathodes deliver peak capacities of 926 and 765 mA h g-1 , respectively, at C/10 and C/5 rates, which translate into high areal, gravimetric, and volumetric capacities of, respectively, 43 and 35 mA h cm-2 , 648 and 536 mA h g-1 , and 1067 and 881 mA h cm-3 with a stable cyclability. They also exhibit superior cell-storage capability with 95% capacity-retention, a low self-discharge constant of just 0.0012 per day, and stable poststorage cyclability after storing over a long period of six months. This work demonstrates a viable approach to develop lithium-sulfur batteries with practical energy densities exceeding that of lithium-ion batteries.

[1]  Arumugam Manthiram,et al.  Lithium–Sulfur Batteries: Progress and Prospects , 2015, Advanced materials.

[2]  Jens Tübke,et al.  Development and costs calculation of lithium–sulfur cells with high sulfur load and binder free electrodes , 2013 .

[3]  Jiaqi Huang,et al.  Multi-functional separator/interlayer system for high-stable lithium-sulfur batteries: Progress and prospects , 2015 .

[4]  Mark Wild,et al.  Lithium sulfur batteries, a mechanistic review , 2015 .

[5]  Jie Xiao,et al.  Understanding the Lithium Sulfur Battery System at Relevant Scales , 2015 .

[6]  A. Manthiram,et al.  A Carbon-Cotton Cathode with Ultrahigh-Loading Capability for Statically and Dynamically Stable Lithium-Sulfur Batteries. , 2016, ACS nano.

[7]  L. Nazar,et al.  A Comprehensive Approach toward Stable Lithium–Sulfur Batteries with High Volumetric Energy Density , 2017 .

[8]  Junho Ahn,et al.  Self-discharge characteristics of lithium/sulfur batteries using TEGDME liquid electrolyte , 2006 .

[9]  Hong‐Jie Peng,et al.  Nanoarchitectured Graphene/CNT@Porous Carbon with Extraordinary Electrical Conductivity and Interconnected Micro/Mesopores for Lithium‐Sulfur Batteries , 2014 .

[10]  Jun Liu,et al.  Improving Lithium-Sulfur Battery Performance under Lean Electrolyte through Nanoscale Confinement in Soft Swellable Gels. , 2017, Nano letters.

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

[12]  Jean-Marie Tarascon,et al.  Li–S batteries: simple approaches for superior performance , 2013 .

[13]  A. Manthiram,et al.  Bifunctional Separator with a Light‐Weight Carbon‐Coating for Dynamically and Statically Stable Lithium‐Sulfur Batteries , 2014 .

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

[15]  X. Lou,et al.  A sulfur host based on titanium monoxide@carbon hollow spheres for advanced lithium–sulfur batteries , 2016, Nature Communications.

[16]  A. Manthiram,et al.  A core–shell electrode for dynamically and statically stable Li–S battery chemistry , 2016 .

[17]  Feng Li,et al.  Carbon–sulfur composites for Li–S batteries: status and prospects , 2013 .

[18]  Micro‐ and Mesoporous Carbide‐Derived Carbon–Selenium Cathodes for High‐Performance Lithium Selenium Batteries , 2015 .

[19]  Xiyuan Chen,et al.  Self-adaptive strain-relaxation optimization for high-energy lithium storage material through crumpling of graphene , 2014, Nature Communications.

[20]  A. Manthiram,et al.  Lithium–Sulfur Batteries with the Lowest Self-Discharge and the Longest Shelf life , 2017 .

[21]  K. Sing.  Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity (Recommendations 1984) , 1985 .

[22]  A. Manthiram,et al.  A Shell‐Shaped Carbon Architecture with High‐Loading Capability for Lithium Sulfide Cathodes , 2017 .

[23]  Doron Aurbach,et al.  Challenges in the development of advanced Li-ion batteries: a review , 2011 .

[24]  J. Muldoon,et al.  A layer-by-layer supramolecular structure for a sulfur cathode , 2016 .

[25]  A. Manthiram,et al.  Carbonized Eggshell Membrane as a Natural Polysulfide Reservoir for Highly Reversible Li‐S Batteries , 2014, Advanced materials.

[26]  K. M. Abraham,et al.  A Lithium/Dissolved Sulfur Battery with an Organic Electrolyte , 1979 .

[27]  Elton J. Cairns,et al.  Self-discharge of lithium–sulfur cells using stainless-steel current-collectors , 2005 .

[28]  Patrik Johansson,et al.  A review of electrolytes for lithium–sulphur batteries , 2014 .

[29]  Chaohe Xu,et al.  Graphene-based electrodes for electrochemical energy storage , 2013 .

[30]  A. Manthiram,et al.  Porous Carbon Mat as an Electrochemical Testing Platform for Investigating the Polysulfide Retention of Various Cathode Configurations in Li-S Cells. , 2015, The journal of physical chemistry letters.

[31]  Anthony F. Hollenkamp,et al.  Lithium–sulfur batteries—the solution is in the electrolyte, but is the electrolyte a solution? , 2014 .

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

[33]  Michael A. Pope,et al.  Structural Design of Cathodes for Li‐S Batteries , 2015 .

[34]  Arumugam Manthiram,et al.  Highly reversible lithium/dissolved polysulfide batteries with carbon nanotube electrodes. , 2013, Angewandte Chemie.

[35]  Li-Jun Wan,et al.  Lithium-sulfur batteries: electrochemistry, materials, and prospects. , 2013, Angewandte Chemie.

[36]  Bruno Scrosati,et al.  Recent progress and remaining challenges in sulfur-based lithium secondary batteries--a review. , 2013, Chemical communications.

[37]  Feixiang Wu,et al.  Li-ion battery materials: present and future , 2015 .

[38]  Yuriy V. Mikhaylik,et al.  Polysulfide Shuttle Study in the Li/S Battery System , 2004 .

[39]  Xin-Bing Cheng,et al.  Nanostructured energy materials for electrochemical energy conversion and storage: A review , 2016 .

[40]  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 .

[41]  B. McCloskey,et al.  Attainable gravimetric and volumetric energy density of Li-S and li ion battery cells with solid separator-protected Li metal anodes. , 2015, The journal of physical chemistry letters.

[42]  L. Nazar,et al.  Interwoven MXene Nanosheet/Carbon‐Nanotube Composites as Li–S Cathode Hosts , 2017, Advanced materials.

[43]  Shuru Chen,et al.  High capacity of lithium-sulfur batteries at low electrolyte/sulfur ratio enabled by an organosulfide containing electrolyte , 2017 .

[44]  Zaiping Guo,et al.  A Strategy for Configuration of an Integrated Flexible Sulfur Cathode for High-Performance Lithium-Sulfur Batteries. , 2016, Angewandte Chemie.