Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries

Li, Dazhe; Wang, Hui; Luo, Longbo; Zhu, Jiadeng; Li, Junfeng; Liu, Pengqing; Yu, Yuanyuan; Jiang, Mengjin

doi:10.1021/acsaem.0c02767

Title: Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries

Abstract

Traditional polyolefin separators used in lithium-ion batteries (LIBs) are seriously limited by the issues of inferior security and poor electrolyte wettability. Most of the very promising candidate separators based on heat-resistant polymers are, however, inherently difficult to process. Herein, a unique sulfonated aromatic heterocyclic polymer, lithiated poly(diphenyl ether oxadiazole) sulfonate (Li-SPEOD), was synthesized through a simple one-pot method and further electrospun to act as a novel separator (es-Li-SPEOD) for LIBs. In this work, the prepared Li-SPEOD possesses a high degree of sulfonation with a high molecular weight (M_w = 4.31 × 10⁵). The es-Li-SPEOD separator exhibits excellent mechanical and fire-resistance properties and is able to maintain dimensional stability at a temperature of even up to 400 °C in air. The ionic conductivity (3.57 mS cm^–1) and lithium-ion transference number (0.37) of the es-Li-SPEOD with an electrochemical stability window of 4.5 V vs Li⁺/Li can be improved by 382.4 and 32.1%, respectively, compared to those of Celgard-2500 in the LiPF₆ electrolyte. The enhanced rate capability and cycle performance of the LiFePO₄–Li half-cell are therefore obtained. Moreover, the es-Li-SPEOD displays an outstanding dendrite-suppressing effect for the lithium metal anode. This research proves that the Li-SPEOD-based separator has a broad application perspective inmore » next-generation lithium batteries.« less

Authors:

Li, Dazhe ^[1]; Wang, Hui ^[1]; Luo, Longbo ^[1];

^[2]; Li, Junfeng ^[3];

^[1]; Yu, Yuanyuan ^[1];

^[1]

Sichuan Univ., Chengdu (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Luoyang Normal University (China)

Publication Date:: Wed Jan 06 00:00:00 EST 2021

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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

OSTI Identifier:: 1845804

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: ACS Applied Energy Materials

Additional Journal Information:: Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2574-0962

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 25 ENERGY STORAGE; polyoxadiazole sulfonate; polymeric single-lithium-ion conductor; heat-resistant polymer; nanofibrous separator; LIBs

Citation Formats


                    Li, Dazhe, Wang, Hui, Luo, Longbo, Zhu, Jiadeng, Li, Junfeng, Liu, Pengqing, Yu, Yuanyuan, and Jiang, Mengjin. Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries.  United States: N. p., 2021. 
Web.  doi:10.1021/acsaem.0c02767.

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                    Li, Dazhe, Wang, Hui, Luo, Longbo, Zhu, Jiadeng, Li, Junfeng, Liu, Pengqing, Yu, Yuanyuan, & Jiang, Mengjin. Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries.  United States.  https://doi.org/10.1021/acsaem.0c02767

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                    Li, Dazhe, Wang, Hui, Luo, Longbo, Zhu, Jiadeng, Li, Junfeng, Liu, Pengqing, Yu, Yuanyuan, and Jiang, Mengjin. Wed .  
"Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries".  United States.  https://doi.org/10.1021/acsaem.0c02767.  https://www.osti.gov/servlets/purl/1845804.

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@article{osti_1845804,

  title        = {Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries},

  author       = {Li, Dazhe and Wang, Hui and Luo, Longbo and Zhu, Jiadeng and Li, Junfeng and Liu, Pengqing and Yu, Yuanyuan and Jiang, Mengjin},

  abstractNote = {Traditional polyolefin separators used in lithium-ion batteries (LIBs) are seriously limited by the issues of inferior security and poor electrolyte wettability. Most of the very promising candidate separators based on heat-resistant polymers are, however, inherently difficult to process. Herein, a unique sulfonated aromatic heterocyclic polymer, lithiated poly(diphenyl ether oxadiazole) sulfonate (Li-SPEOD), was synthesized through a simple one-pot method and further electrospun to act as a novel separator (es-Li-SPEOD) for LIBs. In this work, the prepared Li-SPEOD possesses a high degree of sulfonation with a high molecular weight (Mw = 4.31 × 105). The es-Li-SPEOD separator exhibits excellent mechanical and fire-resistance properties and is able to maintain dimensional stability at a temperature of even up to 400 °C in air. The ionic conductivity (3.57 mS cm–1) and lithium-ion transference number (0.37) of the es-Li-SPEOD with an electrochemical stability window of 4.5 V vs Li+/Li can be improved by 382.4 and 32.1%, respectively, compared to those of Celgard-2500 in the LiPF6 electrolyte. The enhanced rate capability and cycle performance of the LiFePO4–Li half-cell are therefore obtained. Moreover, the es-Li-SPEOD displays an outstanding dendrite-suppressing effect for the lithium metal anode. This research proves that the Li-SPEOD-based separator has a broad application perspective in next-generation lithium batteries.},

