High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

Periyapperuma, Kalani; Arca, Elisabetta; Harvey, Steven; Pathirana, Thushan; Ban, Chunmei; Burrell, Anthony; Pozo-Gonzalo, Cristina; Howlett, Patrick C.

doi:10.1021/acsami.0c09074

Title: High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

Abstract

High-energy-density systems with fast charging rates and suppressed dendrite growth are critical for the implementation of efficient and safe next-generation advanced battery technologies such as those based on Li metal. However, there are few studies that investigate reliable cycling of Li metal electrodes under high-rate conditions. in this work, by employing a superconcentrated ionic liquid (IL) electrolyte, we highlight the effect of Li salt concentration and applied current density on the resulting Li deposit morphology and solid electrolyte interphase (SEI) characteristics, demonstrating exceptional deposition/dissolution rates and efficiency in these systems. Operation at higher current densities enhanced the cycling efficiency, e.g., from 64 ± 3% at 1 mA cm^–2 up to 96 ± 1% at 20 mA cm^–2 (overpotential <±0.2 V), while resulting in lower electrode resistance and dendrite-free Li morphology. A maximum current density of 50 mA cm^–2 resulted in 88 ± 3% cycling efficiency, displaying tolerance for high overpotentials at the Ni working electrode (0.5 V). X-ray photoelectron microscopy (XPS), time-of-flight secondary-ion mass spectroscopy (ToF-SIMS), and scanning electron microscopy (SEM) surface measurements revealed that the formation of a stable SEI, rich in LiF and deficient in organic carbon species, coupled with nondendritic and compact Li morphologies enabled enhanced cyclingmore »« less

Authors:

^[1]; Arca, Elisabetta ^[2];

^[2]; Pathirana, Thushan ^[1];

^[2]; Burrell, Anthony ^[2]; Pozo-Gonzalo, Cristina ^[1];

^[1]

Deakin Univ., Melbourne, VIC (Australia)
National Renewable Energy Lab. (NREL), Golden, CO (United States)

Publication Date:: Wed Sep 02 00:00:00 EDT 2020

Research Org.:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Org.:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office; Australian Research Council (ARC)

OSTI Identifier:: 1665837

Report Number(s):: NREL/JA-5K00-77342
Journal ID: ISSN 1944-8244; MainId:26288;UUID:6235ead2-13a4-467a-805f-05520f9f6078;MainAdminID:17447

Grant/Contract Number:: AC36-08GO28308

Resource Type:: Accepted Manuscript

Journal Name:: ACS Applied Materials and Interfaces

Additional Journal Information:: Journal Volume: 12; Journal Issue: 37; Journal ID: ISSN 1944-8244

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; batteries; high current; high efficiency; ionic liquid; LiF; SEI; silicon; superconcentrated

Citation Formats


                    Periyapperuma, Kalani, Arca, Elisabetta, Harvey, Steven, Pathirana, Thushan, Ban, Chunmei, Burrell, Anthony, Pozo-Gonzalo, Cristina, and Howlett, Patrick C. High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase.  United States: N. p., 2020. 
Web.  doi:10.1021/acsami.0c09074.

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                    Periyapperuma, Kalani, Arca, Elisabetta, Harvey, Steven, Pathirana, Thushan, Ban, Chunmei, Burrell, Anthony, Pozo-Gonzalo, Cristina, & Howlett, Patrick C. High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase.  United States.  https://doi.org/10.1021/acsami.0c09074

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                    Periyapperuma, Kalani, Arca, Elisabetta, Harvey, Steven, Pathirana, Thushan, Ban, Chunmei, Burrell, Anthony, Pozo-Gonzalo, Cristina, and Howlett, Patrick C. Wed .  
"High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase".  United States.  https://doi.org/10.1021/acsami.0c09074.  https://www.osti.gov/servlets/purl/1665837.

