Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries

Chen, Ji; Fan, Xiulin; Li, Qin; Yang, Hongbin; Khoshi, M. Reza; Xu, Yaobin; Hwang, Sooyeon; Chen, Long; Ji, Xiao; Yang, Chongyin; He, Huixin; Wang, Chongmin; Garfunkel, Eric; Su, Dong; Borodin, Oleg; Wang, Chunsheng

doi:10.1038/s41560-020-0601-1

Title: Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries

Abstract

Lithium batteries with Si, Al or Bi microsized (>10 µm) particle anodes promise high capacity, ease of production, low cost and lesser environmental impact, yet they suffer from fast degradation and low Coulombic efficiency (CE). Here we demonstrate that a rationally designed electrolyte (2 M LiPF6 in 1:1 v/v mixture of tetrahydrofuran and 2-methyl tetrahydrofuran) enables 100 cycles of full cells containing microsized Si, Al and Bi anodes with commercial LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes. Alloy anodes with areal capacities of more than 2.5 mAh cm-2 achieved >300 cycles with high initial CE of >90% and average CE of >99.9%.These improvements are facilitated by the formation of a high modulus LiF|organic bilayer interphase possessing high interfacial energy with the alloy anode to accommodate plastic deformation of the lithiated alloy during cycling. This work provides a simple yet practical solution to current battery technology without any binder modification or special fabrication methods.

Authors:

^[1]; Fan, Xiulin ^[1]; Li, Qin ^[1]; Yang, Hongbin ^[2];

^[2];

^[3]; Hwang, Sooyeon ^[4]; Chen, Long ^[1];

^[1];

^[1]; He, Huixin ^[2];

^[3]; Garfunkel, Eric ^[2]; Su, Dong ^[4];

^[5];

^[1]

Univ. of Maryland, College Park, MD (United States)
Rutgers Univ., New Brunswick, NJ (United States); The State Univ. of New Jersey, New Brunswick, NJ (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
US Army Combat Capabilities Development Command Army Research Laboratory, Adelphi, MA (United States)

Publication Date:: Mon Apr 20 00:00:00 EDT 2020

Research Org.:: Brookhaven National Lab. (BNL), Upton, NY (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

OSTI Identifier:: 1619250

Alternate Identifier(s):: OSTI ID: 1633614

Report Number(s):: BNL-215931-2020-JAAM; PNNL-SA-151702
Journal ID: ISSN 2058-7546

Grant/Contract Number:: SC0012704; EE0008202; AC05-76RL01830

Resource Type:: Accepted Manuscript

Journal Name:: Nature Energy

Additional Journal Information:: Journal Volume: 5; Journal Issue: 5; Journal ID: ISSN 2058-7546

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; 36 MATERIALS SCIENCE

Citation Formats


                    Chen, Ji, Fan, Xiulin, Li, Qin, Yang, Hongbin, Khoshi, M. Reza, Xu, Yaobin, Hwang, Sooyeon, Chen, Long, Ji, Xiao, Yang, Chongyin, He, Huixin, Wang, Chongmin, Garfunkel, Eric, Su, Dong, Borodin, Oleg, and Wang, Chunsheng. Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries.  United States: N. p., 2020. 
Web.  doi:10.1038/s41560-020-0601-1.

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                    Chen, Ji, Fan, Xiulin, Li, Qin, Yang, Hongbin, Khoshi, M. Reza, Xu, Yaobin, Hwang, Sooyeon, Chen, Long, Ji, Xiao, Yang, Chongyin, He, Huixin, Wang, Chongmin, Garfunkel, Eric, Su, Dong, Borodin, Oleg, & Wang, Chunsheng. Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries.  United States.  https://doi.org/10.1038/s41560-020-0601-1

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                    Chen, Ji, Fan, Xiulin, Li, Qin, Yang, Hongbin, Khoshi, M. Reza, Xu, Yaobin, Hwang, Sooyeon, Chen, Long, Ji, Xiao, Yang, Chongyin, He, Huixin, Wang, Chongmin, Garfunkel, Eric, Su, Dong, Borodin, Oleg, and Wang, Chunsheng. Mon .  
"Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries".  United States.  https://doi.org/10.1038/s41560-020-0601-1.  https://www.osti.gov/servlets/purl/1619250.

