High rate and stable cycling of lithium metal anode

Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu; Bhattacharya, Priyanka; Engelhard, Mark H.; Borodin, Oleg; Zhang, Jiguang

doi:10.1038/ncomms7362

Title: High rate and stable cycling of lithium metal anode

Abstract

Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm^-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stabilitymore » of other electrochemical systems.« less

Authors:

Qian, Jiangfeng ^[1]; Henderson, Wesley A. ^[1]; Xu, Wu ^[1]; Bhattacharya, Priyanka ^[2]; Engelhard, Mark H. ^[3]; Borodin, Oleg ^[4]; Zhang, Jiguang ^[1]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Joint Center for Energy Storage Research; Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy & Environment Directorate
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
U.S. Army Research Lab., Adelphi, MD (United States). Sensor & Electron Devices Directorate

Publication Date:: 2015-02-20

Research Org.:: Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1184948

Report Number(s):: PNNL-SA-107989
Journal ID: ISSN 2041-1723; 48379; 48316; KC0208010

Grant/Contract Number:: AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 6; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE

Citation Formats


                    Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. High rate and stable cycling of lithium metal anode.  United States: N. p., 2015. 
Web.  doi:10.1038/ncomms7362.

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                    Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, & Zhang, Jiguang. High rate and stable cycling of lithium metal anode.  United States.  https://doi.org/10.1038/ncomms7362

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                    Qian, Jiangfeng, Henderson, Wesley A., Xu, Wu, Bhattacharya, Priyanka, Engelhard, Mark H., Borodin, Oleg, and Zhang, Jiguang. Fri .  
"High rate and stable cycling of lithium metal anode".  United States.  https://doi.org/10.1038/ncomms7362.  https://www.osti.gov/servlets/purl/1184948.

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@article{osti_1184948,

  title        = {High rate and stable cycling of lithium metal anode},

  author       = {Qian, Jiangfeng and Henderson, Wesley A. and Xu, Wu and Bhattacharya, Priyanka and Engelhard, Mark H. and Borodin, Oleg and Zhang, Jiguang},

  abstractNote = {Lithium (Li) metal is an ideal anode material for rechargeable batteries. However, dendritic Li growth and limited Coulombic efficiency (CE) during repeated Li deposition/stripping processes have prevented the application of this anode in rechargeable Li metal batteries, especially for use at high current densities. Here, we report that the use of highly concentrated electrolytes composed of ether solvents and the lithium bis(fluorosulfonyl)imide (LiFSI) salt enables the high rate cycling of a Li metal anode at high CE (up to 99.1 %) without dendrite growth. With 4 M LiFSI in 1,2-dimethoxyethane (DME) as the electrolyte, a Li|Li cell can be cycled at high rates (10 mA cm-2) for more than 6000 cycles with no increase in the cell impedance, and a Cu|Li cell can be cycled at 4 mA cm-2 for more than 1000 cycles with an average CE of 98.4%. These excellent high rate performances can be attributed to the increased solvent coordination and increased availability of Li+ concentration in the electrolyte. Lastly, further development of this electrolyte may lead to practical applications for Li metal anode in rechargeable batteries. The fundamental mechanisms behind the high rate ion exchange and stability of the electrolytes also shine light on the stability of other electrochemical systems.},

  doi          = {10.1038/ncomms7362},

  journal      = {Nature Communications},

  number       = ,

  volume       = 6,

  place        = {United States},

  year         = {2015},

  month        = {2}

}

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Title: High rate and stable cycling of lithium metal anode

Abstract

Citation Formats

History, Evolution, and Future Status of Energy Storage journal, May 2012

Lithium metal anodes for rechargeable batteries journal, January 2014

Identification of Surface Films Formed on Lithium in Propylene Carbonate Solutions journal, January 1987

A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions journal, June 2002

Carbon materials for lithium-ion rechargeable batteries journal, February 1999

Li–O2 and Li–S batteries with high energy storage journal, January 2012

Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes journal, September 2014

Interconnected hollow carbon nanospheres for stable lithium metal anodes journal, July 2014

Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism journal, March 2013

A Highly Reversible Lithium Metal Anode journal, January 2014

Stable lithium electrodeposition in liquid and nanoporous solid electrolytes journal, August 2014

Effects of Carbonate Solvents and Lithium Salts on Morphology and Coulombic Efficiency of Lithium Electrode journal, January 2013

The Study of Electrolyte Solutions Based on Ethylene and Diethyl Carbonates for Rechargeable Li Batteries journal, January 1995

Lithium Ethylene Dicarbonate Identified as the Primary Product of Chemical and Electrochemical Reduction of EC in 1.2 M LiPF 6 /EC:EMC Electrolyte journal, September 2005

The study of electrolyte solutions based on solvents from the “glyme” family (linear polyethers) for secondary Li battery systems journal, January 1997

Suppression of dendritic lithium formation by using concentrated electrolyte solutions journal, April 2008

Sulfamides and Glymes as Aprotic Solvents for Lithium Batteries journal, January 1998

1H, 7Li, and 19F nuclear magnetic resonance and ionic conductivity studies for liquid electrolytes composed of glymes and polyetheneglycol dimethyl ethers of CH3O(CH2CH2O)nCH3 (n=3–50) doped with LiN(SO2CF3)2 journal, September 2002

Glyme−Lithium Salt Phase Behavior journal, July 2006

Glyme−Lithium Bis(trifluoromethanesulfonyl)imide and Glyme−Lithium Bis(perfluoroethanesulfonyl)imide Phase Behavior and Solvate Structures journal, April 2005

Complexes of Lithium Imide Salts with Tetraglyme and Their Polyelectrolyte Composite Materials journal, January 2004

Oxidative-Stability Enhancement and Charge Transport Mechanism in Glyme–Lithium Salt Equimolar Complexes journal, August 2011

A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries journal, February 2013

Suppression of aluminum corrosion by using high concentration LiTFSI electrolyte journal, June 2013

A superconcentrated ether electrolyte for fast-charging Li-ion batteries journal, January 2013

Unusual Stability of Acetonitrile-Based Superconcentrated Electrolytes for Fast-Charging Lithium-Ion Batteries journal, March 2014

Concentrated electrolytes: decrypting electrolyte properties and reassessing Al corrosion mechanisms journal, January 2014

A New Sealed Lithium-Peroxide Battery with a Co-Doped Li2O Cathode in a Superconcentrated Lithium Bis(fluorosulfonyl)amide Electrolyte journal, July 2014

Lithium bis(fluorosulfonyl)imide (LiFSI) as conducting salt for nonaqueous liquid electrolytes for lithium-ion batteries: Physicochemical and electrochemical properties journal, April 2011

Novel dual-salts electrolyte solution for dendrite-free lithium-metal based rechargeable batteries with high cycle reversibility journal, December 2014

Morphological Transitions on Lithium Metal Anodes journal, January 2009

Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes journal, November 2013

Transport and Electrochemical Properties and Spectral Features of Non-Aqueous Electrolytes Containing LiFSI in Linear Carbonate Solvents journal, January 2011

Ionic Liquids with the Bis(fluorosulfonyl)imide Anion: Electrochemical Properties and Applications in Battery Technology journal, January 2010

Molecular Dynamics Simulation Studies of the Structure of a Mixed Carbonate/LiPF 6 Electrolyte near Graphite Surface as a Function of Electrode Potential journal, December 2011

Electrolyte Solvation and Ionic Association III. Acetonitrile-Lithium Salt Mixtures–Transport Properties journal, January 2013

Sacrificial Anion Reduction Mechanism for Electrochemical Stability Improvement in Highly Concentrated Li-Salt Electrolyte journal, June 2014

Polarizable Force Field Development and Molecular Dynamics Simulations of Ionic Liquids journal, August 2009