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@article{osti_1665837,

  title        = {High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase},

  author       = {Periyapperuma, Kalani and Arca, Elisabetta and Harvey, Steven and Pathirana, Thushan and Ban, Chunmei and Burrell, Anthony and Pozo-Gonzalo, Cristina and Howlett, Patrick C.},

  abstractNote = {High-energy-density systems with fast charging rates and suppressed dendrite growth are critical for the implementation of efficient and safe next-generation advanced battery technologies such as those based on Li metal. However, there are few studies that investigate reliable cycling of Li metal electrodes under high-rate conditions. in this work, by employing a superconcentrated ionic liquid (IL) electrolyte, we highlight the effect of Li salt concentration and applied current density on the resulting Li deposit morphology and solid electrolyte interphase (SEI) characteristics, demonstrating exceptional deposition/dissolution rates and efficiency in these systems. Operation at higher current densities enhanced the cycling efficiency, e.g., from 64 ± 3% at 1 mA cm–2 up to 96 ± 1% at 20 mA cm–2 (overpotential <±0.2 V), while resulting in lower electrode resistance and dendrite-free Li morphology. A maximum current density of 50 mA cm–2 resulted in 88 ± 3% cycling efficiency, displaying tolerance for high overpotentials at the Ni working electrode (0.5 V). X-ray photoelectron microscopy (XPS), time-of-flight secondary-ion mass spectroscopy (ToF-SIMS), and scanning electron microscopy (SEM) surface measurements revealed that the formation of a stable SEI, rich in LiF and deficient in organic carbon species, coupled with nondendritic and compact Li morphologies enabled enhanced cycling efficiency at higher currents. Reduced dendrite formation at high current is further highlighted by the use of a highly porous separator in coin cell cycling (1 mAh cm–2 at 50 °C), sustaining 500 cycles at 10 mA cm–2.},

  doi          = {10.1021/acsami.0c09074},

  journal      = {ACS Applied Materials and Interfaces},

  number       = 37,

  volume       = 12,

  place        = {United States},

  year         = {Wed Sep 02 00:00:00 EDT 2020},

  month        = {Wed Sep 02 00:00:00 EDT 2020}

}

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Title: High Current Cycling in a Superconcentrated Ionic Liquid Electrolyte to Promote Uniform Li Morphology and a Uniform LiF-Rich Solid Electrolyte Interphase

Abstract

Citation Formats

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Structure of ionic liquids under external electric field: a molecular dynamics simulation journal, March 2012

Engineering high-energy-density sodium battery anodes for improved cycling with superconcentrated ionic-liquid electrolytes journal, May 2020

A new asymmetric Pseudo-Voigt function for more efficient fitting of XPS lines: New asymmetric Pseudo-Voigt function for efficient XPS line fitting journal, June 2014

High Lithium Metal Cycling Efficiency in a Room-Temperature Ionic Liquid journal, January 2004

(Invited) Long-Term Cyclability of Lithium Metal Electrodes in Ionic Liquid-Based Electrolytes at Room Temperature conference, January 2010

The Correlation Between Surface Chemistry, Surface Morphology, and Cycling Efficiency of Lithium Electrodes in a Few Polar Aprotic Systems journal, January 1989

Status of the secondary lithium electrode journal, January 1981

Some problems of the cycleability of lithium electrodes journal, May 1989

Effect of Current Density on Morphology of Lithium Electrodeposited in Ionic Liquid-Based Electrolytes journal, January 2014

Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal journal, January 2017

Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes journal, January 2017

Electrochemical reduction mechanisms and stabilities of some cation types used in ionic liquids and other organic salts journal, November 2012

Study of the Initial Stage of Solid Electrolyte Interphase Formation upon Chemical Reaction of Lithium Metal and N -Methyl- N -Propyl-Pyrrolidinium-Bis(Fluorosulfonyl)Imide journal, September 2012

A comparative AFM study of the interfacial nanostructure in imidazolium or pyrrolidinium ionic liquid electrolytes for zinc electrochemical systems journal, January 2016

Dendrite-Free Lithium Deposition with Self-Aligned Columnar Structure in a Carbonate–Ether Mixed Electrolyte journal, May 2017

Stabilizing lithium metal using ionic liquids for long-lived batteries journal, June 2016

