Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte

Mackanic, David G.; Michaels, Wesley; Lee, Minah; Feng, Dawei; Lopez, Jeffrey; Qin, Jian; Cui, Yi; Bao, Zhenan

doi:10.1002/aenm.201800703

Title: Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte

Abstract

Abstract Solid polymer electrolytes (SPEs) promise to improve the safety and performance of lithium ion batteries (LIBs). However, the low ionic conductivity and transference number of conventional poly(ethylene oxide) (PEO)‐based SPEs preclude their widespread implementation. Herein, crosslinked poly(tetrahydrofuran) (xPTHF) is introduced as a promising polymer matrix for “beyond PEO” SPEs. The crosslinking procedure creates thermally stable, mechanically robust membranes for use in LIBs. Molecular dynamics and density functional theory (DFT) simulations accompanied by ⁷ Li NMR measurements show that the lower spatial concentration of oxygen atoms in the xPTHF backbone leads to loosened O–Li ⁺ coordination. This weakened interaction enhances ion transport; xPTHF has a high lithium transference number of 0.53 and higher lithium conductivity than a xPEO SPE of the same length at room temperature. It is demonstrated that organic additives further weaken the O–Li ⁺ interaction, enabling room temperature ionic conductivity of 1.2 × 10 ⁻⁴ S cm ⁻¹ with 18 wt% N,N ‐dimethylformamide in xPTHF. In a solid‐state LIB application, neat xPTHF SPEs cycle with near theoretical capacity for 100 cycles at 70 °C, with rate capability up to 1 C. The plasticized xPTHF SPEs operate at room temperature while maintaining respectable rate capability and capacity. Themore »« less

Authors:

^[1]; Michaels, Wesley ^[1]; Lee, Minah ^[1]; Feng, Dawei ^[1]; Lopez, Jeffrey ^[1]; Qin, Jian ^[1]; Cui, Yi ^[2];

^[1]

Stanford University Department of Chemical Engineering Shriram Center 443 Via Ortega, Room 307 Stanford CA 94305‐4125 USA
Stanford University Department of Materials Science McCullough 476 Lomita Mall, Room 343 Stanford CA 94305 USA

Publication Date:: Sun Jul 15 00:00:00 EDT 2018

Sponsoring Org.:: USDOE

OSTI Identifier:: 1460461

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: Advanced Energy Materials

Additional Journal Information:: Journal Name: Advanced Energy Materials Journal Volume: 8 Journal Issue: 25; Journal ID: ISSN 1614-6832

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Mackanic, David G., Michaels, Wesley, Lee, Minah, Feng, Dawei, Lopez, Jeffrey, Qin, Jian, Cui, Yi, and Bao, Zhenan. Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte.  Germany: N. p., 2018. 
Web.  doi:10.1002/aenm.201800703.

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                    Mackanic, David G., Michaels, Wesley, Lee, Minah, Feng, Dawei, Lopez, Jeffrey, Qin, Jian, Cui, Yi, & Bao, Zhenan. Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte.  Germany.  https://doi.org/10.1002/aenm.201800703

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                    Mackanic, David G., Michaels, Wesley, Lee, Minah, Feng, Dawei, Lopez, Jeffrey, Qin, Jian, Cui, Yi, and Bao, Zhenan. Sun .  
"Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte".  Germany.  https://doi.org/10.1002/aenm.201800703.