Molecular Dynamics Simulation and Pulsed-Field Gradient NMR Studies of Bis(fluorosulfonyl)imide (FSI) and Bis[(trifluoromethyl)sulfonyl]imide (TFSI)-Based Ionic Liquids journal, May 2010

Electrolyte Solvation and Ionic Association: V. Acetonitrile-Lithium Bis(fluorosulfonyl)imide (LiFSI) Mixtures journal, January 2014

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Anode-Free Rechargeable Lithium Metal Batteries journal, August 2016

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Design Strategies to Enable the Efficient Use of Sodium Metal Anodes in High‐Energy Batteries journal, October 2019

A Review of Solid Electrolyte Interphases on Lithium Metal Anode journal, November 2015

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Dendrite-Free and Performance-Enhanced Lithium Metal Batteries through Optimizing Solvent Compositions and Adding Combinational Additives journal, February 2018

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High‐Performance Silicon Anodes Enabled By Nonflammable Localized High‐Concentration Electrolytes journal, July 2019

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The Origin of the Reduced Reductive Stability of Ion–Solvent Complexes on Alkali and Alkaline Earth Metal Anodes journal, December 2018

Active‐Oxygen‐Enhanced Homogeneous Nucleation of Lithium Metal on Ultrathin Layered Double Hydroxide journal, February 2019

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A Flexible Solid Electrolyte Interphase Layer for Long-Life Lithium Metal Anodes journal, January 2018

History, Evolution, and Future Status of Energy Storage
journal, May 2012

Lithium metal anodes for rechargeable batteries
journal, January 2014

Identification of Surface Films Formed on Lithium in Propylene Carbonate Solutions
journal, January 1987

A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions
journal, June 2002

Carbon materials for lithium-ion rechargeable batteries
journal, February 1999

Li–O₂ and Li–S batteries with high energy storage
journal, January 2012

Failure Mechanism for Fast-Charged Lithium Metal Batteries with Liquid Electrolytes
journal, September 2014

Interconnected hollow carbon nanospheres for stable lithium metal anodes
journal, July 2014

Dendrite-Free Lithium Deposition via Self-Healing Electrostatic Shield Mechanism
journal, March 2013

A Highly Reversible Lithium Metal Anode
journal, January 2014

Stable lithium electrodeposition in liquid and nanoporous solid electrolytes
journal, August 2014

Effects of Carbonate Solvents and Lithium Salts on Morphology and Coulombic Efficiency of Lithium Electrode
journal, January 2013

The Study of Electrolyte Solutions Based on Ethylene and Diethyl Carbonates for Rechargeable Li Batteries
journal, January 1995

Lithium Ethylene Dicarbonate Identified as the Primary Product of Chemical and Electrochemical Reduction of EC in 1.2 M LiPF ₆ /EC:EMC Electrolyte
journal, September 2005

The study of electrolyte solutions based on solvents from the “glyme” family (linear polyethers) for secondary Li battery systems
journal, January 1997

Suppression of dendritic lithium formation by using concentrated electrolyte solutions
journal, April 2008

Sulfamides and Glymes as Aprotic Solvents for Lithium Batteries
journal, January 1998

1H, 7Li, and 19F nuclear magnetic resonance and ionic conductivity studies for liquid electrolytes composed of glymes and polyetheneglycol dimethyl ethers of CH3O(CH2CH2O)nCH3 (n=3–50) doped with LiN(SO2CF3)2
journal, September 2002

Glyme−Lithium Salt Phase Behavior
journal, July 2006

Glyme−Lithium Bis(trifluoromethanesulfonyl)imide and Glyme−Lithium Bis(perfluoroethanesulfonyl)imide Phase Behavior and Solvate Structures
journal, April 2005

Complexes of Lithium Imide Salts with Tetraglyme and Their Polyelectrolyte Composite Materials
journal, January 2004

Oxidative-Stability Enhancement and Charge Transport Mechanism in Glyme–Lithium Salt Equimolar Complexes
journal, August 2011