  doi          = {10.1021/acsaem.0c02767},

  journal      = {ACS Applied Energy Materials},

  number       = 1,

  volume       = 4,

  place        = {United States},

  year         = {Wed Jan 06 00:00:00 EST 2021},

  month        = {Wed Jan 06 00:00:00 EST 2021}

}

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Title: Electrospun Separator Based on Sulfonated Polyoxadiazole with Outstanding Thermal Stability and Electrochemical Properties for Lithium-Ion Batteries

Abstract

Citation Formats

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Sulfonated polyoxadiazole synthesis and processing into ion‐conducting films journal, July 2020

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Proton Dissociation of Sulfonated Polysulfones: Influence of Molecular Structure and Conformation journal, January 2015

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Single-Ion Conducting Electrolyte Based on Electrospun Nanofibers for High-Performance Lithium Batteries journal, January 2019

Ultrastrong Polyoxyzole Nanofiber Membranes for Dendrite-Proof and Heat-Resistant Battery Separators journal, April 2016

Robust fluorinated polyimide nanofibers membrane for high-performance lithium-ion batteries journal, March 2018

Preparation and Properties of an Alginate-Based Fiber Separator for Lithium-Ion Batteries journal, August 2020

The Effect of Sulfonation Level and Molecular Weight on the Tensile Properties of Polyoxadiazoles journal, November 2008

Performance enhancement of polybenzimidazole based high temperature proton exchange membranes with multifunctional crosslinker and highly sulfonated polyaniline journal, March 2018

Single-step synthesis of sulfonated polyoxadiazoles and their use as proton conducting membranes journal, January 2008

Highly porous single ion conducting polymer electrolyte for advanced lithium-ion batteries via facile water-induced phase separation process journal, December 2018

Uniform Li deposition regulated via three-dimensional polyvinyl alcohol nanofiber networks for effective Li metal anodes journal, January 2018

Synthesis and Characterization of New Coordination Polymers Generated from Oxadiazole-Containing Organic Ligands and Inorganic Silver(I) Salts journal, January 2003

Characterization of partially sulfonated polyoxadiazoles and oxadiazole–triazole copolymers journal, May 2007

From Nature to Energy Storage: A Novel Sustainable 3D Cross-Linked Chitosan–PEGGE-Based Gel Polymer Electrolyte with Excellent Lithium-Ion Transport Properties for Lithium Batteries journal, October 2018

Novel lithium ion battery separator based on hydroxymethyl functionalized poly(ether ether ketone) journal, October 2017

A review of recent developments in membrane separators for rechargeable lithium-ion batteries journal, January 2014

Thermotolerant separators for safe lithium-ion batteries under extreme conditions journal, January 2020

Two-dimensional molecular brush-functionalized porous bilayer composite separators toward ultrastable high-current density lithium metal anodes journal, March 2019

Aromatic Poly(1, 3, 4-Oxadiazoe)s as Advanced materials journal, July 1997

Electrochemical characteristics of electrospun poly(methyl methacrylate)/polyvinyl chloride as gel polymer electrolytes for lithium ion battery journal, December 2011

Study of the thermal decomposition and flame-retardant mechanism of sulfonated polyoxadiazole fibers journal, August 2016

Polarity-assisted formation of hollow-frame sheathed nitrogen-doped nanofibrous carbon for supercapacitors journal, January 2019

Novel Polyimide Separator Prepared with Two Porogens for Safe Lithium-Ion Batteries journal, December 2019

Ultrahigh-strength, nonflammable and high-wettability separators based on novel polyimide-core@polybenzimidazole-sheath nanofibers for advanced and safe lithium-ion batteries journal, July 2019

Polymer electrolyte based on chemically stable and highly conductive alkali-doped polyoxadiazole for direct borohydride fuel cell journal, September 2011

Gel Polymer Electrolyte with High Li + Transference Number Enhancing the Cycling Stability of Lithium Anodes journal, January 2019

Design Principles of Functional Polymer Separators for High-Energy, Metal-Based Batteries journal, December 2017

Eco-friendly cellulose nanofiber paper-derived separator membranes featuring tunable nanoporous network channels for lithium-ion batteries journal, January 2012

A Composite Gel Polymer Electrolyte with High Performance Based on Poly(Vinylidene Fluoride) and Polyborate for Lithium Ion Batteries journal, August 2013

PAN/PI functional double-layer coating for dendrite-free lithium metal anodes journal, January 2020

