Transport and mechanical behavior in PEO-LLZO composite electrolytes

Kim, Hong-Keun; Barai, Pallab; Chavan, Kanchan; Srinivasan, Venkat

doi:10.1007/s10008-022-05231-w

Title: Transport and mechanical behavior in PEO-LLZO composite electrolytes

Abstract

Abstract Composite solid electrolytes (CEs), wherein ion-conducting polymer and ceramic/glass is mixed, are promising candidates for all-solid-state batteries due to their promise of acceptable ionic conductivity and mechanical properties compared to their individual constituents. While numerous studies have focused on improving the performance of CEs, it is still unclear what the material targets are that can result in improved macroscopic performance especially in light of the coupled needs for high transport and high mechanical strength in these materials. In this study, a two-dimensional (2D) mathematical model is developed to investigate electrochemical and mechanical characteristics of CEs. The model is compared to CEs consisting of poly-ethylene-oxide (PEO) polymer and lithium lanthanum zirconium oxide (LLZO) ceramic material with examination of the impact of varying LLZO volume fractions. The potential drop at the PEO-LLZO interface is evaluated using the junction potential theory. Using experimental data from the literature, the model estimates the ionic conductivity, effective transference number, and mechanical stiffness of the CEs. While the mechanical stiffness improves with increasing volume fraction of LLZO, the impact on conductivity and transference number depends on interfacial resistance at the interface. Finally, the study reports CE’s potential to enhance Li-ion transport and mechanical properties to inhibitmore » lithium (Li) dendrite growth.« less

Authors:

Kim, Hong-Keun; Barai, Pallab; Chavan, Kanchan;

Publication Date:: Mon Jul 25 00:00:00 EDT 2022

Research Org.:: Argonne National Lab. (ANL), Argonne, IL (United States)

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

OSTI Identifier:: 1877696

Alternate Identifier(s):: OSTI ID: 1905891

Grant/Contract Number:: DEAC02-06CH11357; AC02-06CH11357

Resource Type:: Published Article

Journal Name:: Journal of Solid State Electrochemistry

Additional Journal Information:: Journal Name: Journal of Solid State Electrochemistry Journal Volume: 26 Journal Issue: 9; Journal ID: ISSN 1432-8488

Publisher:: Springer Science + Business Media

Country of Publication:: Germany

Language:: English

Subject:: 25 ENERGY STORAGE; composite solid electrolyte (CE); effective transference number; interfacial resistance; mechanical strength; total ionic conductivity

Citation Formats


                    Kim, Hong-Keun, Barai, Pallab, Chavan, Kanchan, and Srinivasan, Venkat. Transport and mechanical behavior in PEO-LLZO composite electrolytes.  Germany: N. p., 2022. 
Web.  doi:10.1007/s10008-022-05231-w.

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                    Kim, Hong-Keun, Barai, Pallab, Chavan, Kanchan, & Srinivasan, Venkat. Transport and mechanical behavior in PEO-LLZO composite electrolytes.  Germany.  https://doi.org/10.1007/s10008-022-05231-w

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                    Kim, Hong-Keun, Barai, Pallab, Chavan, Kanchan, and Srinivasan, Venkat. Mon .  
"Transport and mechanical behavior in PEO-LLZO composite electrolytes".  Germany.  https://doi.org/10.1007/s10008-022-05231-w.

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@article{osti_1877696,

  title        = {Transport and mechanical behavior in PEO-LLZO composite electrolytes},

  author       = {Kim, Hong-Keun and Barai, Pallab and Chavan, Kanchan and Srinivasan, Venkat},

