Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Burning lithium in CS2 for high-performing compact Li2S–graphene nanocapsules for Li–S–batteries

Journal Article · · Nature Energy

Here, tremendous efforts have been made to design the cathode of Li–S batteries to improve their energy density and cycling life. However, challenges remain in achieving fast electronic and ionic transport while accommodating the significant cathode volumetric change, especially for the cathode with a high practical mass loading. Here we report a cathode architecture, which is constructed by burning lithium foils in a CS2 vapour. The obtained structure features crystalline Li2S nanoparticles wrapped by few-layer graphene (Li2S@graphene nanocapsules). Because of the improvement on the volumetric efficiency for accommodating sulfur active species and electrical properties, the cathode design enables promising electrochemical performance. More notably, at a loading of 10 mgLi2S cm–2, the electrode exhibits a high reversible capacity of 1,160 mAh g–1s, namely, an area capacity of 8.1 mAh cm–2. Li2S@graphene cathode demonstrates a great potential for Li-ion batteries, where the Li2S@graphene-cathode//graphite-anode cell displays a high capacity of 730 mAh g–1s as well as stable cycle performance.

Research Organization:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Science Foundation (NSF)
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1366717
Journal Information:
Nature Energy, Journal Name: Nature Energy Vol. 2; ISSN 2058-7546
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

References (43)

A Facile Layer-by-Layer Approach for High-Areal-Capacity Sulfur Cathodes journal January 2015
Li 2 S-Carbon Sandwiched Electrodes with Superior Performance for Lithium-Sulfur Batteries journal August 2013
Harnessing Steric Separation of Freshly Nucleated Li 2 S Nanoparticles for Bottom-Up Assembly of High-Performance Cathodes for Lithium-Sulfur and Lithium-Ion Batteries journal April 2014
Progress in Mechanistic Understanding and Characterization Techniques of Li-S Batteries journal May 2015
Lithium-Sulfur Batteries: Electrochemistry, Materials, and Prospects journal November 2013
Solution-Based Processing of Graphene-Li 2 S Composite Cathodes for Lithium-Ion and Lithium-Sulfur Batteries journal February 2014
Micro-scale Li2S–C composite preparation from Li2SO4 for cathode of lithium ion battery journal November 2015
Reducing CO2 to dense nanoporous graphene by Mg/Zn for high power electrochemical capacitors journal January 2015
Understanding the Anchoring Effect of Two-Dimensional Layered Materials for Lithium–Sulfur Batteries journal May 2015
Lithium Sulfide (Li 2 S)/Graphene Oxide Nanospheres with Conformal Carbon Coating as a High-Rate, Long-Life Cathode for Li/S Cells journal April 2015
Challenges and Prospects of Lithium–Sulfur Batteries journal June 2012
Rechargeable Lithium–Sulfur Batteries journal July 2014
High-Capacity Micrometer-Sized Li2 S Particles as Cathode Materials for Advanced Rechargeable Lithium-Ion Batteries journal September 2012
In Situ -Formed Li 2 S in Lithiated Graphite Electrodes for Lithium–Sulfur Batteries journal November 2013
Durable Carbon-Coated Li 2 S Core–Shell Spheres for High Performance Lithium/Sulfur Cells journal March 2014
