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Title: High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)

Abstract

Flexible and low-cost poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state Li-metal batteries because of their compatibility with a metallic lithium anode. However, the low room-temperature Li-ion conductivity of PEO solid electrolytes and severe lithium-dendrite growth limit their application in high-energy Li-metal batteries. Here we prepared a PEO/perovskite Li 3/8 Sr 7/16 Ta 3/4 Zr 1/4 O 3 composite electrolyte with a Li-ion conductivity of 5.4 × 10 −5 and 3.5 × 10 −4 S cm −1 at 25 and 45 °C, respectively; the strong interaction between the F of TFSI (bis-trifluoromethanesulfonimide) and the surface Ta 5+ of the perovskite improves the Li-ion transport at the PEO/perovskite interface. A symmetric Li/composite electrolyte/Li cell shows an excellent cyclability at a high current density up to 0.6 mA cm −2 . A solid electrolyte interphase layer formed in situ between the metallic lithium anode and the composite electrolyte suppresses lithium-dendrite formation and growth. All-solid-state Li|LiFePO 4 and high-voltage Li|LiNi 0.8 Mn 0.1 Co 0.1 O 2 batteries with the composite electrolyte have an impressive performance with high Coulombic efficiencies, small overpotentials, and good cycling stability.

Authors:
ORCiD logo; ; ; ; ; ORCiD logo; ; ORCiD logo
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); Welch Foundation
OSTI Identifier:
1559398
Alternate Identifier(s):
OSTI ID: 1614047
Grant/Contract Number:  
EE000762; UTA17-001111; EE0007762; F-1959-20180324; DMR-1808517; DMR-1644779
Resource Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 38; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; polymer electrolyte; high conductivity; solid-state batteries; high-voltage cathode

Citation Formats

Xu, Henghui, Chien, Po-Hsiu, Shi, Jianjian, Li, Yutao, Wu, Nan, Liu, Yuanyue, Hu, Yan-Yan, and Goodenough, John B. High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide). United States: N. p., 2019. Web. https://doi.org/10.1073/pnas.1907507116.
Xu, Henghui, Chien, Po-Hsiu, Shi, Jianjian, Li, Yutao, Wu, Nan, Liu, Yuanyue, Hu, Yan-Yan, & Goodenough, John B. High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide). United States. https://doi.org/10.1073/pnas.1907507116
Xu, Henghui, Chien, Po-Hsiu, Shi, Jianjian, Li, Yutao, Wu, Nan, Liu, Yuanyue, Hu, Yan-Yan, and Goodenough, John B. Thu . "High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)". United States. https://doi.org/10.1073/pnas.1907507116.
@article{osti_1559398,
title = {High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide)},
author = {Xu, Henghui and Chien, Po-Hsiu and Shi, Jianjian and Li, Yutao and Wu, Nan and Liu, Yuanyue and Hu, Yan-Yan and Goodenough, John B.},
abstractNote = {Flexible and low-cost poly(ethylene oxide) (PEO)-based electrolytes are promising for all-solid-state Li-metal batteries because of their compatibility with a metallic lithium anode. However, the low room-temperature Li-ion conductivity of PEO solid electrolytes and severe lithium-dendrite growth limit their application in high-energy Li-metal batteries. Here we prepared a PEO/perovskite Li 3/8 Sr 7/16 Ta 3/4 Zr 1/4 O 3 composite electrolyte with a Li-ion conductivity of 5.4 × 10 −5 and 3.5 × 10 −4 S cm −1 at 25 and 45 °C, respectively; the strong interaction between the F − of TFSI − (bis-trifluoromethanesulfonimide) and the surface Ta 5+ of the perovskite improves the Li-ion transport at the PEO/perovskite interface. A symmetric Li/composite electrolyte/Li cell shows an excellent cyclability at a high current density up to 0.6 mA cm −2 . A solid electrolyte interphase layer formed in situ between the metallic lithium anode and the composite electrolyte suppresses lithium-dendrite formation and growth. All-solid-state Li|LiFePO 4 and high-voltage Li|LiNi 0.8 Mn 0.1 Co 0.1 O 2 batteries with the composite electrolyte have an impressive performance with high Coulombic efficiencies, small overpotentials, and good cycling stability.},
doi = {10.1073/pnas.1907507116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 38,
volume = 116,
place = {United States},
year = {2019},
month = {8}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1073/pnas.1907507116

