DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity

Abstract

We report that the use of lithium-ion conductive solid electrolytes offers a promising approach to address the polysulfide-shuttle and the lithium-dendrite problems in lithium-sulfur (Li-S) batteries. One critical issue with the development of solid-electrolyte Li-S batteries is the electrode-electrolyte interfaces. We present herein a strategic approach by employing a thin layer of a polymer with intrinsic nanoporosity (PIN) on a Li+-ion conductive solid electrolyte, which significantly enhances the ionic interfaces between the electrodes and the solid electrolyte. Among the various types of Li+-ion solid electrolytes, NASICON-type Li1+xAlxTi2-x(PO4)3 (LATP) offers advantages in terms of Li+-ion conductivity, stability in ambient environment, and practical viability. However, LATP is susceptible to reaction with both the Li-metal anode and polysulfides in Li-S batteries due to the presence of easily reducible Ti4+ ions in it. The coating with a thin layer of PIN presented in this study overcomes the above issues. At the negative-electrode side, the PIN layer prevents the direct contact of Li-metal with the LATP solid electrolyte, circumventing the reduction of LATP by Li metal. Lastly, at the positive electrode side, the PIN layer prevents the migration of polysulfides to the surface of LATP, preventing the reduction of LATP by polysulfides.

Authors:
 [1]; ORCiD logo [1]
  1. Univ. of Texas, Austin, TX (United States). Materials Science & Engineering Program and Texas Materials Institute
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1598245
Alternate Identifier(s):
OSTI ID: 1483149
Grant/Contract Number:  
SC0005397
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 29; Journal Issue: 3; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; electrode–electrolyte interface; lithium polysulfide; lithium‐sulfur batteries; polymer with intrinsic nanoporosity; solid electrolyte

Citation Formats

Yu, Xingwen, and Manthiram, Arumugam. Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity. United States: N. p., 2018. Web. doi:10.1002/adfm.201805996.
Yu, Xingwen, & Manthiram, Arumugam. Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity. United States. https://doi.org/10.1002/adfm.201805996
Yu, Xingwen, and Manthiram, Arumugam. Fri . "Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity". United States. https://doi.org/10.1002/adfm.201805996. https://www.osti.gov/servlets/purl/1598245.
@article{osti_1598245,
title = {Enhanced Interfacial Stability of Hybrid-Electrolyte Lithium-Sulfur Batteries with a Layer of Multifunctional Polymer with Intrinsic Nanoporosity},
author = {Yu, Xingwen and Manthiram, Arumugam},
abstractNote = {We report that the use of lithium-ion conductive solid electrolytes offers a promising approach to address the polysulfide-shuttle and the lithium-dendrite problems in lithium-sulfur (Li-S) batteries. One critical issue with the development of solid-electrolyte Li-S batteries is the electrode-electrolyte interfaces. We present herein a strategic approach by employing a thin layer of a polymer with intrinsic nanoporosity (PIN) on a Li+-ion conductive solid electrolyte, which significantly enhances the ionic interfaces between the electrodes and the solid electrolyte. Among the various types of Li+-ion solid electrolytes, NASICON-type Li1+xAlxTi2-x(PO4)3 (LATP) offers advantages in terms of Li+-ion conductivity, stability in ambient environment, and practical viability. However, LATP is susceptible to reaction with both the Li-metal anode and polysulfides in Li-S batteries due to the presence of easily reducible Ti4+ ions in it. The coating with a thin layer of PIN presented in this study overcomes the above issues. At the negative-electrode side, the PIN layer prevents the direct contact of Li-metal with the LATP solid electrolyte, circumventing the reduction of LATP by Li metal. Lastly, at the positive electrode side, the PIN layer prevents the migration of polysulfides to the surface of LATP, preventing the reduction of LATP by polysulfides.},
doi = {10.1002/adfm.201805996},
journal = {Advanced Functional Materials},
number = 3,
volume = 29,
place = {United States},
year = {Fri Nov 23 00:00:00 EST 2018},
month = {Fri Nov 23 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 39 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Lithium battery chemistries enabled by solid-state electrolytes
journal, February 2017


Building better batteries
journal, February 2008

  • Armand, M.; Tarascon, J.-M.
  • Nature, Vol. 451, Issue 7179, p. 652-657
  • DOI: 10.1038/451652a

Current status and challenges for automotive battery production technologies
journal, April 2018


High-voltage positive electrode materials for lithium-ion batteries
journal, January 2017

  • Li, Wangda; Song, Bohang; Manthiram, Arumugam
  • Chemical Society Reviews, Vol. 46, Issue 10
  • DOI: 10.1039/C6CS00875E

Electrode–electrolyte interfaces in lithium-based batteries
journal, January 2018

  • Yu, Xingwen; Manthiram, Arumugam
  • Energy & Environmental Science, Vol. 11, Issue 3
  • DOI: 10.1039/C7EE02555F

Lithium Batteries and Cathode Materials
journal, October 2004

  • Whittingham, M. Stanley
  • Chemical Reviews, Vol. 104, Issue 10, p. 4271-4302
  • DOI: 10.1021/cr020731c