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@article{osti_1460461,

  title        = {Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte},

  author       = {Mackanic, David G. and Michaels, Wesley and Lee, Minah and Feng, Dawei and Lopez, Jeffrey and Qin, Jian and Cui, Yi and Bao, Zhenan},

  abstractNote = {Abstract Solid polymer electrolytes (SPEs) promise to improve the safety and performance of lithium ion batteries (LIBs). However, the low ionic conductivity and transference number of conventional poly(ethylene oxide) (PEO)‐based SPEs preclude their widespread implementation. Herein, crosslinked poly(tetrahydrofuran) (xPTHF) is introduced as a promising polymer matrix for “beyond PEO” SPEs. The crosslinking procedure creates thermally stable, mechanically robust membranes for use in LIBs. Molecular dynamics and density functional theory (DFT) simulations accompanied by 7 Li NMR measurements show that the lower spatial concentration of oxygen atoms in the xPTHF backbone leads to loosened O–Li + coordination. This weakened interaction enhances ion transport; xPTHF has a high lithium transference number of 0.53 and higher lithium conductivity than a xPEO SPE of the same length at room temperature. It is demonstrated that organic additives further weaken the O–Li + interaction, enabling room temperature ionic conductivity of 1.2 × 10 −4 S cm −1 with 18 wt% N,N ‐dimethylformamide in xPTHF. In a solid‐state LIB application, neat xPTHF SPEs cycle with near theoretical capacity for 100 cycles at 70 °C, with rate capability up to 1 C. The plasticized xPTHF SPEs operate at room temperature while maintaining respectable rate capability and capacity. The novel PTHF system demonstrated here represents an exciting platform for future studies involving SPEs.},

  doi          = {10.1002/aenm.201800703},

  journal      = {Advanced Energy Materials},

  number       = 25,

  volume       = 8,

  place        = {Germany},

  year         = {Sun Jul 15 00:00:00 EDT 2018},

  month        = {Sun Jul 15 00:00:00 EDT 2018}

}

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Molecular Force Field for Ionic Liquids Composed of Triflate or Bistriflylimide Anions
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High rate and stable cycling of lithium metal anode
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Qian, Jiangfeng; Henderson, Wesley A.; Xu, Wu
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DOI: 10.1038/ncomms7362

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Title: Crosslinked Poly(tetrahydrofuran) as a Loosely Coordinating Polymer Electrolyte

Abstract

Citation Formats

Transferable Potentials for Phase Equilibria. 6. United-Atom Description for Ethers, Glycols, Ketones, and Aldehydes journal, November 2004

The plastic-crystalline phase of succinonitrile as a universal matrix for solid-state ionic conductors journal, June 2004

Preparation of organic/inorganic hybrid semi-interpenetrating network polymer electrolytes based on poly(ethylene oxide-co-ethylene carbonate) for all-solid-state lithium batteries at elevated temperatures journal, June 2014

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A Superior Polymer Electrolyte with Rigid Cyclic Carbonate Backbone for Rechargeable Lithium Ion Batteries journal, May 2017

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In Situ Generation of Poly (Vinylene Carbonate) Based Solid Electrolyte with Interfacial Stability for LiCoO 2 Lithium Batteries journal, November 2016

Effect of donor number of solvent on the conductivity behaviour of nonaqueous proton-conducting polymer gel electrolytes journal, June 2003

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High Performance Solid Polymer Electrolytes for Rechargeable Batteries: A Self-Catalyzed Strategy toward Facile Synthesis journal, August 2017

Variation of the mesh size of PEO-based networks filled with TFSILi: from an Arrhenius to WLF type conductivity behavior journal, February 2000

Interfacial Challenges in Solid-State Li Ion Batteries journal, October 2015

Flexible Organic–Inorganic Hybrid Solid Electrolytes Formed via Thiol–Acrylate Photopolymerization journal, February 2017

Polymer Electrolytes journal, July 2013

Fast Li-ion conduction in poly(ethylene carbonate)-based electrolytes and composites filled with TiO 2 nanoparticles journal, January 2014

GROMACS: High performance molecular simulations through multi-level parallelism from laptops to supercomputers journal, September 2015

Ionic conductivity in crystalline polymer electrolytes journal, August 2001

Review of gel-type polymer electrolytes for lithium-ion batteries journal, February 1999

Li+-conductive polymer electrolytes derived from poly(1,3-dioxolane) and polytetrahydrofuran journal, January 1991