Spectroscopic Characterization of the SEI Layer Formed on Lithium Metal Electrodes in Phosphonium Bis(fluorosulfonyl)imide Ionic Liquid Electrolytes journal, February 2018

Characterization of the Lithium Surface in N-Methyl-N-alkylpyrrolidinium Bis(trifluoromethanesulfonyl)amide Room-Temperature Ionic Liquid Electrolytes journal, January 2006

Characterization of Lithium Electrode in Lithium Imides/Ethylene Carbonate and Cyclic Ether Electrolytes journal, January 2004

Influence of the lithium salt nature over the surface film formation on a graphite electrode in Li-ion batteries: An XPS study journal, March 2007

Improving high-capacity Li1.2Ni0.15Mn0.55Co0.1O2-based lithium-ion cells by modifiying the positive electrode with alumina journal, July 2013

Conformal Lithium Fluoride Protection Layer on Three-Dimensional Lithium by Nonhazardous Gaseous Reagent Freon journal, May 2017

Fluoroethylene Carbonate Additives to Render Uniform Li Deposits in Lithium Metal Batteries journal, January 2017

Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters journal, February 2015

Structure and Nanostructure in Ionic Liquids journal, June 2015

Structure and dynamics of the interfacial layer between ionic liquids and electrode materials journal, April 2014

Composite nonwoven separator for lithium-ion battery: Development and characterization journal, July 2010

Polyethylene separator activated by hybrid coating improving Li+ ion transference number and ionic conductivity for Li-metal battery journal, February 2017

Development of microporous PE films to improve lithium ion batteries journal, April 2010

Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review
journal, July 2017

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

Lithium batteries: a 50-year perspective, 1959–2009
journal, October 2000

α-CuV ₂ O ₆ Nanowires: Hydrothermal Synthesis and Primary Lithium Battery Application
journal, April 2008

A review of hazards associated with primary lithium and lithium-ion batteries
journal, November 2011

Composite lithium metal anode by melt infusion of lithium into a 3D conducting scaffold with lithiophilic coating
journal, February 2016

3D Porous Cu Current Collector/Li-Metal Composite Anode for Stable Lithium-Metal Batteries
journal, March 2017

Accommodating lithium into 3D current collectors with a submicron skeleton towards long-life lithium metal anodes
journal, August 2015

Ionic Liquid Electrolytes for Li–Air Batteries: Lithium Metal Cycling
journal, May 2014

Accurate Determination of Coulombic Efficiency for Lithium Metal Anodes and Lithium Metal Batteries
journal, October 2017

A reversible dendrite-free high-areal-capacity lithium metal electrode
journal, April 2017

An Artificial Solid Electrolyte Interphase with High Li-Ion Conductivity, Mechanical Strength, and Flexibility for Stable Lithium Metal Anodes
journal, December 2016

Columnar Lithium Metal Anodes
journal, September 2017

Synergistic Effect of 3D Current Collectors and ALD Surface Modification for High Coulombic Efficiency Lithium Metal Anodes
journal, December 2018

Utmost limits of various solid electrolytes in all-solid-state lithium batteries: A critical review
journal, July 2019

Reviving the lithium metal anode for high-energy batteries
journal, March 2017

Review—Superconcentrated Electrolytes for Lithium Batteries
journal, January 2015

Energy applications of ionic liquids
journal, January 2014

Application of the N-propyl-N-methyl-pyrrolidinium Bis(fluorosulfonyl)imide RTIL Containing Lithium Bis(fluorosulfonyl)imide in Ionic Liquid Based Lithium Batteries
journal, January 2010

Prospects of applying ionic liquids and deep eutectic solvents for renewable energy storage by means of redox flow batteries
journal, February 2014

Physical properties of high Li-ion content N-propyl-N-methylpyrrolidinium bis(fluorosulfonyl)imide based ionic liquid electrolytes
journal, January 2015

Why Bis(fluorosulfonyl)imide Is a “Magic Anion” for Electrochemistry
journal, August 2014

Fast Charge/Discharge of Li Metal Batteries Using an Ionic Liquid Electrolyte
journal, January 2013

Toward Practical Li Metal Batteries: Importance of Separator Compatibility Using Ionic Liquid Electrolytes
journal, August 2019