Promises and challenges of nanomaterials for lithium-based rechargeable batteries
journal, June 2016


Rechargeable Lithium–Sulfur Batteries
journal, July 2014

  • Manthiram, Arumugam; Fu, Yongzhu; Chung, Sheng-Heng
  • Chemical Reviews, Vol. 114, Issue 23
  • DOI: 10.1021/cr500062v

Advances in lithium–sulfur batteries based on multifunctional cathodes and electrolytes
journal, September 2016


Electrode–Electrolyte Interfaces in Lithium–Sulfur Batteries with Liquid or Inorganic Solid Electrolytes
journal, October 2017


Bifunctional Separator with a Light-Weight Carbon-Coating for Dynamically and Statically Stable Lithium-Sulfur Batteries
journal, June 2014

  • Chung, Sheng-Heng; Manthiram, Arumugam
  • Advanced Functional Materials, Vol. 24, Issue 33
  • DOI: 10.1002/adfm.201400845

Challenges and Prospects of Lithium–Sulfur Batteries
journal, June 2012

  • Manthiram, Arumugam; Fu, Yongzhu; Su, Yu-Sheng
  • Accounts of Chemical Research, Vol. 46, Issue 5
  • DOI: 10.1021/ar300179v

Lithium-Sulfur Batteries: Progress and Prospects
journal, February 2015

  • Manthiram, Arumugam; Chung, Sheng-Heng; Zu, Chenxi
  • Advanced Materials, Vol. 27, Issue 12
  • DOI: 10.1002/adma.201405115

Highly Reversible Lithium/Dissolved Polysulfide Batteries with Carbon Nanotube Electrodes
journal, May 2013

  • Fu, Yongzhu; Su, Yu-Sheng; Manthiram, Arumugam
  • Angewandte Chemie International Edition, Vol. 52, Issue 27
  • DOI: 10.1002/anie.201301250

Review on High-Loading and High-Energy Lithium-Sulfur Batteries
journal, May 2017

  • Peng, Hong-Jie; Huang, Jia-Qi; Cheng, Xin-Bing
  • Advanced Energy Materials, Vol. 7, Issue 24
  • DOI: 10.1002/aenm.201700260

Revisiting the Role of Polysulfides in Lithium-Sulfur Batteries
journal, March 2018


More Reliable Lithium-Sulfur Batteries: Status, Solutions and Prospects
journal, April 2017

  • Fang, Ruopian; Zhao, Shiyong; Sun, Zhenhua
  • Advanced Materials, Vol. 29, Issue 48
  • DOI: 10.1002/adma.201606823

Hybrid Lithium–Sulfur Batteries with a Solid Electrolyte Membrane and Lithium Polysulfide Catholyte
journal, July 2015

  • Yu, Xingwen; Bi, Zhonghe; Zhao, Feng
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 30
  • DOI: 10.1021/acsami.5b04209

Polysulfide-Shuttle Control in Lithium-Sulfur Batteries with a Chemically/Electrochemically Compatible NaSICON-Type Solid Electrolyte
journal, August 2016

  • Yu, Xingwen; Bi, Zhonghe; Zhao, Feng
  • Advanced Energy Materials, Vol. 6, Issue 24
  • DOI: 10.1002/aenm.201601392

Progress and Perspective of Solid-State Lithium-Sulfur Batteries
journal, March 2018


A review of solid electrolytes for safe lithium-sulfur batteries
journal, November 2017


Moving to a Solid-State Configuration: A Valid Approach to Making Lithium-Sulfur Batteries Viable for Practical Applications
journal, September 2010

  • Hassoun, Jusef; Scrosati, Bruno
  • Advanced Materials, Vol. 22, Issue 45, p. 5198-5201
  • DOI: 10.1002/adma.201002584

All-solid-state Li/S batteries with highly conductive glass–ceramic electrolytes
journal, August 2003

  • Hayashi, Akitoshi; Ohtomo, Takamasa; Mizuno, Fuminori
  • Electrochemistry Communications, Vol. 5, Issue 8, p. 701-705
  • DOI: 10.1016/S1388-2481(03)00167-X

All-solid-state rechargeable lithium batteries with Li2S as a positive electrode material
journal, August 2008


All solid-state battery with sulfur electrode and thio-LISICON electrolyte
journal, August 2008


All-solid-state Li–sulfur batteries with mesoporous electrode and thio-LISICON solid electrolyte
journal, January 2013


Polymer lithium–sulfur batteries with a Nafion membrane and an advanced sulfur electrode
journal, January 2015

  • Yu, Xingwen; Joseph, Jorphin; Manthiram, Arumugam
  • Journal of Materials Chemistry A, Vol. 3, Issue 30
  • DOI: 10.1039/C5TA04289E

Suppression of the polysulfide-shuttle behavior in Li–S batteries through the development of a facile functional group on the polypropylene separator
journal, January 2016

  • Yu, Xingwen; Joseph, Jorphin; Manthiram, Arumugam
  • Materials Horizons, Vol. 3, Issue 4
  • DOI: 10.1039/C6MH00043F