In situ preparation of poly(ethylene oxide)–SiO2 composite polymer electrolytes journal, April 2004

Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes journal, July 2015

CHARMM general force field: A force field for drug-like molecules compatible with the CHARMM all-atom additive biological force fields journal, January 2009

Complexes of alkali metal ions with poly(ethylene oxide) journal, November 1973

Polymer electrolytes for lithium polymer batteries journal, January 2016

Effect of propylene carbonate as a plasticizer in high molecular weight PEO_LiCF3SO3 electrolytes journal, May 1996

Vibrational, ac impedance and dielectric spectroscopic studies of poly(vinylacetate)–N,N–dimethylformamide–LiClO4 polymer gel electrolytes journal, August 2004

A comparison of models for calculating nuclear magnetic resonance shielding tensors journal, April 1996

Lithium ion conductivity in polyoxyethylene/polyethylenimine blends journal, March 2001

Transferable Potentials for Phase Equilibria. 1. United-Atom Description of n-Alkanes journal, March 1998

Review—Solid Electrolytes in Rechargeable Electrochemical Cells journal, January 2015

Conductivities of electrolytes based on PEI-b-PEO-b-PEI triblock copolymers with lithium and copper TFSI salts journal, March 2006

Replies to comments contained in “Conductivity hysteresis in polymer electrolytes incorporating poly(tetrahydrofuran)” by O. Akbulut, et al., Electrochim. Acta 52 (2007) 1983 journal, August 2007

Conductivity hysteresis in polymer electrolytes incorporating poly(tetrahydrofuran) journal, January 2007

What Can We Learn from Ionic Conductivity Measurements in Polymer Electrolytes? A Case Study on Poly(ethylene oxide) (PEO)–NaI and PEO–LiTFSI journal, February 2012

Review—On Order and Disorder in Polymer Electrolytes journal, January 2015

Brønsted acid-free controlled polymerization of tetrahydrofuran catalyzed by recyclable rare earth triflates in the presence of epoxides journal, August 2012

The effects of radiation-induced crosslinking on the conductance of LiClO4·PEO electrolytes journal, January 1984

The Compensation Effect in the Vogel–Tammann–Fulcher (VTF) Equation for Polymer-Based Electrolytes journal, May 2017

Thermal stability and decomposition of lithium bis(fluorosulfonyl)imide (LiFSI) salts journal, January 2016

Computational Investigation on the Role of Plasticizers on Ion Conductivity in Poly(ethylene oxide) LiTFSI Electrolytes journal, April 2010

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Super Soft All-Ethylene Oxide Polymer Electrolyte for Safe All-Solid Lithium Batteries journal, January 2016

Improved Description of Nuclear Magnetic Resonance Chemical Shielding Constants Using the M06-L Meta-Generalized-Gradient-Approximation Density Functional journal, July 2008

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Thermally cured semi-interpenetrating electrolyte networks (s-IPN) for safe and aging-resistant secondary lithium polymer batteries journal, February 2016

Measurement of transference numbers for lithium ion electrolytes via four different methods, a comparative study journal, April 2011

Fire retardant, superionic solid state polymer electrolyte membranes for lithium ion batteries journal, February 2017

Nanocomposite polymer electrolytes for lithium batteries journal, July 1998

Highly conductive, completely amorphous polymer electrolyte membranes fabricated through photo-polymerization of poly(ethylene glycol diacrylate) in mixtures of solid plasticizer and lithium salt journal, January 2014

A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions journal, November 2006

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Thermal, electrical and mechanical properties of plasticized polymer electrolytes based on PEO/P(VDF-HFP) blends journal, November 2002

Electrochemical measurement of transference numbers in polymer electrolytes journal, December 1987

Investigation on solvent-free solid polymer electrolytes for advanced lithium batteries and their performance journal, February 2003

Performance of gel-type polymer electrolytes according to the affinity between polymer matrix and plasticizing solvent molecules journal, February 2001

