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

Title: Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors

Abstract

Abstract The emergence of wearable electronics puts batteries closer to the human skin, exacerbating the need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy to overcome the canonical tradeoff between mechanical robustness and ionic conductivity in polymer electrolytes. The supramolecular lithium ion conductor utilizes orthogonally functional H-bonding domains and ion-conducting domains to create a polymer electrolyte with unprecedented toughness (29.3 MJ m −3 ) and high ionic conductivity (1.2 × 10 −4 S cm −1 at 25 °C). Implementation of the supramolecular ion conductor as a binder material allows for the creation of stretchable lithium-ion battery electrodes with strain capability of over 900% via a conventional slurry process. The supramolecular nature of these battery components enables intimate bonding at the electrode-electrolyte interface. Combination of these stretchable components leads to a stretchable battery with a capacity of 1.1 mAh cm −2 that functions even when stretched to 70% strain. The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications.

Authors:
ORCiD logo; ORCiD logo; ORCiD logo; ; ORCiD logo; ; ; ; ; ; ORCiD logo; ORCiD logo; ORCiD logo
Publication Date:
Research Org.:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); Japan Society for the Promotion of Science (JSPS); USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Biological and Environmental Research (BER); National Institutes of Health (NIH)
OSTI Identifier:
1619593
Alternate Identifier(s):
OSTI ID: 1595360
Grant/Contract Number:  
Battery 500; AC02-76SF00515; 21901161; ECCS‐1542152; DGE‐114747; P41GM103393
Resource Type:
Published Article
Journal Name:
Nature Communications
Additional Journal Information:
Journal Name: Nature Communications Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United Kingdom
Language:
English
Subject:
25 ENERGY STORAGE; Batteries; Mechanical properties; Polymer characterization; Supramolecular polymers

Citation Formats

Mackanic, David G., Yan, Xuzhou, Zhang, Qiuhong, Matsuhisa, Naoji, Yu, Zhiao, Jiang, Yuanwen, Manika, Tuheen, Lopez, Jeffrey, Yan, Hongping, Liu, Kai, Chen, Xiaodong, Cui, Yi, and Bao, Zhenan. Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors. United Kingdom: N. p., 2019. Web. doi:10.1038/s41467-019-13362-4.
Mackanic, David G., Yan, Xuzhou, Zhang, Qiuhong, Matsuhisa, Naoji, Yu, Zhiao, Jiang, Yuanwen, Manika, Tuheen, Lopez, Jeffrey, Yan, Hongping, Liu, Kai, Chen, Xiaodong, Cui, Yi, & Bao, Zhenan. Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors. United Kingdom. https://doi.org/10.1038/s41467-019-13362-4
Mackanic, David G., Yan, Xuzhou, Zhang, Qiuhong, Matsuhisa, Naoji, Yu, Zhiao, Jiang, Yuanwen, Manika, Tuheen, Lopez, Jeffrey, Yan, Hongping, Liu, Kai, Chen, Xiaodong, Cui, Yi, and Bao, Zhenan. Tue . "Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors". United Kingdom. https://doi.org/10.1038/s41467-019-13362-4.
@article{osti_1619593,
title = {Decoupling of mechanical properties and ionic conductivity in supramolecular lithium ion conductors},
author = {Mackanic, David G. and Yan, Xuzhou and Zhang, Qiuhong and Matsuhisa, Naoji and Yu, Zhiao and Jiang, Yuanwen and Manika, Tuheen and Lopez, Jeffrey and Yan, Hongping and Liu, Kai and Chen, Xiaodong and Cui, Yi and Bao, Zhenan},
abstractNote = {Abstract The emergence of wearable electronics puts batteries closer to the human skin, exacerbating the need for battery materials that are robust, highly ionically conductive, and stretchable. Herein, we introduce a supramolecular design as an effective strategy to overcome the canonical tradeoff between mechanical robustness and ionic conductivity in polymer electrolytes. The supramolecular lithium ion conductor utilizes orthogonally functional H-bonding domains and ion-conducting domains to create a polymer electrolyte with unprecedented toughness (29.3 MJ m −3 ) and high ionic conductivity (1.2 × 10 −4 S cm −1 at 25 °C). Implementation of the supramolecular ion conductor as a binder material allows for the creation of stretchable lithium-ion battery electrodes with strain capability of over 900% via a conventional slurry process. The supramolecular nature of these battery components enables intimate bonding at the electrode-electrolyte interface. Combination of these stretchable components leads to a stretchable battery with a capacity of 1.1 mAh cm −2 that functions even when stretched to 70% strain. The method reported here of decoupling ionic conductivity from mechanical properties opens a promising route to create high-toughness ion transport materials for energy storage applications.},
doi = {10.1038/s41467-019-13362-4},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United Kingdom},
year = {Tue Nov 26 00:00:00 EST 2019},
month = {Tue Nov 26 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1038/s41467-019-13362-4

Citation Metrics:
Cited by: 162 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Effect of Molecular Weight on the Mechanical and Electrical Properties of Block Copolymer Electrolytes
journal, June 2007