Citation Metrics:
Cited by: 23 works
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Works referenced in this record:

Flexible, Scalable, and Highly Conductive Garnet-Polymer Solid Electrolyte Templated by Bacterial Cellulose
journal, March 2018

  • Xie, Hua; Yang, Chunpeng; Fu, Kun Kelvin
  • Advanced Energy Materials, Vol. 8, Issue 18
  • DOI: 10.1002/aenm.201703474

PVDF/Palygorskite Nanowire Composite Electrolyte for 4 V Rechargeable Lithium Batteries with High Energy Density
journal, August 2018


Lithium Ion Conducting Poly(ethylene oxide)-Based Solid Electrolytes Containing Active or Passive Ceramic Nanoparticles
journal, January 2017

  • Wang, Weimin; Yi, Eongyu; Fici, Anthony J.
  • The Journal of Physical Chemistry C, Vol. 121, Issue 5
  • DOI: 10.1021/acs.jpcc.6b11136

Challenges for Rechargeable Li Batteries
journal, February 2010

  • Goodenough, John B.; Kim, Youngsik
  • Chemistry of Materials, Vol. 22, Issue 3, p. 587-603
  • DOI: 10.1021/cm901452z

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

  • Zheng, Jin; Tang, Mingxue; Hu, Yan-Yan
  • Angewandte Chemie International Edition, Vol. 55, Issue 40
  • DOI: 10.1002/anie.201607539

Li 3 N-Modified Garnet Electrolyte for All-Solid-State Lithium Metal Batteries Operated at 40 °C
journal, October 2018


Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016

  • Li, Yutao; Xu, Biyi; Xu, Henghui
  • Angewandte Chemie International Edition, Vol. 56, Issue 3
  • DOI: 10.1002/anie.201608924

Fluorinated solid electrolyte interphase enables highly reversible solid-state Li metal battery
journal, December 2018


Enhancing ionic conductivity in composite polymer electrolytes with well-aligned ceramic nanowires
journal, April 2017


Biocompatible and biodegradable solid polymer electrolytes for high voltage and high temperature lithium batteries
journal, January 2017


New Insights into the Compositional Dependence of Li-Ion Transport in Polymer–Ceramic Composite Electrolytes
journal, January 2018


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

  • Xue, Zhigang; He, Dan; Xie, Xiaolin
  • Journal of Materials Chemistry A, Vol. 3, Issue 38
  • DOI: 10.1039/C5TA03471J

A Silica-Aerogel-Reinforced Composite Polymer Electrolyte with High Ionic Conductivity and High Modulus
journal, June 2018

  • Lin, Dingchang; Yuen, Pak Yan; Liu, Yayuan
  • Advanced Materials, Vol. 30, Issue 32
  • DOI: 10.1002/adma.201802661

A Flexible Solid Electrolyte Interphase Layer for Long-Life Lithium Metal Anodes
journal, January 2018

  • Li, Nian-Wu; Shi, Yang; Yin, Ya-Xia
  • Angewandte Chemie International Edition, Vol. 57, Issue 6
  • DOI: 10.1002/anie.201710806

At the polymer electrolyte interfaces: the role of the polymer host in interphase layer formation in Li-batteries
journal, January 2015

  • Sun, Bing; Xu, Chao; Mindemark, Jonas
  • Journal of Materials Chemistry A, Vol. 3, Issue 26
  • DOI: 10.1039/C5TA02485D

Flexible Composite Solid Electrolyte Facilitating Highly Stable “Soft Contacting” Li-Electrolyte Interface for Solid State Lithium-Ion Batteries
journal, September 2017

  • Yang, Luyi; Wang, Zijian; Feng, Yancong
  • Advanced Energy Materials, Vol. 7, Issue 22
  • DOI: 10.1002/aenm.201701437

A multifunctional polymer electrolyte enables ultra-long cycle-life in a high-voltage lithium metal battery
journal, January 2018

  • Dong, Tiantian; Zhang, Jianjun; Xu, Gaojie
  • Energy & Environmental Science, Vol. 11, Issue 5
  • DOI: 10.1039/C7EE03365F

Solid polymer electrolytes incorporating cubic Li7La3Zr2O12 for all-solid-state lithium rechargeable batteries
journal, December 2017


Ionic Conductivity Enhancement of Polymer Electrolytes with Ceramic Nanowire Fillers
journal, March 2015