Enhancing Cation Diffusion and Suppressing Anion Diffusion via Lewis-Acidic Polymer Electrolytes journal, January 2017

NMR determination of ionic structure in plasticized polyether-urethane polymer electrolytes journal, May 1996

Polymer electrolytes journal, January 1993

In-situ plasticized polymer electrolyte with double-network for flexible solid-state lithium-metal batteries journal, January 2018

Crystal Structure of the Polymer Electrolyte Poly(ethylene oxide)3:LiCF3SO3 journal, November 1993

Solid polymer electrolytes: materials designing and all-solid-state battery applications: an overview journal, October 2008

Importance of donor number in determining solvating ability of polymers and transport properties in gel-type polymer electrolytes journal, March 2000

PEO-Based Electrolyte Membranes Based on LiBC[sub 4]O[sub 8] Salt journal, January 2004

Self‐consistent molecular orbital methods 25. Supplementary functions for Gaussian basis sets journal, April 1984

Photocured PEO-based solid polymer electrolyte and its application to lithium–polymer batteries journal, January 2001

Mechanism of ion transport in PEO/LiTFSI complexes: Effect of temperature, molecular weight and end groups journal, October 2012

Electrochemical characterization of new conducting polymer electrolytes journal, June 1993

Hybrid Electrolytes with Controlled Network Structures for Lithium Metal Batteries journal, August 2015

Monte Carlo Calculations for Alcohols and Their Mixtures with Alkanes. Transferable Potentials for Phase Equilibria. 5. United-Atom Description of Primary, Secondary, and Tertiary Alcohols journal, April 2001

Transferable Potentials for Phase Equilibria. 6. United-Atom Description for Ethers, Glycols, Ketones, and Aldehydes
journal, November 2004

The plastic-crystalline phase of succinonitrile as a universal matrix for solid-state ionic conductors
journal, June 2004

Preparation of organic/inorganic hybrid semi-interpenetrating network polymer electrolytes based on poly(ethylene oxide-co-ethylene carbonate) for all-solid-state lithium batteries at elevated temperatures
journal, June 2014

Electrochemical comparison of several cross-linked polyethers
journal, April 1998

Correlation between Solvation Structure and Ion-Conductive Behavior of Concentrated Poly(ethylene carbonate)-Based Electrolytes
journal, June 2016

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

Conductivities, thermal properties and Raman studies of poly(tetramethylene glycol) based polymer electrolytes
journal, April 1998

Single-Ion Conducting Polymer Electrolytes for Lithium Metal Polymer Batteries that Operate at Ambient Temperature
journal, September 2016

A Superior Polymer Electrolyte with Rigid Cyclic Carbonate Backbone for Rechargeable Lithium Ion Batteries
journal, May 2017

Poly(ethylene oxide)-based electrolytes for lithium-ion batteries
journal, January 2015

Polymer solid electrolytes based on viologen-type poly(oxytetramethylene) ionene
journal, April 2004

In Situ Generation of Poly (Vinylene Carbonate) Based Solid Electrolyte with Interfacial Stability for LiCoO ₂ Lithium Batteries
journal, November 2016

Effect of donor number of solvent on the conductivity behaviour of nonaqueous proton-conducting polymer gel electrolytes
journal, June 2003

Solid Hybrid Polymer Electrolyte Networks: Nano-Structurable Materials for Lithium Batteries
journal, August 2002

Cross-Linked Solid Polymer Electrolyte for All-Solid-State Rechargeable Lithium Batteries
journal, December 2016

High Performance Solid Polymer Electrolytes for Rechargeable Batteries: A Self-Catalyzed Strategy toward Facile Synthesis
journal, August 2017

Variation of the mesh size of PEO-based networks filled with TFSILi: from an Arrhenius to WLF type conductivity behavior
journal, February 2000