Orthorhombic Bipyramidal Sulfur Coated with Polypyrrole Nanolayers As a Cathode Material for Lithium–Sulfur Batteries journal April 2012
Toward a Molecular Understanding of Energetics in Li–S Batteries Using Nonaqueous Electrolytes: A High-Level Quantum Chemical Study journal May 2014
New Nanostructured Li2S/Silicon Rechargeable Battery with High Specific Energy journal April 2010
Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium–Sulfur Battery Cathode Material with High Capacity and Cycling Stability journal July 2011
Hollow Carbon Nanofiber-Encapsulated Sulfur Cathodes for High Specific Capacity Rechargeable Lithium Batteries journal October 2011
Nanostructured Li 2 S–C Composites as Cathode Material for High-Energy Lithium/Sulfur Batteries journal February 2012
Amphiphilic Surface Modification of Hollow Carbon Nanofibers for Improved Cycle Life of Lithium Sulfur Batteries journal February 2013
Graphene-Based Three-Dimensional Hierarchical Sandwich-type Architecture for High-Performance Li/S Batteries journal September 2013
Sulfur Cathodes with Hydrogen Reduced Titanium Dioxide Inverse Opal Structure journal April 2014
Freestanding three-dimensional core–shell nanoarrays for lithium-ion battery anodes journal June 2016
Stabilizing lithium–sulphur cathodes using polysulphide reservoirs journal May 2011
Sulphur–TiO2 yolk–shell nanoarchitecture with internal void space for long-cycle lithium–sulphur batteries journal January 2013
Two-dimensional layered transition metal disulphides for effective encapsulation of high-capacity lithium sulphide cathodes journal September 2014
A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries journal May 2009
Li–O2 and Li–S batteries with high energy storage journal January 2012
Ultrasmall Li2S Nanoparticles Anchored in Graphene Nanosheets for High-Energy Lithium-Ion Batteries journal September 2014
In situ synthesis of lithium sulfide–carbon composites as cathode materials for rechargeable lithium batteries journal January 2013
A high performance lithium-ion sulfur battery based on a Li 2 S cathode using a dual-phase electrolyte journal January 2015
Conversion of carbon dioxide to few-layer graphene journal January 2011
Nanostructured sulfur cathodes journal January 2013
In situ synthesis of lithium sulfide–carbon composites as cathode materials for rechargeable lithium batteries journal January 2013
Facile synthesis of Li2S–polypyrrole composite structures for high-performance Li2S cathodes journal January 2014
High-capacity Li2S–graphene oxide composite cathodes with stable cycling performance journal January 2014
High-performance hollow sulfur nanostructured battery cathode through a scalable, room temperature, one-step, bottom-up approach journal April 2013
Visualizing the electrochemical reaction of ZnO nanoparticles with lithium by in situ TEM: two reaction modes are revealed journal May 2013
Raman Spectrum of Graphene and Graphene Layers journal October 2006
Interstitial and Interlayer Ion Diffusion Geometry Extraction in Graphitic Nanosphere Battery Materials journal January 2016
Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium-Sulfur-Battery Cathode Material with High Capacity and Cycling Stability text January 2011