  abstractNote = {Abstract Composite solid electrolytes (CEs), wherein ion-conducting polymer and ceramic/glass is mixed, are promising candidates for all-solid-state batteries due to their promise of acceptable ionic conductivity and mechanical properties compared to their individual constituents. While numerous studies have focused on improving the performance of CEs, it is still unclear what the material targets are that can result in improved macroscopic performance especially in light of the coupled needs for high transport and high mechanical strength in these materials. In this study, a two-dimensional (2D) mathematical model is developed to investigate electrochemical and mechanical characteristics of CEs. The model is compared to CEs consisting of poly-ethylene-oxide (PEO) polymer and lithium lanthanum zirconium oxide (LLZO) ceramic material with examination of the impact of varying LLZO volume fractions. The potential drop at the PEO-LLZO interface is evaluated using the junction potential theory. Using experimental data from the literature, the model estimates the ionic conductivity, effective transference number, and mechanical stiffness of the CEs. While the mechanical stiffness improves with increasing volume fraction of LLZO, the impact on conductivity and transference number depends on interfacial resistance at the interface. Finally, the study reports CE’s potential to enhance Li-ion transport and mechanical properties to inhibit lithium (Li) dendrite growth.},

  doi          = {10.1007/s10008-022-05231-w},

  journal      = {Journal of Solid State Electrochemistry},

  number       = 9,

  volume       = 26,

  place        = {Germany},

  year         = {Mon Jul 25 00:00:00 EDT 2022},

  month        = {Mon Jul 25 00:00:00 EDT 2022}

}

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Title: Transport and mechanical behavior in PEO-LLZO composite electrolytes

Abstract

Citation Formats

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Mechanical behavior of Li-ion-conducting crystalline oxide-based solid electrolytes: a brief review journal, November 2017

Composite modeling for the effective elastic properties of semicrystalline polymers journal, January 2007

Enhanced mechanical strength and ionic conductivity of LLZO solid electrolytes by oscillatory pressure sintering journal, October 2019

The Influence of Inert Oxide Fillers on Poly(ethylene oxide) and Amorphous Poly(ethylene oxide) Based Polymer Electrolytes † journal, September 2001

Properties of the Interphase Formed between Argyrodite-Type Li 6 PS 5 Cl and Polymer-Based PEO 10 :LiTFSI journal, October 2019

Interrelationships among Grain Size, Surface Composition, Air Stability, and Interfacial Resistance of Al-Substituted Li 7 La 3 Zr 2 O 12 Solid Electrolytes journal, August 2015

Fabrication and Properties of Composites of Poly(ethylene oxide) and Functionalized Carbon Nanotubes journal, October 2002

Influence of Electrolyte Modulus on the Local Current Density at a Dendrite Tip on a Lithium Metal Electrode journal, January 2016

Interfacial Stability of Li Metal–Solid Electrolyte Elucidated via in Situ Electron Microscopy journal, October 2016

Electrochemical properties of a ceramic-polymer-composite-solid electrolyte for Li-ion batteries journal, January 2016

Nanocomposites of Titanium Dioxide and Polystyrene-Poly(ethylene oxide) Block Copolymer as Solid-State Electrolytes for Lithium Metal Batteries journal, January 2013

Design of composite polymer electrolytes for Li ion batteries based on mechanical stability criteria journal, March 2012

Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure journal, October 2019

A theory of plasticity for carbon nanotube reinforced composites journal, April 2011

Free-Standing PEO/LiTFSI/LAGP Composite Electrolyte Membranes for Applications to Flexible Solid-State Lithium-Based Batteries journal, January 2019

Microstructure and Pressure-Driven Electrodeposition Stability in Solid-State Batteries journal, January 2021

Influence of the Processing on the Ionic Conductivity of Solid-State Hybrid Electrolytes Based on Glass-Ceramic Particles Dispersed in PEO with LiTFSI journal, September 2020

Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth journal, January 2018

Unveiling Interfacial Li-Ion Dynamics in Li 7 La 3 Zr 2 O 12 /PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteries journal, June 2021

Rational Design of Hierarchical “Ceramic‐in‐Polymer” and “Polymer‐in‐Ceramic” Electrolytes for Dendrite‐Free Solid‐State Batteries journal, March 2019

Effective properties of composite material based on total strain energy equivalence journal, June 2019