Interfacial Challenges in Solid-State Li Ion Batteries
journal, October 2015

Flexible Organic–Inorganic Hybrid Solid Electrolytes Formed via Thiol–Acrylate Photopolymerization
journal, February 2017

Polymer Electrolytes
journal, July 2013

Fast Li-ion conduction in poly(ethylene carbonate)-based electrolytes and composites filled with TiO ₂ nanoparticles
journal, January 2014

GROMACS: High performance molecular simulations through multi-level parallelism from laptops to supercomputers
journal, September 2015

Ionic conductivity in crystalline polymer electrolytes
journal, August 2001

Review of gel-type polymer electrolytes for lithium-ion batteries
journal, February 1999

Li+-conductive polymer electrolytes derived from poly(1,3-dioxolane) and polytetrahydrofuran
journal, January 1991

In situ preparation of poly(ethylene oxide)–SiO2 composite polymer electrolytes
journal, April 2004

Systematic Computational and Experimental Investigation of Lithium-Ion Transport Mechanisms in Polyester-Based Polymer Electrolytes
journal, July 2015

CHARMM general force field: A force field for drug-like molecules compatible with the CHARMM all-atom additive biological force fields
journal, January 2009

Complexes of alkali metal ions with poly(ethylene oxide)
journal, November 1973

Polymer electrolytes for lithium polymer batteries
journal, January 2016

Effect of propylene carbonate as a plasticizer in high molecular weight PEO_LiCF3SO3 electrolytes
journal, May 1996

Vibrational, ac impedance and dielectric spectroscopic studies of poly(vinylacetate)–N,N–dimethylformamide–LiClO4 polymer gel electrolytes
journal, August 2004

A comparison of models for calculating nuclear magnetic resonance shielding tensors
journal, April 1996

Lithium ion conductivity in polyoxyethylene/polyethylenimine blends
journal, March 2001

Transferable Potentials for Phase Equilibria. 1. United-Atom Description of n-Alkanes
journal, March 1998

Review—Solid Electrolytes in Rechargeable Electrochemical Cells
journal, January 2015

Conductivities of electrolytes based on PEI-b-PEO-b-PEI triblock copolymers with lithium and copper TFSI salts
journal, March 2006

Replies to comments contained in “Conductivity hysteresis in polymer electrolytes incorporating poly(tetrahydrofuran)” by O. Akbulut, et al., Electrochim. Acta 52 (2007) 1983
journal, August 2007

Conductivity hysteresis in polymer electrolytes incorporating poly(tetrahydrofuran)
journal, January 2007

What Can We Learn from Ionic Conductivity Measurements in Polymer Electrolytes? A Case Study on Poly(ethylene oxide) (PEO)–NaI and PEO–LiTFSI
journal, February 2012

Review—On Order and Disorder in Polymer Electrolytes
journal, January 2015

Brønsted acid-free controlled polymerization of tetrahydrofuran catalyzed by recyclable rare earth triflates in the presence of epoxides
journal, August 2012

The effects of radiation-induced crosslinking on the conductance of LiClO4·PEO electrolytes
journal, January 1984

The Compensation Effect in the Vogel–Tammann–Fulcher (VTF) Equation for Polymer-Based Electrolytes
journal, May 2017

Thermal stability and decomposition of lithium bis(fluorosulfonyl)imide (LiFSI) salts
journal, January 2016

Computational Investigation on the Role of Plasticizers on Ion Conductivity in Poly(ethylene oxide) LiTFSI Electrolytes
journal, April 2010

Nonflammable perfluoropolyether-based electrolytes for lithium batteries
journal, February 2014

Super Soft All-Ethylene Oxide Polymer Electrolyte for Safe All-Solid Lithium Batteries
journal, January 2016

Improved Description of Nuclear Magnetic Resonance Chemical Shielding Constants Using the M06-L Meta-Generalized-Gradient-Approximation Density Functional
journal, July 2008