Polymer Nanofiber-Guided Uniform Lithium Deposition for Battery Electrodes journal, April 2015

Synthesis and characterization of polyhydrazides and poly(1,3,4-oxadiazole)s containing multiple arylene ether linkages and pendent pentadecyl chains journal, August 2016

Recent advances on separator membranes for lithium-ion battery applications: From porous membranes to solid electrolytes journal, November 2019

PMMA-assisted Li deposition towards 3D continuous dendrite-free lithium anode journal, January 2019

Protonation of Sulfonated Poly(4,4′-diphenylether-1,3,4-oxadiazole) Membranes journal, March 2007

Porous cellulose diacetate-SiO 2 composite coating on polyethylene separator for high-performance lithium-ion battery journal, August 2016

Fluorinated polyoxadiazole for high-temperature polymer electrolyte membrane fuel cells journal, August 2008

Hierarchical Chitin Fibers with Aligned Nanofibrillar Architectures: A Nonwoven-Mat Separator for Lithium Metal Batteries journal, May 2017

One-pot method for the synthesis of sulfonated poly(1,3,4-oxadiazoles) based on 4,4’-oxydibenzoic acid journal, September 2016

Core–shell-structured nanofibrous membrane as advanced separator for lithium-ion batteries journal, July 2016

Robust polyetherimide fibrous membrane with crosslinked topographies fabricated via in-situ micro-melting and its application as superior Lithium-ion battery separator with shutdown function journal, March 2018

Thermomechanical analysis and durability of commercial micro-porous polymer Li-ion battery separators journal, March 2011

A borate-rich, cross-linked gel polymer electrolyte with near-single ion conduction for lithium metal batteries journal, January 2019

Hydroxyl Functionalized Polytriazole- co -polyoxadiazole as Substrates for Forward Osmosis Membranes journal, February 2015

Determination of hydrazide content in poly(oxadiazole-hydrazide) copolymers by NMR and thermal analysis journal, September 2003

Stability Analysis of Electrodeposition across a Structured Electrolyte with Immobilized Anions journal, January 2014

Poly(arylene ether)-Based Single-Ion Conductors for Lithium-Ion Batteries
journal, December 2015

Electrostatically Assembling 2D Nanosheets of MXene and MOF‐Derivatives into 3D Hollow Frameworks for Enhanced Lithium Storage
journal, October 2019

Superior Thermally Stable and Nonflammable Porous Polybenzimidazole Membrane with High Wettability for High-Power Lithium-Ion Batteries
journal, February 2017

A facile grinding approach to embed red phosphorus in N,P-codoped hierarchical porous carbon for superior lithium storage
journal, September 2019

Uniform Lithium Deposition Induced by Polyacrylonitrile Submicron Fiber Array for Stable Lithium Metal Anode
journal, March 2017

Sulfonated polyoxadiazole synthesis and processing into ion‐conducting films
journal, July 2020

In Situ Fabrication of Ni ₂ P Nanoparticles Embedded in Nitrogen and Phosphorus Codoped Carbon Nanofibers as a Superior Anode for Li-Ion Batteries
journal, October 2018

Proton Dissociation of Sulfonated Polysulfones: Influence of Molecular Structure and Conformation
journal, January 2015

Poly(m-phenylene isophthalamide) separator for improving the heat resistance and power density of lithium-ion batteries
journal, October 2016

Synthesis, Characterization, and Study of the Thermal Properties of New Poly(arylene ether 1,3,4-oxadiazole)s
journal, December 2000

Preparation and evaluation of sulfonated polyoxadiazole membrane containing phenol moiety for PEMFC application
journal, September 2015

Single-Ion Conducting Electrolyte Based on Electrospun Nanofibers for High-Performance Lithium Batteries
journal, January 2019

Ultrastrong Polyoxyzole Nanofiber Membranes for Dendrite-Proof and Heat-Resistant Battery Separators
journal, April 2016

Robust fluorinated polyimide nanofibers membrane for high-performance lithium-ion batteries
journal, March 2018

Preparation and Properties of an Alginate-Based Fiber Separator for Lithium-Ion Batteries
journal, August 2020

The Effect of Sulfonation Level and Molecular Weight on the Tensile Properties of Polyoxadiazoles
journal, November 2008

Performance enhancement of polybenzimidazole based high temperature proton exchange membranes with multifunctional crosslinker and highly sulfonated polyaniline
journal, March 2018

Single-step synthesis of sulfonated polyoxadiazoles and their use as proton conducting membranes
journal, January 2008

Highly porous single ion conducting polymer electrolyte for advanced lithium-ion batteries via facile water-induced phase separation process
journal, December 2018

Uniform Li deposition regulated via three-dimensional polyvinyl alcohol nanofiber networks for effective Li metal anodes
journal, January 2018