A class of polysulfide catholytes for lithium–sulfur batteries: energy density, cyclability, and voltage enhancement
journal, January 2015

  • Yu, Xingwen; Manthiram, Arumugam
  • Physical Chemistry Chemical Physics, Vol. 17, Issue 3
  • DOI: 10.1039/C4CP04895D

A high performance lithium-ion sulfur battery based on a Li 2 S cathode using a dual-phase electrolyte
journal, January 2015

  • Wang, Lina; Wang, Yonggang; Xia, Yongyao
  • Energy & Environmental Science, Vol. 8, Issue 5
  • DOI: 10.1039/C5EE00058K

A shuttle effect free lithium sulfur battery based on a hybrid electrolyte
journal, January 2014

  • Wang, Qingsong; Jin, Jun; Wu, Xiangwei
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 39
  • DOI: 10.1039/C4CP03694H

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


Review—Solid Electrolytes for Safe and High Energy Density Lithium-Sulfur Batteries: Promises and Challenges
journal, June 2017

  • Judez, Xabier; Zhang, Heng; Li, Chunmei
  • Journal of The Electrochemical Society, Vol. 165, Issue 1
  • DOI: 10.1149/2.0041801jes

Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries
journal, January 2017

  • Kerman, Kian; Luntz, Alan; Viswanathan, Venkatasubramanian
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.1571707jes

Interfacial Chemistry in Solid-State Batteries: Formation of Interphase and Its Consequences
journal, December 2017

  • Wang, Shaofei; Xu, Henghui; Li, Wangda
  • Journal of the American Chemical Society, Vol. 140, Issue 1
  • DOI: 10.1021/jacs.7b09531

Durability of the Li 1+ x Ti 2– x Al x (PO 4 ) 3 Solid Electrolyte in Lithium–Sulfur Batteries
journal, November 2016


Mastering the interface for advanced all-solid-state lithium rechargeable batteries
journal, November 2016

  • Li, Yutao; Zhou, Weidong; Chen, Xi
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 47
  • DOI: 10.1073/pnas.1615912113

Plating a Dendrite-Free Lithium Anode with a Polymer/Ceramic/Polymer Sandwich Electrolyte
journal, July 2016

  • Zhou, Weidong; Wang, Shaofei; Li, Yutao
  • Journal of the American Chemical Society, Vol. 138, Issue 30
  • DOI: 10.1021/jacs.6b05341

Controlling the polysulfide diffusion in lithium-sulfur batteries with a polymer membrane with intrinsic nanoporosity
journal, March 2018


Recent Advancements in Li-Ion Conductors for All-Solid-State Li-Ion Batteries
journal, November 2017


Lithium–sulphur batteries with a microporous carbon paper as a bifunctional interlayer
journal, January 2012

  • Su, Yu-Sheng; Manthiram, Arumugam
  • Nature Communications, Vol. 3, Article No. 1166
  • DOI: 10.1038/ncomms2163

Multi-functional separator/interlayer system for high-stable lithium-sulfur batteries: Progress and prospects
journal, November 2015


Ambient-Temperature Sodium-Sulfur Batteries with a Sodiated Nafion Membrane and a Carbon Nanofiber-Activated Carbon Composite Electrode
journal, April 2015


A reversible nonaqueous room-temperature potassium-sulfur chemistry for electrochemical energy storage
journal, November 2018


Understanding the Redox Obstacles in High Sulfur-Loading Li–S Batteries and Design of an Advanced Gel Cathode
journal, March 2016


Breaking Down the Crystallinity: The Path for Advanced Lithium Batteries
journal, December 2015

  • Zu, Chenxi; Dolocan, Andrei; Xiao, Penghao
  • Advanced Energy Materials, Vol. 6, Issue 5
  • DOI: 10.1002/aenm.201501933

In Operando X-ray Diffraction and Transmission X-ray Microscopy of Lithium Sulfur Batteries
journal, March 2012

  • Nelson, Johanna; Misra, Sumohan; Yang, Yuan
  • Journal of the American Chemical Society, Vol. 134, Issue 14
  • DOI: 10.1021/ja2121926

Burning lithium in CS2 for high-performing compact Li2S–graphene nanocapsules for Li–S batteries
journal, June 2017


Highly Reversible Lithium/Dissolved Polysulfide Batteries with Carbon Nanotube Electrodes
journal, May 2013

  • Fu, Yongzhu; Su, Yu-Sheng; Manthiram, Arumugam
  • Angewandte Chemie, Vol. 125, Issue 27, p. 7068-7073
  • DOI: 10.1002/ange.201301250

Lithium Batteries and Cathode Materials
journal, December 2004


Review : Solid Electrolytes for Safe and High Energy Density Lithium-Sulfur Batteries : Promises and Challenges
text, January 2018


Works referencing / citing this record:

Lab‐Scale In Situ X‐Ray Diffraction Technique for Different Battery Systems: Designs, Applications, and Perspectives
journal, May 2019


Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition
journal, October 2019


Lithiophilic montmorillonite serves as lithium ion reservoir to facilitate uniform lithium deposition
journal, October 2019