A new class of Solvent-in-Salt electrolyte for high-energy rechargeable metallic lithium batteries
journal, February 2013

Suppression of aluminum corrosion by using high concentration LiTFSI electrolyte
journal, June 2013

A superconcentrated ether electrolyte for fast-charging Li-ion batteries
journal, January 2013

Unusual Stability of Acetonitrile-Based Superconcentrated Electrolytes for Fast-Charging Lithium-Ion Batteries
journal, March 2014

Concentrated electrolytes: decrypting electrolyte properties and reassessing Al corrosion mechanisms
journal, January 2014

A New Sealed Lithium-Peroxide Battery with a Co-Doped Li2O Cathode in a Superconcentrated Lithium Bis(fluorosulfonyl)amide Electrolyte
journal, July 2014

Lithium bis(fluorosulfonyl)imide (LiFSI) as conducting salt for nonaqueous liquid electrolytes for lithium-ion batteries: Physicochemical and electrochemical properties
journal, April 2011

Novel dual-salts electrolyte solution for dendrite-free lithium-metal based rechargeable batteries with high cycle reversibility
journal, December 2014

Morphological Transitions on Lithium Metal Anodes
journal, January 2009

Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes
journal, November 2013

Transport and Electrochemical Properties and Spectral Features of Non-Aqueous Electrolytes Containing LiFSI in Linear Carbonate Solvents
journal, January 2011

Ionic Liquids with the Bis(fluorosulfonyl)imide Anion: Electrochemical Properties and Applications in Battery Technology
journal, January 2010

Molecular Dynamics Simulation Studies of the Structure of a Mixed Carbonate/LiPF ₆ Electrolyte near Graphite Surface as a Function of Electrode Potential
journal, December 2011

Electrolyte Solvation and Ionic Association III. Acetonitrile-Lithium Salt Mixtures–Transport Properties
journal, January 2013

Sacrificial Anion Reduction Mechanism for Electrochemical Stability Improvement in Highly Concentrated Li-Salt Electrolyte
journal, June 2014

Polarizable Force Field Development and Molecular Dynamics Simulations of Ionic Liquids
journal, August 2009

Molecular Dynamics Simulation and Pulsed-Field Gradient NMR Studies of Bis(fluorosulfonyl)imide (FSI) and Bis[(trifluoromethyl)sulfonyl]imide (TFSI)-Based Ionic Liquids
journal, May 2010

Electrolyte Solvation and Ionic Association: V. Acetonitrile-Lithium Bis(fluorosulfonyl)imide (LiFSI) Mixtures
journal, January 2014

In Situ Formation of Protective Coatings on Sulfur Cathodes in Lithium Batteries with LiFSI-Based Organic Electrolytes
journal, December 2014

Anode-Free Rechargeable Lithium Metal Batteries
journal, August 2016

Prestoring Lithium into Stable 3D Nickel Foam Host as Dendrite-Free Lithium Metal Anode
journal, May 2017

Materials and Device Constructions for Aqueous Lithium-Sulfur Batteries
journal, March 2018

Creating Effective Nanoreactors on Carbon Nanotubes with Mechanochemical Treatments for High-Areal-Capacity Sulfur Cathodes and Lithium Anodes
journal, June 2018

Iron Fluoride-Carbon Nanocomposite Nanofibers as Free-Standing Cathodes for High-Energy Lithium Batteries
journal, June 2018

Pseudocapacitance Induced Uniform Plating/Stripping of Li Metal Anode in Vertical Graphene Nanowalls
journal, October 2018

Ceramic–Salt Composite Electrolytes from Cold Sintering
journal, April 2019

Sulfurized Polyacrylonitrile Cathodes with High Compatibility in Both Ether and Carbonate Electrolytes for Ultrastable Lithium–Sulfur Batteries
journal, July 2019

Conductive Nanostructured Scaffolds Render Low Local Current Density to Inhibit Lithium Dendrite Growth
journal, January 2016