Particles in composite polymer electrolyte for solid-state lithium batteries: A review journal, January 2022

Investigating the Calcination and Sintering of Li 7 La 3 Zr 2 O 12 (LLZO) Solid Electrolytes Using Operando Synchrotron X-ray Characterization and Mesoscale Modeling journal, June 2021

Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction journal, December 2015

Polymer-ceramic composite electrolytes for all-solid-state lithium batteries: Ionic conductivity and chemical interaction enhanced by oxygen vacancy in ceramic nanofibers journal, May 2021

Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes journal, January 2019

Determining and Minimizing Resistance for Ion Transport at the Polymer/Ceramic Electrolyte Interface
journal, April 2019

Elastic Properties of the Solid Electrolyte Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO)
journal, December 2015

Optimization of Block Copolymer Electrolytes for Lithium Metal Batteries
journal, June 2015

PEO/LAGP hybrid solid polymer electrolytes for ambient temperature lithium batteries by solvent-free, “one pot” preparation
journal, December 2019

Promising Routes to a High Li ⁺ Transference Number Electrolyte for Lithium Ion Batteries
journal, October 2017

Lithium Dendrite in All-Solid-State Batteries: Growth Mechanisms, Suppression Strategies, and Characterizations
journal, July 2020

Controlling Ionic Transport through the PEO-LiTFSI/LLZTO Interface
journal, January 2019

Improving Ionic Conductivity with Bimodal-Sized Li ₇ La ₃ Zr ₂ O ₁₂ Fillers for Composite Polymer Electrolytes
journal, March 2019

Room temperature elastic moduli and Vickers hardness of hot-pressed LLZO cubic garnet
journal, July 2012

Review on Polymer-Based Composite Electrolytes for Lithium Batteries
journal, August 2019

Recent advances in all-solid-state rechargeable lithium batteries
journal, March 2017

Publisher Correction: High-energy long-cycling all-solid-state lithium metal batteries enabled by silver–carbon composite anodes
journal, March 2020

Comparing Cycling Characteristics of Symmetric Lithium-Polymer-Lithium Cells with Theoretical Predictions
journal, January 2018

Some elastic properties of reinforced solids, with special reference to isotropic ones containing spherical inclusions
journal, January 1984

Ionic Conduction in Composite Polymer Electrolytes: Case of PEO:Ga-LLZO Composites
journal, December 2018

Li ₂ CO ₃ : A Critical Issue for Developing Solid Garnet Batteries
journal, November 2019

Garnet–Polymer Composite Electrolytes: New Insights on Local Li-Ion Dynamics and Electrodeposition Stability with Li Metal Anodes
journal, January 2019

Electrochemical performance of a solvent-free hybrid ceramic-polymer electrolyte based on Li 7 La 3 Zr 2 O 12 in P(EO) 15 LiTFSI
journal, June 2017

Flexible and ion-conducting membrane electrolytes for solid-state lithium batteries: Dispersion of garnet nanoparticles in insulating polyethylene oxide
journal, October 2016

The Impact of Elastic Deformation on Deposition Kinetics at Lithium/Polymer Interfaces
journal, January 2005

Synergistic Coupling between Li _6.75 La ₃ Zr _1.75 Ta _0.25 O ₁₂ and Poly(vinylidene fluoride) Induces High Ionic Conductivity, Mechanical Strength, and Thermal Stability of Solid Composite Electrolytes
journal, September 2017

Electrochemical Stability of Li ₁₀ GeP ₂ S ₁₂ and Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolytes
journal, January 2016

A three-dimensional interconnected polymer/ceramic composite as a thin film solid electrolyte
journal, April 2020

Newman and Balsara on Electrochemical Systems Fourth Edition
journal, March 2021

Microstructure Evolution in Lithium-Ion Battery Electrode Processing
journal, January 2014

Effect of particle agglomeration and interphase on the glass transition temperature of polymer nanocomposites
journal, April 2011

