skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Organosulfide-plasticized solid-electrolyte interphase layer enables stable lithium metal anodes for long-cycle lithium-sulfur batteries

Journal Article · · Nature Communications

Lithium metal is a promising anode candidate for the next-generation rechargeable battery due to its highest specific capacity (3860 mA h g-1) and lowest potential, but low Coulombic efficiency and formation of lithium dendrites hinder its practical application. Here, we report a self-formed flexible hybrid solid-electrolyte interphase layer through co-deposition of organosulfides/organopolysulfides and inorganic lithium salts using sulfur-containing polymers as an additive in the electrolyte. The organosulfides/organopolysulfides serve as “plasticizer” in the solid-electrolyte interphase layer to improve its mechanical flexibility and toughness. The as-formed robust solid-electrolyte interphase layers enable dendrite-free lithium deposition and significantly improve Coulombic efficiency (99% over 400 cycles at a current density of 2mAcm-2). A lithium-sulfur battery based on this strategy exhibits long cycling life (1000 cycles) and good capacity retention. This study reveals an avenue to effectively fabricate stable solid-electrolyte interphase layer for solving the issues associated with lithium metal anodes.

Research Organization:
Pennsylvania State Univ., University Park, PA (United States). Department of Mechanical and Nuclear Engineering; Pennsylvania State Univ., University Park, PA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
EE0007795
OSTI ID:
1430243
Alternate ID(s):
OSTI ID: 1435961
Report Number(s):
DOE-PENN STATE-0007795; DOE-PENNSTATE-0007795; PII: 974
Journal Information:
Nature Communications, Vol. 8, Issue 1; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 204 works
Citation information provided by
Web of Science

References (63)