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@article{osti_1619250,

  title        = {Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries},

  author       = {Chen, Ji and Fan, Xiulin and Li, Qin and Yang, Hongbin and Khoshi, M. Reza and Xu, Yaobin and Hwang, Sooyeon and Chen, Long and Ji, Xiao and Yang, Chongyin and He, Huixin and Wang, Chongmin and Garfunkel, Eric and Su, Dong and Borodin, Oleg and Wang, Chunsheng},

  abstractNote = {Lithium batteries with Si, Al or Bi microsized (>10 µm) particle anodes promise high capacity, ease of production, low cost and lesser environmental impact, yet they suffer from fast degradation and low Coulombic efficiency (CE). Here we demonstrate that a rationally designed electrolyte (2 M LiPF6 in 1:1 v/v mixture of tetrahydrofuran and 2-methyl tetrahydrofuran) enables 100 cycles of full cells containing microsized Si, Al and Bi anodes with commercial LiFePO4 and LiNi0.8Co0.15Al0.05O2 cathodes. Alloy anodes with areal capacities of more than 2.5 mAh cm-2 achieved >300 cycles with high initial CE of >90% and average CE of >99.9%.These improvements are facilitated by the formation of a high modulus LiF|organic bilayer interphase possessing high interfacial energy with the alloy anode to accommodate plastic deformation of the lithiated alloy during cycling. This work provides a simple yet practical solution to current battery technology without any binder modification or special fabrication methods.},

  doi          = {10.1038/s41560-020-0601-1},

  journal      = {Nature Energy},

  number       = 5,

  volume       = 5,

  place        = {United States},

  year         = {Mon Apr 20 00:00:00 EDT 2020},

  month        = {Mon Apr 20 00:00:00 EDT 2020}

}

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Title: Electrolyte design for LiF-rich solid–electrolyte interfaces to enable high-performance microsized alloy anodes for batteries

Abstract

Citation Formats

An In Situ X-Ray Diffraction Study of the Reaction of Li with Crystalline Si journal, January 2007

Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells journal, January 2007

Design of Amorphous Alloy Electrodes for Li-Ion Batteries journal, January 2004

Effect of electrode structure on performance of Si anode in Li-ion batteries: Si particle size and conductive additive journal, January 2005

Reversible Cycling of Crystalline Silicon Powder journal, January 2007

A Critical Size of Silicon Nano-Anodes for Lithium Rechargeable Batteries journal, March 2010

Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation journal, August 2011

Crystalline-Amorphous Core−Shell Silicon Nanowires for High Capacity and High Current Battery Electrodes journal, January 2009

High-rate aluminium yolk-shell nanoparticle anode for Li-ion battery with long cycle life and ultrahigh capacity journal, August 2015

Interconnected Silicon Hollow Nanospheres for Lithium-Ion Battery Anodes with Long Cycle Life journal, July 2011

Silicon Nanotube Battery Anodes journal, November 2009

Nonfilling Carbon Coating of Porous Silicon Micrometer-Sized Particles for High-Performance Lithium Battery Anodes journal, February 2015

High-performance lithium-ion anodes using a hierarchical bottom-up approach journal, March 2010

Atomic-level characterization of transport cycle thermodynamics in the glycerol-3-phosphate:phosphate antiporter journal, September 2015

High capacity silicon anodes enabled by MXene viscous aqueous ink journal, February 2019

Self-healing chemistry enables the stable operation of silicon microparticle anodes for high-energy lithium-ion batteries journal, November 2013

Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries journal, July 2017

Silicon Microparticle Anodes with Self-Healing Multiple Network Binder journal, May 2018

A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries journal, September 2011

Growth of conformal graphene cages on micrometre-sized silicon particles as stable battery anodes journal, January 2016

Review—SEI: Past, Present and Future journal, January 2017

Direct Visualization of the Solid Electrolyte Interphase and Its Effects on Silicon Electrochemical Performance journal, August 2016

Solid Electrolyte Interphase Growth and Capacity Loss in Silicon Electrodes journal, June 2016

Understanding Fluoroethylene Carbonate and Vinylene Carbonate Based Electrolytes for Si Anodes in Lithium Ion Batteries with NMR Spectroscopy journal, July 2018

The Mechanism of SEI Formation on a Single Crystal Si(100) Electrode journal, January 2015

"Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries journal, November 2015

Challenges with prediction of battery electrolyte electrochemical stability window and guiding the electrode – electrolyte stabilization journal, February 2019

Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte journal, April 2016

Dielectric Constants for Quantum Chemistry and Li-Ion Batteries: Solvent Blends of Ethylene Carbonate and Ethyl Methyl Carbonate journal, September 2015

Stable cycling of high-voltage lithium metal batteries in ether electrolytes journal, July 2018

High-Concentration Ether Electrolytes for Stable High-Voltage Lithium Metal Batteries journal, March 2019

Surface chemistry and morphology of the solid electrolyte interphase on silicon nanowire lithium-ion battery anodes journal, April 2009

Lithium Salt Effects on Silicon Electrode Performance and Solid Electrolyte Interphase (SEI) Structure, Role of Solution Structure on SEI Formation journal, January 2017

Enabling high performance lithium storage in aluminum: The double edged surface oxide journal, November 2017

Comparison of Cycling Performance of Lithium Ion Cell Anode Graphites journal, January 2012

