Li-Ion-Permeable and Electronically Conductive Membrane Comprising Garnet-Type Li6La3Ta1.5Y0.5O12 and Graphene Toward Ultrastable and High-Rate Lithium Sulfur Batteries

State-of-the-art lithium sulfur (Li–S) batteries suffer from serious systemic issues, which are mainly derived from polysulfide shuttling effect, poor sulfur utilization, and low Coulombic efficiency. These fundamental challenges impede the practical use of sulfur cathode in commercial battery, albeit its higher theoretical storage capacity compared to intercalation electrodes based Li ion batteries, including graphite-LiCoO2, graphite–LiFePO4, and graphite-Li(Ni,Mn,Co)O2 cells. In this Article, we designed a multifunctional membrane, comprising a graphene nanosheet and Li-stuffed garnet solid-state electrolyte (SSE) composite, to synergistically enhance both cycle stability and rate capability of general sulfur cathode in a facile and effective way. With the synergistic contribution of graphene nanosheet and SSE, the sulfur cathode exhibited a superior capacity of 1165 mAh g–1 at 0.5 C and retained an excellent discharge capacity of 947.03 mAh g–1 (81% of initial capacity) over 200 cycles when a Gr/SSE-s...

[1]  Venkataraman Thangadurai,et al.  Fast Lithium Ion Conduction in Garnet‐Type Li7La3Zr2O12 , 2007 .

[2]  Jou-Hyeon Ahn,et al.  Effects of carbon coating on the electrochemical properties of sulfur cathode for lithium/sulfur cell , 2008 .

[3]  L. Nazar,et al.  A highly ordered nanostructured carbon-sulphur cathode for lithium-sulphur batteries. , 2009, Nature materials.

[4]  C. Chen,et al.  Analysis of the chemical diffusion coefficient of lithium ions in Li3V2(PO4)3 cathode material , 2010 .

[5]  L. Nazar,et al.  Advances in Li–S batteries , 2010 .

[6]  Feng Li,et al.  Doped graphene sheets as anode materials with superhigh rate and large capacity for lithium ion batteries. , 2011, ACS nano.

[7]  Arumugam Manthiram,et al.  Improved lithium-sulfur cells with a treated carbon paper interlayer. , 2013, Physical chemistry chemical physics : PCCP.

[8]  A. Manthiram,et al.  Challenges and prospects of lithium-sulfur batteries. , 2013, Accounts of chemical research.

[9]  Khalil Amine,et al.  Ultrasound Assisted Design of Sulfur/Carbon Cathodes with Partially Fluorinated Ether Electrolytes for Highly Efficient Li/S Batteries , 2013, Advanced materials.

[10]  Guangyuan Zheng,et al.  Nanostructured sulfur cathodes. , 2013, Chemical Society reviews.

[11]  Yang Liu,et al.  A highly ordered meso@microporous carbon-supported sulfur@smaller sulfur core-shell structured cathode for Li-S batteries. , 2014, ACS nano.

[12]  Venkataraman Thangadurai,et al.  Garnet-type solid-state fast Li ion conductors for Li batteries: critical review. , 2014, Chemical Society reviews.

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

[14]  Shaogang Wang,et al.  A Graphene–Pure‐Sulfur Sandwich Structure for Ultrafast, Long‐Life Lithium–Sulfur Batteries , 2014, Advanced materials.

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

[16]  Hong‐Jie Peng,et al.  Unstacked double-layer templated graphene for high-rate lithium–sulphur batteries , 2014, Nature Communications.

[17]  U. Paik,et al.  3D-interconnected Nanoporous RGO-CNT Structure for Supercapacitors Application , 2014 .

[18]  E. Wachsman,et al.  Effect of Excess Li on the Structural and Electrical Properties of Garnet-Type Li6La3Ta1.5Y0.5O12 , 2015 .

[19]  Songtao Lu,et al.  Flexible Carbon Nanotube–Graphene/Sulfur Composite Film: Free-Standing Cathode for High-Performance Lithium/Sulfur Batteries , 2015 .