Synthesis and Characterization of New Coordination Polymers Generated from Oxadiazole-Containing Organic Ligands and Inorganic Silver(I) Salts
journal, January 2003

Characterization of partially sulfonated polyoxadiazoles and oxadiazole–triazole copolymers
journal, May 2007

From Nature to Energy Storage: A Novel Sustainable 3D Cross-Linked Chitosan–PEGGE-Based Gel Polymer Electrolyte with Excellent Lithium-Ion Transport Properties for Lithium Batteries
journal, October 2018

Novel lithium ion battery separator based on hydroxymethyl functionalized poly(ether ether ketone)
journal, October 2017

A review of recent developments in membrane separators for rechargeable lithium-ion batteries
journal, January 2014

Thermotolerant separators for safe lithium-ion batteries under extreme conditions
journal, January 2020

Two-dimensional molecular brush-functionalized porous bilayer composite separators toward ultrastable high-current density lithium metal anodes
journal, March 2019

Aromatic Poly(1, 3, 4-Oxadiazoe)s as Advanced materials
journal, July 1997

Electrochemical characteristics of electrospun poly(methyl methacrylate)/polyvinyl chloride as gel polymer electrolytes for lithium ion battery
journal, December 2011

Study of the thermal decomposition and flame-retardant mechanism of sulfonated polyoxadiazole fibers
journal, August 2016

Polarity-assisted formation of hollow-frame sheathed nitrogen-doped nanofibrous carbon for supercapacitors
journal, January 2019

Novel Polyimide Separator Prepared with Two Porogens for Safe Lithium-Ion Batteries
journal, December 2019

Ultrahigh-strength, nonflammable and high-wettability separators based on novel polyimide-core@polybenzimidazole-sheath nanofibers for advanced and safe lithium-ion batteries
journal, July 2019

Polymer electrolyte based on chemically stable and highly conductive alkali-doped polyoxadiazole for direct borohydride fuel cell
journal, September 2011

Gel Polymer Electrolyte with High Li ⁺ Transference Number Enhancing the Cycling Stability of Lithium Anodes
journal, January 2019

Design Principles of Functional Polymer Separators for High-Energy, Metal-Based Batteries
journal, December 2017

Eco-friendly cellulose nanofiber paper-derived separator membranes featuring tunable nanoporous network channels for lithium-ion batteries
journal, January 2012

A Composite Gel Polymer Electrolyte with High Performance Based on Poly(Vinylidene Fluoride) and Polyborate for Lithium Ion Batteries
journal, August 2013

PAN/PI functional double-layer coating for dendrite-free lithium metal anodes
journal, January 2020

Polymer Nanofiber-Guided Uniform Lithium Deposition for Battery Electrodes
journal, April 2015

Synthesis and characterization of polyhydrazides and poly(1,3,4-oxadiazole)s containing multiple arylene ether linkages and pendent pentadecyl chains
journal, August 2016

Recent advances on separator membranes for lithium-ion battery applications: From porous membranes to solid electrolytes
journal, November 2019

PMMA-assisted Li deposition towards 3D continuous dendrite-free lithium anode
journal, January 2019

Protonation of Sulfonated Poly(4,4′-diphenylether-1,3,4-oxadiazole) Membranes
journal, March 2007

Porous cellulose diacetate-SiO 2 composite coating on polyethylene separator for high-performance lithium-ion battery
journal, August 2016

Fluorinated polyoxadiazole for high-temperature polymer electrolyte membrane fuel cells
journal, August 2008

Hierarchical Chitin Fibers with Aligned Nanofibrillar Architectures: A Nonwoven-Mat Separator for Lithium Metal Batteries
journal, May 2017

One-pot method for the synthesis of sulfonated poly(1,3,4-oxadiazoles) based on 4,4’-oxydibenzoic acid
journal, September 2016

Core–shell-structured nanofibrous membrane as advanced separator for lithium-ion batteries
journal, July 2016

Robust polyetherimide fibrous membrane with crosslinked topographies fabricated via in-situ micro-melting and its application as superior Lithium-ion battery separator with shutdown function
journal, March 2018

Thermomechanical analysis and durability of commercial micro-porous polymer Li-ion battery separators
journal, March 2011

A borate-rich, cross-linked gel polymer electrolyte with near-single ion conduction for lithium metal batteries
journal, January 2019

Hydroxyl Functionalized Polytriazole- co -polyoxadiazole as Substrates for Forward Osmosis Membranes
journal, February 2015

Determination of hydrazide content in poly(oxadiazole-hydrazide) copolymers by NMR and thermal analysis
journal, September 2003

Stability Analysis of Electrodeposition across a Structured Electrolyte with Immobilized Anions
journal, January 2014