High damage tolerance of electrochemically lithiated silicon journal, September 2015

Nanoscale Chemical Evolution of Silicon Negative Electrodes Characterized by Low-Loss STEM-EELS journal, November 2016

Valence electron energy-loss spectroscopy of silicon negative electrodes for lithium batteries journal, January 2010

Synergetic Effects of Inorganic Components in Solid Electrolyte Interphase on High Cycle Efficiency of Lithium Ion Batteries journal, February 2016

Li + Transport and Mechanical Properties of Model Solid Electrolyte Interphases (SEI): Insight from Atomistic Molecular Dynamics Simulations journal, July 2017

Cryogenic Electron Microscopy for Characterizing and Diagnosing Batteries journal, November 2018

Inhomogeneous Electron Gas journal, November 1964

Self-Consistent Equations Including Exchange and Correlation Effects journal, November 1965

Ab initiomolecular dynamics for liquid metals journal, January 1993

Projector augmented-wave method journal, December 1994

Generalized Gradient Approximation Made Simple journal, October 1996

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Li Segregation Induces Structure and Strength Changes at the Amorphous Si/Cu Interface journal, September 2013

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

Bisalt ether electrolytes: a pathway towards lithium metal batteries with Ni-rich cathodes journal, January 2019

High-Efficiency Lithium-Metal Anode Enabled by Liquefied Gas Electrolytes journal, August 2019

Insights into the Structure and Transport of the Lithium, Sodium, Magnesium, and Zinc Bis(trifluoromethansulfonyl)imide Salts in Ionic Liquids journal, August 2018

Quantum Chemistry and Molecular Dynamics Simulation Study of Dimethyl Carbonate: Ethylene Carbonate Electrolytes Doped with LiPF 6 journal, February 2009

Computer simulation and the dielectric constant of polarizable polar systems journal, May 1984

Densities and Viscosities of the Binary Mixtures of Tetrahydrofuran with Isomeric Chlorobutanes at 298.15 K and 313.15 K journal, July 2006

Excess Enthalpy, Density, Speed of Sound, and Viscosity for 2-Methyltetrahydrofuran + 1-Butanol at (283.15, 298.15, and, 313.15) K journal, May 2006

Pulse-Gradient Spin-Echo 1 H, 7 Li, and 19 F NMR Diffusion and Ionic Conductivity Measurements of 14 Organic Electrolytes Containing LiN(SO 2 CF 3 ) 2 journal, January 1999

Molecular relaxation of lithium salts in 2-methyltetrahydrofuran at 25.degree.C journal, May 1984

Oxidative Stability and Initial Decomposition Reactions of Carbonate, Sulfone, and Alkyl Phosphate-Based Electrolytes journal, April 2013

Computational applications in organic electrochemistry journal, April 2017

Electrolytes for Lithium and Lithium-Ion Batteries book, January 2014

An In Situ X-Ray Diffraction Study of the Reaction of Li with Crystalline Si
journal, January 2007

Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells
journal, January 2007

Design of Amorphous Alloy Electrodes for Li-Ion Batteries
journal, January 2004

Effect of electrode structure on performance of Si anode in Li-ion batteries: Si particle size and conductive additive
journal, January 2005

Reversible Cycling of Crystalline Silicon Powder
journal, January 2007

A Critical Size of Silicon Nano-Anodes for Lithium Rechargeable Batteries
journal, March 2010

Anisotropic Swelling and Fracture of Silicon Nanowires during Lithiation
journal, August 2011

Crystalline-Amorphous Core−Shell Silicon Nanowires for High Capacity and High Current Battery Electrodes
journal, January 2009

High-rate aluminium yolk-shell nanoparticle anode for Li-ion battery with long cycle life and ultrahigh capacity
journal, August 2015

Interconnected Silicon Hollow Nanospheres for Lithium-Ion Battery Anodes with Long Cycle Life
journal, July 2011

Silicon Nanotube Battery Anodes
journal, November 2009

Nonfilling Carbon Coating of Porous Silicon Micrometer-Sized Particles for High-Performance Lithium Battery Anodes
journal, February 2015

High-performance lithium-ion anodes using a hierarchical bottom-up approach
journal, March 2010

Atomic-level characterization of transport cycle thermodynamics in the glycerol-3-phosphate:phosphate antiporter
journal, September 2015

High capacity silicon anodes enabled by MXene viscous aqueous ink
journal, February 2019

Self-healing chemistry enables the stable operation of silicon microparticle anodes for high-energy lithium-ion batteries
journal, November 2013

Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries
journal, July 2017

Silicon Microparticle Anodes with Self-Healing Multiple Network Binder
journal, May 2018

A Major Constituent of Brown Algae for Use in High-Capacity Li-Ion Batteries
journal, September 2011

Growth of conformal graphene cages on micrometre-sized silicon particles as stable battery anodes
journal, January 2016