A Generalized Approach for Evaluating the Mechanical Properties of Polymer Nanocomposites Reinforced with Spherical Fillers
journal, March 2021

A.c. electrical properties of composite solid electrolytes
journal, October 1991

Lithium Ion Pathway within Li ₇ La ₃ Zr ₂ O ₁₂ -Polyethylene Oxide Composite Electrolytes
journal, September 2016

Mechanical behavior of Li-ion-conducting crystalline oxide-based solid electrolytes: a brief review
journal, November 2017

Composite modeling for the effective elastic properties of semicrystalline polymers
journal, January 2007

Enhanced mechanical strength and ionic conductivity of LLZO solid electrolytes by oscillatory pressure sintering
journal, October 2019

The Influence of Inert Oxide Fillers on Poly(ethylene oxide) and Amorphous Poly(ethylene oxide) Based Polymer Electrolytes ^†
journal, September 2001

Properties of the Interphase Formed between Argyrodite-Type Li ₆ PS ₅ Cl and Polymer-Based PEO ₁₀ :LiTFSI
journal, October 2019

Interrelationships among Grain Size, Surface Composition, Air Stability, and Interfacial Resistance of Al-Substituted Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolytes
journal, August 2015

Fabrication and Properties of Composites of Poly(ethylene oxide) and Functionalized Carbon Nanotubes
journal, October 2002

Influence of Electrolyte Modulus on the Local Current Density at a Dendrite Tip on a Lithium Metal Electrode
journal, January 2016

Interfacial Stability of Li Metal–Solid Electrolyte Elucidated via in Situ Electron Microscopy
journal, October 2016

Electrochemical properties of a ceramic-polymer-composite-solid electrolyte for Li-ion batteries
journal, January 2016

Nanocomposites of Titanium Dioxide and Polystyrene-Poly(ethylene oxide) Block Copolymer as Solid-State Electrolytes for Lithium Metal Batteries
journal, January 2013

Design of composite polymer electrolytes for Li ion batteries based on mechanical stability criteria
journal, March 2012

Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure
journal, October 2019

A theory of plasticity for carbon nanotube reinforced composites
journal, April 2011

Free-Standing PEO/LiTFSI/LAGP Composite Electrolyte Membranes for Applications to Flexible Solid-State Lithium-Based Batteries
journal, January 2019

Microstructure and Pressure-Driven Electrodeposition Stability in Solid-State Batteries
journal, January 2021

Influence of the Processing on the Ionic Conductivity of Solid-State Hybrid Electrolytes Based on Glass-Ceramic Particles Dispersed in PEO with LiTFSI
journal, September 2020

Impact of External Pressure and Electrolyte Transport Properties on Lithium Dendrite Growth
journal, January 2018

Unveiling Interfacial Li-Ion Dynamics in Li ₇ La ₃ Zr ₂ O ₁₂ /PEO(LiTFSI) Composite Polymer-Ceramic Solid Electrolytes for All-Solid-State Lithium Batteries
journal, June 2021

Rational Design of Hierarchical “Ceramic‐in‐Polymer” and “Polymer‐in‐Ceramic” Electrolytes for Dendrite‐Free Solid‐State Batteries
journal, March 2019

Effective properties of composite material based on total strain energy equivalence
journal, June 2019

Particles in composite polymer electrolyte for solid-state lithium batteries: A review
journal, January 2022

Investigating the Calcination and Sintering of Li ₇ La ₃ Zr ₂ O ₁₂ (LLZO) Solid Electrolytes Using Operando Synchrotron X-ray Characterization and Mesoscale Modeling
journal, June 2021

Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction
journal, December 2015

Polymer-ceramic composite electrolytes for all-solid-state lithium batteries: Ionic conductivity and chemical interaction enhanced by oxygen vacancy in ceramic nanofibers
journal, May 2021

Nanothin film conductivity measurements reveal interfacial influence on ion transport in polymer electrolytes
journal, January 2019