Nanostructured Electrolytes for Stable Lithium Electrodeposition in Secondary Batteries journal October 2015
Functional Organosulfide Electrolyte Promotes an Alternate Reaction Pathway to Achieve High Performance in Lithium–Sulfur Batteries journal February 2016
Effect of vinylene carbonate as additive to electrolyte for lithium metal anode journal February 2004
X-ray Photoelectron Spectroscopy Study of Surface Films Formed on Li Electrodes Freshly Prepared in Alkyl Carbonate Solutions journal April 1999
Protection of lithium metal surfaces using tetraethoxysilane journal January 2011
Future prospects of the lithium metal anode journal September 1997
An Artificial Solid Electrolyte Interphase Layer for Stable Lithium Metal Anodes journal December 2015
Calibration of rectangular atomic force microscope cantilevers journal October 1999
Dendrite-Free Electrodeposition and Reoxidation of Lithium-Sodium Alloy for Metal-Anode Battery journal January 2011
Lithium Fluoride Additives for Stable Cycling of Lithium Batteries at High Current Densities journal January 2016
Lithium metal stripping/plating mechanisms studies: A metallurgical approach journal October 2006
Unusual Stability of Acetonitrile-Based Superconcentrated Electrolytes for Fast-Charging Lithium-Ion Batteries journal March 2014
On the role of cyclic unsaturated additives on the behaviour of lithium metal electrodes in ionic liquid electrolytes journal February 2010
Recent Advances in Battery Science and Technology journal June 2015
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries journal October 2004
In situ scanning vibrating electrode technique for lithium metal anodes journal October 1997
A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries journal February 2013
Sustainable Redox Mediation for Lithium-Oxygen Batteries by a Composite Protective Layer on the Lithium-Metal Anode journal December 2015
Polysulfide-Scission Reagents for the Suppression of the Shuttle Effect in Lithium–Sulfur Batteries journal February 2017
A Lightweight TiO 2 /Graphene Interlayer, Applied as a Highly Effective Polysulfide Absorbent for Fast, Long-Life Lithium-Sulfur Batteries journal March 2015
Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism journal March 2013
Metallic anodes for next generation secondary batteries journal January 2013
Healing High-Loading Sulfur Electrodes with Unprecedented Long Cycling Life: Spatial Heterogeneity Control journal March 2017
Measurement of Thin Film Mechanical Properties Using Nanoindentation journal July 1992
Film forming reaction at the lithium/electrolyte interface journal January 1983
Effects of Some Organic Additives on Lithium Deposition in Propylene Carbonate journal January 2002
Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes journal November 2013
Surface Condition Changes in Lithium Metal Deposited in Nonaqueous Electrolyte Containing HF by Dissolution-Deposition Cycles journal January 1999
The synergetic effect of lithium polysulfide and lithium nitrate to prevent lithium dendrite growth journal June 2015
Lithium-methylamine reduction. I. Reduction of furan, 2-methylfuran, and furfuryl alcohol journal February 1970
Kilogram scale inverse vulcanization of elemental sulfur to prepare high capacity polymer electrodes for Li-S batteries journal July 2014
An Artificial Solid Electrolyte Interphase with High Li-Ion Conductivity, Mechanical Strength, and Flexibility for Stable Lithium Metal Anodes journal December 2016
Effects of Triacetoxyvinylsilane as SEI Layer Additive on Electrochemical Performance of Lithium Metal Secondary Battery journal January 2007
Electrical Energy Storage and Intercalation Chemistry journal June 1976
Stabilizing lithium metal using ionic liquids for long-lived batteries journal June 2016
Lithium-Sulfur Batteries: Electrochemistry, Materials, and Prospects journal November 2013
Recent studies of the lithium-liquid electrolyte interface Electrochemical, morphological and spectral studies of a few important systems journal March 1995
Design principles for electrolytes and interfaces for stable lithium-metal batteries journal September 2016
Impedance Study on the Electrochemical Lithium Intercalation into Natural Graphite Powder journal January 1998
Force measurements with the atomic force microscope: Technique, interpretation and applications journal October 2005
A Comparative Study of Synthetic Graphite and Li Electrodes in Electrolyte Solutions Based on Ethylene Carbonate-Dimethyl Carbonate Mixtures journal January 1996
Long Cycle-Life Secondary Lithium Cells Utilizing Tetrahydrofuran journal January 1984
Functional Organosulfide Electrolyte Promotes an Alternate Reaction Pathway to Achieve High Performance in Lithium-Sulfur Batteries journal February 2016
Inverse Vulcanization of Elemental Sulfur to Prepare Polymeric Electrode Materials for Li–S Batteries journal February 2014
Nonaqueous Liquid Electrolytes for Lithium-Based Rechargeable Batteries journal December 2004
Stable lithium electrodeposition in liquid and nanoporous solid electrolytes journal August 2014
The use of elemental sulfur as an alternative feedstock for polymeric materials journal April 2013
Dendrite-Free Lithium Deposition with Self-Aligned Nanorod Structure journal November 2014
Role of LiNO3 in rechargeable lithium/sulfur battery journal May 2012
Three-dimensional porous carbon composites containing high sulfur nanoparticle content for high-performance lithium–sulfur batteries journal February 2016
Stable Lithium Electrodeposition in Liquid and Nanoporous Solid Electrolytes text January 2014
Regulating Li deposition at artificial solid electrolyte interphases journal January 2017
The study of electrolyte solutions based on solvents from the “glyme” family (linear polyethers) for secondary Li battery systems journal January 1997
Direct Observation of Inhomogeneous Solid Electrolyte Interphase on MnO Anode with Atomic Force Microscopy and Spectroscopy journal January 2012
In Situ Scanning Vibrating Electrode Technique for the Characterization of Interface Between Lithium Electrode and Electrolytes Containing Additives journal January 1994
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions journal June 2002
Lithium metal anodes for rechargeable batteries journal January 2014
Next-Generation Lithium Metal Anode Engineering via Atomic Layer Deposition journal May 2015
Lithium metal protection through in-situ formed solid electrolyte interphase in lithium-sulfur batteries: The role of polysulfides on lithium anode journal September 2016
On the Surface Chemical Aspects of Very High Energy Density, Rechargeable Li–Sulfur Batteries journal January 2009
Reviving rechargeable lithium metal batteries: enabling next-generation high-energy and high-power cells journal January 2012
Ionic liquids as electrolytes for Li-ion batteries—An overview of electrochemical studies journal December 2009
High rate and stable cycling of lithium metal anode journal February 2015

Cited By (51)