Ionic Conductivity of Polymeric Solid Electrolytes Based on Poly(propylene oxide) or Poly(tetramethylene oxide)
journal, November 1982

Improvement of heat stability of poly(l-lactic acid) by radiation-induced crosslinking
journal, June 2005

Thermally cured semi-interpenetrating electrolyte networks (s-IPN) for safe and aging-resistant secondary lithium polymer batteries
journal, February 2016

Measurement of transference numbers for lithium ion electrolytes via four different methods, a comparative study
journal, April 2011

Fire retardant, superionic solid state polymer electrolyte membranes for lithium ion batteries
journal, February 2017

Nanocomposite polymer electrolytes for lithium batteries
journal, July 1998

Highly conductive, completely amorphous polymer electrolyte membranes fabricated through photo-polymerization of poly(ethylene glycol diacrylate) in mixtures of solid plasticizer and lithium salt
journal, January 2014

A new local density functional for main-group thermochemistry, transition metal bonding, thermochemical kinetics, and noncovalent interactions
journal, November 2006

Highly conductive solid polymer electrolyte membranes based on polyethylene glycol-bis-carbamate dimethacrylate networks
journal, August 2017

Suppression of Lithium Dendrite Growth Using Cross-Linked Polyethylene/Poly(ethylene oxide) Electrolytes: A New Approach for Practical Lithium-Metal Polymer Batteries
journal, May 2014

Thermal, electrical and mechanical properties of plasticized polymer electrolytes based on PEO/P(VDF-HFP) blends
journal, November 2002

Electrochemical measurement of transference numbers in polymer electrolytes
journal, December 1987

Investigation on solvent-free solid polymer electrolytes for advanced lithium batteries and their performance
journal, February 2003

Performance of gel-type polymer electrolytes according to the affinity between polymer matrix and plasticizing solvent molecules
journal, February 2001

Enhancing Cation Diffusion and Suppressing Anion Diffusion via Lewis-Acidic Polymer Electrolytes
journal, January 2017

NMR determination of ionic structure in plasticized polyether-urethane polymer electrolytes
journal, May 1996

Polymer electrolytes
journal, January 1993

In-situ plasticized polymer electrolyte with double-network for flexible solid-state lithium-metal batteries
journal, January 2018

Crystal Structure of the Polymer Electrolyte Poly(ethylene oxide)3:LiCF3SO3
journal, November 1993

Solid polymer electrolytes: materials designing and all-solid-state battery applications: an overview
journal, October 2008

Importance of donor number in determining solvating ability of polymers and transport properties in gel-type polymer electrolytes
journal, March 2000

PEO-Based Electrolyte Membranes Based on LiBC[sub 4]O[sub 8] Salt
journal, January 2004

Self‐consistent molecular orbital methods 25. Supplementary functions for Gaussian basis sets
journal, April 1984

Photocured PEO-based solid polymer electrolyte and its application to lithium–polymer batteries
journal, January 2001

Mechanism of ion transport in PEO/LiTFSI complexes: Effect of temperature, molecular weight and end groups
journal, October 2012

Electrochemical characterization of new conducting polymer electrolytes
journal, June 1993

Hybrid Electrolytes with Controlled Network Structures for Lithium Metal Batteries
journal, August 2015

Monte Carlo Calculations for Alcohols and Their Mixtures with Alkanes. Transferable Potentials for Phase Equilibria. 5. United-Atom Description of Primary, Secondary, and Tertiary Alcohols
journal, April 2001

A highly reversible room-temperature lithium metal battery based on crosslinked hairy nanoparticles
journal, December 2015

Phase Behavior and Electrochemical Characterization of Blends of Perfluoropolyether, Poly(ethylene glycol), and a Lithium Salt
journal, January 2015

Structure and Ionic Conductivity of Polystyrene- block -poly(ethylene oxide) Electrolytes in the High Salt Concentration Limit
journal, February 2016