Hybrid Lithium-Sulfur Batteries with an Advanced Gel Cathode and Stabilized Lithium-Metal Anode
journal, May 2018

  • Xu, Henghui; Wang, Shaofei; Manthiram, Arumugam
  • Advanced Energy Materials, Vol. 8, Issue 23
  • DOI: 10.1002/aenm.201800813

Mechanism of Ion Transport in Amorphous Poly(ethylene oxide)/LiTFSI from Molecular Dynamics Simulations
journal, February 2006

  • Borodin, Oleg; Smith, Grant D.
  • Macromolecules, Vol. 39, Issue 4
  • DOI: 10.1021/ma052277v

Ultrahigh Performance All Solid-State Lithium Sulfur Batteries: Salt Anion’s Chemistry-Induced Anomalous Synergistic Effect
journal, July 2018

  • Eshetu, Gebrekidan Gebresilassie; Judez, Xabier; Li, Chunmei
  • Journal of the American Chemical Society, Vol. 140, Issue 31
  • DOI: 10.1021/jacs.8b04612

Flexible, solid-state, ion-conducting membrane with 3D garnet nanofiber networks for lithium batteries
journal, June 2016

  • Fu, Kun (Kelvin); Gong, Yunhui; Dai, Jiaqi
  • Proceedings of the National Academy of Sciences, Vol. 113, Issue 26
  • DOI: 10.1073/pnas.1600422113

Stabilizing Li 10 SnP 2 S 12 /Li Interface via an in Situ Formed Solid Electrolyte Interphase Layer
journal, July 2018

  • Zheng, Bizhu; Zhu, Jianping; Wang, Hongchun
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 30
  • DOI: 10.1021/acsami.8b08860

Perovskite Membranes with Vertically Aligned Microchannels for All-Solid-State Lithium Batteries
journal, August 2018

  • Jiang, Zhouyang; Xie, Huiqi; Wang, Suqing
  • Advanced Energy Materials, Vol. 8, Issue 27
  • DOI: 10.1002/aenm.201801433

Interface layer formation in solid polymer electrolyte lithium batteries: an XPS study
journal, January 2014

  • Xu, Chao; Sun, Bing; Gustafsson, Torbjörn
  • J. Mater. Chem. A, Vol. 2, Issue 20
  • DOI: 10.1039/C4TA00214H

Ionic conductivity of composite electrolytes based on oligo(ethylene oxide) and fumed oxides
journal, January 2004


An advanced construction strategy of all-solid-state lithium batteries with excellent interfacial compatibility and ultralong cycle life
journal, January 2017

  • Zhang, Zhihua; Zhao, Yanran; Chen, Shaojie
  • Journal of Materials Chemistry A, Vol. 5, Issue 32
  • DOI: 10.1039/C7TA04320A

Oxygen Release and Its Effect on the Cycling Stability of LiNi x Mn y Co z O 2 (NMC) Cathode Materials for Li-Ion Batteries
journal, January 2017

  • Jung, Roland; Metzger, Michael; Maglia, Filippo
  • Journal of The Electrochemical Society, Vol. 164, Issue 7
  • DOI: 10.1149/2.0021707jes

A Perovskite Electrolyte That Is Stable in Moist Air for Lithium-Ion Batteries
journal, June 2018

  • Li, Yutao; Xu, Henghui; Chien, Po-Hsiu
  • Angewandte Chemie International Edition, Vol. 57, Issue 28
  • DOI: 10.1002/anie.201804114

An anion-immobilized composite electrolyte for dendrite-free lithium metal anodes
journal, October 2017

  • Zhao, Chen-Zi; Zhang, Xue-Qiang; Cheng, Xin-Bing
  • Proceedings of the National Academy of Sciences, Vol. 114, Issue 42
  • DOI: 10.1073/pnas.1708489114

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


Hybrid Polymer/Garnet Electrolyte with a Small Interfacial Resistance for Lithium-Ion Batteries
journal, December 2016


    Works referencing / citing this record:

    Enhanced Surface Interactions Enable Fast Li + Conduction in Oxide/Polymer Composite Electrolyte
    journal, January 2020


    High cathode utilization efficiency through interface engineering in all-solid-state lithium-metal batteries
    journal, January 2019

    • Guo, Xianwei; Hao, Liangwei; Yang, Yubo
    • Journal of Materials Chemistry A, Vol. 7, Issue 45
    • DOI: 10.1039/c9ta09935b