Dendrite-Free Lithium Deposition Induced by Uniformly Distributed Lithium Ions for Efficient Lithium Metal Batteries
journal, February 2016

Extending the Life of Lithium-Based Rechargeable Batteries by Reaction of Lithium Dendrites with a Novel Silica Nanoparticle Sandwiched Separator
journal, November 2016

Dendrite-Free, High-Rate, Long-Life Lithium Metal Batteries with a 3D Cross-Linked Network Polymer Electrolyte
journal, February 2017

A Dual-Stimuli-Responsive Sodium-Bromine Battery with Ultrahigh Energy Density
journal, April 2018

Boron Embedded in Metal Iron Matrix as a Novel Anode Material of Excellent Performance
journal, July 2018

Anode Interface Engineering and Architecture Design for High‐Performance Lithium–Sulfur Batteries
journal, January 2019

Advances and Prospects of Sulfide All‐Solid‐State Lithium Batteries via One‐to‐One Comparison with Conventional Liquid Lithium Ion Batteries
journal, May 2019

Uniform Distribution of Alloying/Dealloying Stress for High Structural Stability of an Al Anode in High‐Areal‐Density Lithium‐Ion Batteries
journal, February 2019

Highly Elastic Polyrotaxane Binders for Mechanically Stable Lithium Hosts in Lithium‐Metal Batteries
journal, May 2019

Design Strategies to Enable the Efficient Use of Sodium Metal Anodes in High‐Energy Batteries
journal, October 2019

A Review of Solid Electrolyte Interphases on Lithium Metal Anode
journal, November 2015

Metallic Octahedral CoSe ₂ Threaded by N-Doped Carbon Nanotubes: A Flexible Framework for High-Performance Potassium-Ion Batteries
journal, August 2018

A Sulfur Cathode with Pomegranate-Like Cluster Structure
journal, May 2015

SiO ₂ Hollow Nanosphere-Based Composite Solid Electrolyte for Lithium Metal Batteries to Suppress Lithium Dendrite Growth and Enhance Cycle Life
journal, January 2016

Review on High-Loading and High-Energy Lithium-Sulfur Batteries
journal, May 2017

Macroporous Catalytic Carbon Nanotemplates for Sodium Metal Anodes
journal, November 2017

Dendrite-Free and Performance-Enhanced Lithium Metal Batteries through Optimizing Solvent Compositions and Adding Combinational Additives
journal, February 2018

Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte
journal, July 2018

High‐Performance Silicon Anodes Enabled By Nonflammable Localized High‐Concentration Electrolytes
journal, July 2019

Stable Li Metal Anode Enabled by Space Confinement and Uniform Curvature through Lithiophilic Nanotube Arrays
journal, November 2019

The Origin of the Reduced Reductive Stability of Ion–Solvent Complexes on Alkali and Alkaline Earth Metal Anodes
journal, December 2018

Active‐Oxygen‐Enhanced Homogeneous Nucleation of Lithium Metal on Ultrathin Layered Double Hydroxide
journal, February 2019

Fluor und Lithium: Ideale Partner für Elektrolyte in wiederaufladbaren Hochleistungsbatterien
journal, July 2019

Self‐Healable Solid Polymeric Electrolytes for Stable and Flexible Lithium Metal Batteries
journal, October 2019

A Sustainable Solid Electrolyte Interphase for High‐Energy‐Density Lithium Metal Batteries Under Practical Conditions
journal, January 2020

Columnar Lithium Metal Anodes
journal, September 2017

A Flexible Solid Electrolyte Interphase Layer for Long-Life Lithium Metal Anodes
journal, January 2018

A Versatile Halide Ester Enabling Li‐Anode Stability and a High Rate Capability in Lithium–Oxygen Batteries
journal, February 2019

A Hybrid Anion for Ionic Liquid and Battery Electrolyte Applications: Half Triflamide, Half Carbonate
journal, February 2019

Flexible Amalgam Film Enables Stable Lithium Metal Anodes with High Capacities
journal, November 2019