Cited By (71)

Electrochemically primed functional redox mediator generator from the decomposition of solid state electrolyte journal April 2019
Self-Supported 3D Array Electrodes for Sodium Microbatteries journal November 2017
Encapsulating Various Sulfur Allotropes within Graphene Nanocages for Long-Lasting Lithium Storage journal March 2018
Controllable Urchin-Like NiCo 2 S 4 Microsphere Synergized with Sulfur-Doped Graphene as Bifunctional Catalyst for Superior Rechargeable Zn-Air Battery journal January 2018
Toward High Performance Lithium-Sulfur Batteries Based on Li 2 S Cathodes and Beyond: Status, Challenges, and Perspectives journal March 2018
Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity journal November 2018
Manipulating Polysulfide Conversion with Strongly Coupled Fe 3 O 4 and Nitrogen Doped Carbon for Stable and High Capacity Lithium-Sulfur Batteries journal November 2018
Chem-Bonding and Phys-Trapping Se Electrode for Long-Life Rechargeable Batteries journal January 2019
Surface‐Driven Energy Storage Behavior of Dual‐Heteroatoms Functionalized Carbon Material journal February 2019
Engineering Fe–Fe 3 C@Fe–N–C Active Sites and Hybrid Structures from Dual Metal–Organic Frameworks for Oxygen Reduction Reaction in H 2 –O 2 Fuel Cell and Li–O 2 Battery journal April 2019
A Molecular‐Cage Strategy Enabling Efficient Chemisorption–Electrocatalytic Interface in Nanostructured Li 2 S Cathode for Li Metal‐Free Rechargeable Cells with High Energy journal September 2019
Morphology Reshaping Enabling Self‐Densification of Manganese Oxide Hybrid Materials for High‐Density Lithium Storage Anodes journal October 2019
Boosting Sodium Storage in TiO 2 Nanotube Arrays through Surface Phosphorylation journal January 2018
Revisiting the Role of Polysulfides in Lithium-Sulfur Batteries journal March 2018
A Sulfur-Limonene-Based Electrode for Lithium-Sulfur Batteries: High-Performance by Self-Protection journal February 2018
Li 2 S- or S-Based Lithium-Ion Batteries journal July 2018
A Lithium-Sulfur Battery using a 2D Current Collector Architecture with a Large-Sized Sulfur Host Operated under High Areal Loading and Low E/S Ratio journal October 2018
Fundamental Understanding of Water‐Induced Mechanisms in Li–O 2 Batteries: Recent Developments and Perspectives journal November 2018
Two‐Dimensional Arrays of Transition Metal Nitride Nanocrystals journal June 2019
Flexible VO x Nanosphere@SWCNT Hybrid Films with Dual-Confinement Function of Polysulfides for High-Performance Lithium-Sulfur Batteries journal July 2018
An Ultrahigh Capacity Graphite/Li 2 S Battery with Holey-Li 2 S Nanoarchitectures journal May 2018
Updated Metal Compounds (MOFs, S, OH, N, C) Used as Cathode Materials for Lithium-Sulfur Batteries journal January 2018
Rational Design of a Dual-Function Hybrid Cathode Substrate for Lithium-Sulfur Batteries journal June 2018
Nickel–Cobalt Double Hydroxide as a Multifunctional Mediator for Ultrahigh‐Rate and Ultralong‐Life Li–S Batteries journal October 2018
Controllable Chain-Length for Covalent Sulfur-Carbon Materials Enabling Stable and High-Capacity Sodium Storage journal January 2019
Deciphering the Reaction Mechanism of Lithium–Sulfur Batteries by In Situ/Operando Synchrotron‐Based Characterization Techniques journal March 2019
Commercialization of Lithium Battery Technologies for Electric Vehicles journal June 2019
Metal Sulfide‐Decorated Carbon Sponge as a Highly Efficient Electrocatalyst and Absorbant for Polysulfide in High‐Loading Li 2 S Batteries journal April 2019
Insights into Structural Evolution of Lithium Peroxides with Reduced Charge Overpotential in Li−O 2 System journal June 2019
Silica Restricting the Sulfur Volatilization of Nickel Sulfide for High‐Performance Lithium‐Ion Batteries journal October 2019
A Li 2 S‐TiS 2 ‐Electrolyte Composite for Stable Li 2 S‐Based Lithium–Sulfur Batteries journal June 2019
The Radical Pathway Based on a Lithium‐Metal‐Compatible High‐Dielectric Electrolyte for Lithium–Sulfur Batteries journal December 2018
Long‐Life Room‐Temperature Sodium–Sulfur Batteries by Virtue of Transition‐Metal‐Nanocluster–Sulfur Interactions journal January 2019
Prospect of Sulfurized Pyrolyzed Poly(acrylonitrile) (S@pPAN) Cathode Materials for Rechargeable Lithium Batteries journal February 2020
The Radical Pathway Based on a Lithium‐Metal‐Compatible High‐Dielectric Electrolyte for Lithium–Sulfur Batteries journal December 2018