Anode Interface Engineering and Architecture Design for High‐Performance Lithium–Sulfur Batteries journal January 2019
Electrochemical Polishing of Lithium Metal Surface for Highly Demanding Solid-Electrolyte Interphase journal September 2018
A Game Changer: Functional Nano/Micromaterials for Smart Rechargeable Batteries journal August 2019
Novel 2D Sb 2 S 3 Nanosheet/CNT Coupling Layer for Exceptional Polysulfide Recycling Performance journal June 2018
Lithium–Magnesium Alloy as a Stable Anode for Lithium–Sulfur Battery journal February 2019
A dual-phase Li–Ca alloy with a patternable and lithiophilic 3D framework for improving lithium anode performance journal January 2019
Chelation-assisted formation of multi-yolk–shell Co 4 N@carbon nanoboxes for self-discharge-suppressed high-performance Li–SeS 2 batteries journal January 2019
Inside Back Cover: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. Int. Ed. 8/2020) journal February 2020
Polymer–inorganic solid–electrolyte interphase for stable lithium metal batteries under lean electrolyte conditions journal March 2019
An ultrathin ionomer interphase for high efficiency lithium anode in carbonate based electrolyte journal December 2019
Green and tunable fabrication of graphene-like N-doped carbon on a 3D metal substrate as a binder-free anode for high-performance potassium-ion batteries journal January 2019
Uniform High Ionic Conducting Lithium Sulfide Protection Layer for Stable Lithium Metal Anode journal April 2019
Long Cycle Life Organic Polysulfide Catholyte for Rechargeable Lithium Batteries journal December 2019
In situ formation of a multicomponent inorganic-rich SEI layer provides a fast charging and high specific energy Li-metal battery journal January 2019
Porous hybrid aerogels with ultrahigh sulfur loading for lithium–sulfur batteries journal January 2018
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions journal January 2020
Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode journal September 2018
Bi-containing Electrolyte Enables Robust and Li Ion Conductive Solid Electrolyte Interphase for Advanced Lithium Metal Anodes journal January 2020
Advances in Artificial Layers for Stable Lithium Metal Anodes journal April 2020
Infrared spectra, structure and bonding in the LiO 2 , LiO 2 Li, LiO and Li 2 O molecules in solid neon journal April 2009
Development and Challenges of Functional Electrolytes for High-Performance Lithium-Sulfur Batteries journal July 2018
The Radical Pathway Based on a Lithium‐Metal‐Compatible High‐Dielectric Electrolyte for Lithium–Sulfur Batteries journal December 2018
Facile synthesis of Ti 4 O 7 on hollow carbon spheres with enhanced polysulfide binding for high-performance lithium–sulfur batteries journal January 2019
Self‐Formed Protection Layer on a 3D Lithium Metal Anode for Ultrastable Lithium–Sulfur Batteries journal April 2019
Mixture is better: enhanced electrochemical performance of phenyl selenosulfide in rechargeable lithium batteries journal January 2018
Liquid Polydimethylsiloxane Grafting to Enable Dendrite‐Free Li Plating for Highly Reversible Li‐Metal Batteries journal May 2019
Methods to Improve Lithium Metal Anode for Li-S Batteries journal December 2019
In situ formed polymer gel electrolytes for lithium batteries with inherent thermal shutdown safety features journal January 2019
Trimethylsilyl azide (C 3 H 9 N 3 Si): a highly efficient additive for tailoring fluoroethylene carbonate (FEC) based electrolytes for Li-metal batteries journal January 2019
The Radical Pathway Based on a Lithium‐Metal‐Compatible High‐Dielectric Electrolyte for Lithium–Sulfur Batteries journal December 2018
Revisiting the Role of Polysulfides in Lithium-Sulfur Batteries journal March 2018
A compact inorganic layer for robust anode protection in lithium‐sulfur batteries journal November 2019
Effective strategies for long-cycle life lithium–sulfur batteries journal January 2018
Dendrite-Free Metallic Lithium in Lithiophilic Carbonized Metal-Organic Frameworks journal March 2018
A 3D flexible and robust HAPs/PVA separator prepared by a freezing-drying method for safe lithium metal batteries journal January 2019
A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions journal February 2020
Superlithiophilic graphene-silver enabling ultra-stable hosts for lithium metal anodes journal January 2020
Designable ultra-smooth ultra-thin solid-electrolyte interphases of three alkali metal anodes journal April 2018
Design Multifunctional Catalytic Interface: Toward Regulation of Polysulfide and Li 2 S Redox Conversion in Li–S Batteries journal November 2019
Toward Better Lithium–Sulfur Batteries: Functional Non-aqueous Liquid Electrolytes journal August 2018
Expanding pore sizes of ZIF-8-derived nitrogen-doped microporous carbon via C 60 embedding: toward improved anode performance for the lithium-ion battery journal January 2018
Lithium anode stable in air for low-cost fabrication of a dendrite-free lithium battery journal February 2019
Innenrücktitelbild: A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions (Angew. Chem. 8/2020) journal January 2020
Electrokinetic Phenomena Enhanced Lithium‐Ion Transport in Leaky Film for Stable Lithium Metal Anodes journal April 2019
Long Cycle Life Lithium Metal Batteries Enabled with Upright Lithium Anode journal February 2019
“Pea-pod-like” nitrogen-doped hollow porous carbon cathode hosts decorated with polar titanium dioxide nanocrystals as efficient polysulfide reservoirs for advanced lithium–sulfur batteries journal January 2018
Toward High Performance Lithium-Sulfur Batteries Based on Li 2 S Cathodes and Beyond: Status, Challenges, and Perspectives journal March 2018
Revisiting the positive roles of liquid polysulfides in alkali metal–sulfur electrochemistry: from electrolyte additives to active catholyte journal January 2019
Spatial separation of lithiophilic surface and superior conductivity for advanced Li metal anode: the case of acetylene black and N-doped carbon spheres journal January 2019
Artificial Solid‐Electrolyte Interphase Enabled High‐Capacity and Stable Cycling Potassium Metal Batteries journal September 2019
A functional-gradient-structured ultrahigh modulus solid polymer electrolyte for all-solid-state lithium metal batteries journal January 2019