Review—SEI: Past, Present and Future
journal, January 2017

Direct Visualization of the Solid Electrolyte Interphase and Its Effects on Silicon Electrochemical Performance
journal, August 2016

Solid Electrolyte Interphase Growth and Capacity Loss in Silicon Electrodes
journal, June 2016

Understanding Fluoroethylene Carbonate and Vinylene Carbonate Based Electrolytes for Si Anodes in Lithium Ion Batteries with NMR Spectroscopy
journal, July 2018

The Mechanism of SEI Formation on a Single Crystal Si(100) Electrode
journal, January 2015

"Water-in-salt" electrolyte enables high-voltage aqueous lithium-ion chemistries
journal, November 2015

Challenges with prediction of battery electrolyte electrochemical stability window and guiding the electrode – electrolyte stabilization
journal, February 2019

Advanced High-Voltage Aqueous Lithium-Ion Battery Enabled by “Water-in-Bisalt” Electrolyte
journal, April 2016

Dielectric Constants for Quantum Chemistry and Li-Ion Batteries: Solvent Blends of Ethylene Carbonate and Ethyl Methyl Carbonate
journal, September 2015

Stable cycling of high-voltage lithium metal batteries in ether electrolytes
journal, July 2018

High-Concentration Ether Electrolytes for Stable High-Voltage Lithium Metal Batteries
journal, March 2019

Surface chemistry and morphology of the solid electrolyte interphase on silicon nanowire lithium-ion battery anodes
journal, April 2009

Lithium Salt Effects on Silicon Electrode Performance and Solid Electrolyte Interphase (SEI) Structure, Role of Solution Structure on SEI Formation
journal, January 2017

Enabling high performance lithium storage in aluminum: The double edged surface oxide
journal, November 2017

Comparison of Cycling Performance of Lithium Ion Cell Anode Graphites
journal, January 2012

High damage tolerance of electrochemically lithiated silicon
journal, September 2015

Nanoscale Chemical Evolution of Silicon Negative Electrodes Characterized by Low-Loss STEM-EELS
journal, November 2016

Valence electron energy-loss spectroscopy of silicon negative electrodes for lithium batteries
journal, January 2010

Synergetic Effects of Inorganic Components in Solid Electrolyte Interphase on High Cycle Efficiency of Lithium Ion Batteries
journal, February 2016

Li ⁺ Transport and Mechanical Properties of Model Solid Electrolyte Interphases (SEI): Insight from Atomistic Molecular Dynamics Simulations
journal, July 2017

Cryogenic Electron Microscopy for Characterizing and Diagnosing Batteries
journal, November 2018

Inhomogeneous Electron Gas
journal, November 1964

Self-Consistent Equations Including Exchange and Correlation Effects
journal, November 1965

Ab initiomolecular dynamics for liquid metals
journal, January 1993

Projector augmented-wave method
journal, December 1994

Generalized Gradient Approximation Made Simple
journal, October 1996

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Li Segregation Induces Structure and Strength Changes at the Amorphous Si/Cu Interface
journal, September 2013

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

Bisalt ether electrolytes: a pathway towards lithium metal batteries with Ni-rich cathodes
journal, January 2019

High-Efficiency Lithium-Metal Anode Enabled by Liquefied Gas Electrolytes
journal, August 2019

Insights into the Structure and Transport of the Lithium, Sodium, Magnesium, and Zinc Bis(trifluoromethansulfonyl)imide Salts in Ionic Liquids
journal, August 2018

Quantum Chemistry and Molecular Dynamics Simulation Study of Dimethyl Carbonate: Ethylene Carbonate Electrolytes Doped with LiPF ₆
journal, February 2009

Computer simulation and the dielectric constant of polarizable polar systems
journal, May 1984

Densities and Viscosities of the Binary Mixtures of Tetrahydrofuran with Isomeric Chlorobutanes at 298.15 K and 313.15 K
journal, July 2006

Excess Enthalpy, Density, Speed of Sound, and Viscosity for 2-Methyltetrahydrofuran + 1-Butanol at (283.15, 298.15, and, 313.15) K
journal, May 2006

Pulse-Gradient Spin-Echo ¹ H, ⁷ Li, and ¹⁹ F NMR Diffusion and Ionic Conductivity Measurements of 14 Organic Electrolytes Containing LiN(SO ₂ CF ₃ ) ₂
journal, January 1999

Molecular relaxation of lithium salts in 2-methyltetrahydrofuran at 25.degree.C
journal, May 1984

Oxidative Stability and Initial Decomposition Reactions of Carbonate, Sulfone, and Alkyl Phosphate-Based Electrolytes
journal, April 2013

Computational applications in organic electrochemistry
journal, April 2017

Electrolytes for Lithium and Lithium-Ion Batteries
book, January 2014