Long-Life Room-Temperature Sodium-Sulfur Batteries by Virtue of Transition-Metal-Nanocluster-Sulfur Interactions journal January 2019
Prospect of Sulfurized Pyrolyzed Poly(acrylonitrile) (S@pPAN) Cathode Materials for Rechargeable Lithium Batteries journal February 2020
Gyroidal Porous Carbon Activated with NH 3 or CO 2 as Lithium−Sulfur Battery Cathodes journal April 2018
ZnS coating of cathode facilitates lean‐electrolyte Li‐S batteries journal October 2019
Demanding energy from carbon journal September 2019
Hierarchical Porous N‐Doped Carbon Nanosheets Obtained by Organic–Inorganic Bipolymeric Engineering for Improved Lithium–Sulfur Batteries journal February 2019
Cyclic Voltammetry in Lithium–Sulfur Batteries—Challenges and Opportunities journal April 2019
In Situ Electrochemically Derived Amorphous-Li 2 S for High Performance Li 2 S/Graphite Full Cell journal April 2018
Advanced Li 2 S/Si Full Battery Enabled by TiN Polysulfide Immobilizer journal October 2019
Applications of Conventional Vibrational Spectroscopic Methods for Batteries Beyond Li-Ion journal March 2018
Synchrotron-Based X-ray Absorption Fine Structures, X-ray Diffraction, and X-ray Microscopy Techniques Applied in the Study of Lithium Secondary Batteries journal April 2018
Sulfur Hosts against the Shuttle Effect journal April 2018
A Brief Review of Metallothermic Reduction Reactions for Materials Preparation journal August 2018
In Situ Techniques for Developing Robust Li-S Batteries journal August 2018
Understanding the Reaction Mechanism of Lithium–Sulfur Batteries by In Situ/Operando X-ray Absorption Spectroscopy journal March 2019
The bond evolution mechanism of covalent sulfurized carbon during electrochemical sodium storage process journal April 2019
High-Performance Anode Materials for Rechargeable Lithium-Ion Batteries journal March 2018
Graphene for Energy Storage and Conversion: Synthesis and Interdisciplinary Applications journal April 2019
Exceptional catalytic effects of black phosphorus quantum dots in shuttling-free lithium sulfur batteries journal October 2018
Intercalation-conversion hybrid cathodes enabling Li–S full-cell architectures with jointly superior gravimetric and volumetric energy densities journal March 2019
Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries journal May 2019
Scalable chemical-vapour-deposition growth of three-dimensional graphene materials towards energy-related applications journal January 2018
Layered LiTiO 2 for the protection of Li 2 S cathodes against dissolution: mechanisms of the remarkable performance boost journal January 2018
The improvement of pitch activation by graphene for long-cycle Li–S batteries journal January 2018
Harnessing the unique properties of 2D materials for advanced lithium–sulfur batteries journal January 2019
Adsorption and diffusion of lithium polysulfides over blue phosphorene for Li–S batteries journal January 2018
A carbon foam-supported high sulfur loading composite as a self-supported cathode for flexible lithium–sulfur batteries journal January 2018
A green and facile strategy for the low-temperature and rapid synthesis of Li 2 S@PC–CNT cathodes with high Li 2 S content for advanced Li–S batteries journal January 2018
Recent research trends in Li–S batteries journal January 2018
A rechargeable metal-free full-liquid sulfur–bromine battery for sustainable energy storage journal January 2018
Vanadium dioxide–reduced graphene oxide binary host as an efficient polysulfide plague for high-performance lithium–sulfur batteries journal January 2019
A new high-capacity and safe energy storage system: lithium-ion sulfur batteries journal January 2019
A facile synthetic approach to nanostructured Li 2 S cathodes for rechargeable solid-state Li–S batteries journal January 2019
Enhanced Na + pseudocapacitance in a P, S co-doped carbon anode arising from the surface modification by sulfur and phosphorus with C–S–P coupling journal January 2020
A flexible, hierarchically porous PANI/MnO 2 network with fast channels and an extraordinary chemical process for stable fast-charging lithium–sulfur batteries journal January 2020
Review—Li Metal Anode in Working Lithium-Sulfur Batteries journal June 2017

Similar Records

Dense Graphene Monolith for High Volumetric Energy Density Li-S Batteries
Journal Article · Mon Mar 12 00:00:00 EDT 2018 · Advanced Energy Materials · OSTI ID:1466311

An Ultrahigh Capacity Graphite/Li2S Battery with Holey-Li2S Nanoarchitectures
Journal Article · Mon May 07 00:00:00 EDT 2018 · Advanced Science · OSTI ID:1438222