[20]  R. Chellappan,et al.  Fluorinated Reduced Graphene Oxide as an Interlayer in Li–S Batteries , 2015 .

[21]  Liangbing Hu,et al.  Encapsulation of S/SWNT with PANI Web for Enhanced Rate and Cycle Performance in Lithium Sulfur Batteries , 2015, Scientific Reports.

[22]  L. Nazar,et al.  A Nitrogen and Sulfur Dual‐Doped Carbon Derived from Polyrhodanine@Cellulose for Advanced Lithium–Sulfur Batteries , 2015, Advanced materials.

[23]  Sang‐young Lee,et al.  COF-Net on CNT-Net as a Molecularly Designed, Hierarchical Porous Chemical Trap for Polysulfides in Lithium-Sulfur Batteries. , 2016, Nano letters.

[24]  Yeqian Ge,et al.  A novel separator coated by carbon for achieving exceptional high performance lithium-sulfur batteries , 2016 .

[25]  Tingzheng Hou,et al.  Design Principles for Heteroatom-Doped Nanocarbon to Achieve Strong Anchoring of Polysulfides for Lithium-Sulfur Batteries. , 2016, Small.

[26]  Chengwei Wang,et al.  Synergistic Ultrathin Functional Polymer-Coated Carbon Nanotube Interlayer for High Performance Lithium-Sulfur Batteries. , 2016, ACS applied materials & interfaces.

[27]  R. Carter,et al.  Sulfur Vapor-Infiltrated 3D Carbon Nanotube Foam for Binder-Free High Areal Capacity Lithium-Sulfur Battery Composite Cathodes. , 2017, ACS nano.

[28]  Hong‐Jie Peng,et al.  Beaver-dam-like membrane: A robust and sulphifilic MgBO2(OH)/CNT/PP nest separator in Li-S batteries , 2017 .

[29]  Guoxiu Wang,et al.  Fabrication of N‐doped Graphene–Carbon Nanotube Hybrids from Prussian Blue for Lithium–Sulfur Batteries , 2017 .

[30]  Ligui Li,et al.  Conducting Polymers Crosslinked with Sulfur as Cathode Materials for High-Rate, Ultralong-Life Lithium-Sulfur Batteries. , 2017, ChemSusChem.

[31]  Kun Fu,et al.  Synergistic protective effect of a BN-carbon separator for highly stable lithium sulfur batteries , 2017 .

[32]  Bo Zhang,et al.  A Mixed Microporous/Low-range Mesoporous Composite with High Sulfur Loading from Hierarchically-structured Carbon for Lithium Sulfur Batteries , 2017 .

[33]  W. Qin,et al.  Synergistically Assembled Li2S/FWNTs@Reduced Graphene Oxide Nanobundle Forest for Free‐Standing High‐Performance Li2S Cathodes , 2017 .

[34]  Zhian Zhang,et al.  A carbon nanofiber@mesoporous δ-MnO2 nanosheet-coated separator for high-performance lithium-sulfur batteries , 2017 .

[35]  A. Manthiram,et al.  Hydroxylated N-doped carbon nanotube-sulfur composites as cathodes for high-performance lithium-sulfur batteries , 2017 .

[36]  Fengxiang Zhang,et al.  Novel Synergistic Strategy for Developing High-Performance Lithium Sulfur Batteries of Large Areal Sulfur Loading by SEI Modified Separator , 2018 .

[37]  P. Kim,et al.  Toward High-Performance Lithium-Sulfur Batteries: Upcycling of LDPE Plastic into Sulfonated Carbon Scaffold via Microwave-Promoted Sulfonation. , 2018, ACS applied materials & interfaces.

[38]  P. Kim,et al.  Towards highly stable lithium sulfur batteries: Surface functionalization of carbon nanotube scaffolds , 2018 .

[39]  Elise Y. Li,et al.  Adsorption Mechanisms of Lithium Polysulfides on Graphene-Based Interlayers in Lithium Sulfur Batteries , 2018 .