Role of Li Concentration and the SEI Layer in Enabling High Performance Li Metal Electrodes Using a Phosphonium Bis(fluorosulfonyl)imide Ionic Liquid
journal, September 2017

Structure of ionic liquids under external electric field: a molecular dynamics simulation
journal, March 2012

Engineering high-energy-density sodium battery anodes for improved cycling with superconcentrated ionic-liquid electrolytes
journal, May 2020

A new asymmetric Pseudo-Voigt function for more efficient fitting of XPS lines: New asymmetric Pseudo-Voigt function for efficient XPS line fitting
journal, June 2014

High Lithium Metal Cycling Efficiency in a Room-Temperature Ionic Liquid
journal, January 2004

(Invited) Long-Term Cyclability of Lithium Metal Electrodes in Ionic Liquid-Based Electrolytes at Room Temperature
conference, January 2010

The Correlation Between Surface Chemistry, Surface Morphology, and Cycling Efficiency of Lithium Electrodes in a Few Polar Aprotic Systems
journal, January 1989

Status of the secondary lithium electrode
journal, January 1981

Some problems of the cycleability of lithium electrodes
journal, May 1989

Effect of Current Density on Morphology of Lithium Electrodeposited in Ionic Liquid-Based Electrolytes
journal, January 2014

Nanoscale Nucleation and Growth of Electrodeposited Lithium Metal
journal, January 2017

Dead lithium: mass transport effects on voltage, capacity, and failure of lithium metal anodes
journal, January 2017

Electrochemical reduction mechanisms and stabilities of some cation types used in ionic liquids and other organic salts
journal, November 2012

Study of the Initial Stage of Solid Electrolyte Interphase Formation upon Chemical Reaction of Lithium Metal and N -Methyl- N -Propyl-Pyrrolidinium-Bis(Fluorosulfonyl)Imide
journal, September 2012

A comparative AFM study of the interfacial nanostructure in imidazolium or pyrrolidinium ionic liquid electrolytes for zinc electrochemical systems
journal, January 2016

Dendrite-Free Lithium Deposition with Self-Aligned Columnar Structure in a Carbonate–Ether Mixed Electrolyte
journal, May 2017

Stabilizing lithium metal using ionic liquids for long-lived batteries
journal, June 2016

Spectroscopic Characterization of the SEI Layer Formed on Lithium Metal Electrodes in Phosphonium Bis(fluorosulfonyl)imide Ionic Liquid Electrolytes
journal, February 2018

Characterization of the Lithium Surface in N-Methyl-N-alkylpyrrolidinium Bis(trifluoromethanesulfonyl)amide Room-Temperature Ionic Liquid Electrolytes
journal, January 2006

Characterization of Lithium Electrode in Lithium Imides/Ethylene Carbonate and Cyclic Ether Electrolytes
journal, January 2004

Influence of the lithium salt nature over the surface film formation on a graphite electrode in Li-ion batteries: An XPS study
journal, March 2007

Improving high-capacity Li1.2Ni0.15Mn0.55Co0.1O2-based lithium-ion cells by modifiying the positive electrode with alumina
journal, July 2013

Conformal Lithium Fluoride Protection Layer on Three-Dimensional Lithium by Nonhazardous Gaseous Reagent Freon
journal, May 2017

Fluoroethylene Carbonate Additives to Render Uniform Li Deposits in Lithium Metal Batteries
journal, January 2017

Nanoscale Imaging of Fundamental Li Battery Chemistry: Solid-Electrolyte Interphase Formation and Preferential Growth of Lithium Metal Nanoclusters
journal, February 2015

Structure and Nanostructure in Ionic Liquids
journal, June 2015

Structure and dynamics of the interfacial layer between ionic liquids and electrode materials
journal, April 2014

Composite nonwoven separator for lithium-ion battery: Development and characterization
journal, July 2010

Polyethylene separator activated by hybrid coating improving Li+ ion transference number and ionic conductivity for Li-metal battery
journal, February 2017

Development of microporous PE films to improve lithium ion batteries
journal, April 2010