  • Singh, Mohit; Odusanya, Omolola; Wilmes, Gregg M.
  • Macromolecules, Vol. 40, Issue 13
  • DOI: 10.1021/ma0629541

Double-slit photoelectron interference in strong-field ionization of the neon dimer
journal, January 2019


Reversible Polymers Formed from Self-Complementary Monomers Using Quadruple Hydrogen Bonding
journal, November 1997


Super-stretchy lithium-ion battery based on carbon nanotube fiber
journal, January 2014

  • Zhang, Ye; Bai, Wenyu; Ren, Jing
  • Journal of Materials Chemistry A, Vol. 2, Issue 29
  • DOI: 10.1039/c4ta01878h

Flexible and Stretchable Lithium-Ion Batteries and Supercapacitors Based on Electrically Conducting Carbon Nanotube Fiber Springs
journal, October 2014

  • Zhang, Ye; Bai, Wenyu; Cheng, Xunliang
  • Angewandte Chemie International Edition, Vol. 53, Issue 52
  • DOI: 10.1002/anie.201409366

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

  • Kimura, Kento; Motomatsu, Joh; Tominaga, Yoichi
  • The Journal of Physical Chemistry C, Vol. 120, Issue 23
  • DOI: 10.1021/acs.jpcc.6b03277

A flexible, self-healing and highly stretchable polymer electrolyte via quadruple hydrogen bonding for lithium-ion batteries
journal, January 2018

  • Zhou, Binghua; He, Dan; Hu, Ji
  • Journal of Materials Chemistry A, Vol. 6, Issue 25
  • DOI: 10.1039/C8TA01907J

Self‐Healing Polymer Electrolytes Formed via Dual‐Networks: A New Strategy for Flexible Lithium Metal Batteries
journal, November 2018

  • Zhou, Binghua; Zuo, Cai; Xiao, Zhuliu
  • Chemistry – A European Journal, Vol. 24, Issue 72
  • DOI: 10.1002/chem.201803943

Supramolecular Polymer Materials: Chain Extension of Telechelic Polymers Using a Reactive Hydrogen-Bonding Synthon
journal, June 2000


A Stretchable Graphitic Carbon/Si Anode Enabled by Conformal Coating of a Self-Healing Elastic Polymer
journal, January 2016

  • Sun, Yongming; Lopez, Jeffrey; Lee, Hyun-Wook
  • Advanced Materials, Vol. 28, Issue 12
  • DOI: 10.1002/adma.201504723

Microscopic investigation of ionic conductivity in alkali metal salts-poly(ethylene oxide) adducts
journal, September 1983


3D Porous Sponge-Inspired Electrode for Stretchable Lithium-Ion Batteries
journal, March 2016


Optimizing Areal Capacities through Understanding the Limitations of Lithium-Ion Electrodes
journal, November 2015

  • Gallagher, Kevin G.; Trask, Stephen E.; Bauer, Christoph
  • Journal of The Electrochemical Society, Vol. 163, Issue 2
  • DOI: 10.1149/2.0321602jes

An All-Solid-State Fiber-Shaped Aluminum-Air Battery with Flexibility, Stretchability, and High Electrochemical Performance
journal, May 2016

  • Xu, Yifan; Zhao, Yang; Ren, Jing
  • Angewandte Chemie International Edition, Vol. 55, Issue 28
  • DOI: 10.1002/anie.201601804

Designing polymers for advanced battery chemistries
journal, April 2019


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


Synthesis of N -Phenylaminomethyl POSS and Its Utilization in Polyurethane
journal, February 2011

  • Zhang, Qiuhong; He, Hui; Xi, Kai
  • Macromolecules, Vol. 44, Issue 3
  • DOI: 10.1021/ma101825j

Polymer Electrolytes
journal, July 2013


Polymer electrolytes for lithium polymer batteries
journal, January 2016

  • Long, Lizhen; Wang, Shuanjin; Xiao, Min
  • Journal of Materials Chemistry A, Vol. 4, Issue 26
  • DOI: 10.1039/C6TA02621D

Extended cyclic uniaxial loading of stretchable gold thin-films on elastomeric substrates
journal, February 2009

  • Graz, Ingrid M.; Cotton, Darryl P. J.; Lacour, Stéphanie P.
  • Applied Physics Letters, Vol. 94, Issue 7
  • DOI: 10.1063/1.3076103

High-Modulus, High-Conductivity Nanostructured Polymer Electrolyte Membranes via Polymerization-Induced Phase Separation
journal, December 2013

  • Schulze, Morgan W.; McIntosh, Lucas D.; Hillmyer, Marc A.
  • Nano Letters, Vol. 14, Issue 1
  • DOI: 10.1021/nl4034818

A Gum-Like Lithium-Ion Battery Based on a Novel Arched Structure
journal, January 2015


Opportunities and challenges for a sustainable energy future
journal, August 2012

  • Chu, Steven; Majumdar, Arun
  • Nature, Vol. 488, Issue 7411, p. 294-303
  • DOI: 10.1038/nature11475

The Temperature Dependence of Relaxation Mechanisms in Amorphous Polymers and Other Glass-forming Liquids
journal, July 1955

  • Williams, Malcolm L.; Landel, Robert F.; Ferry, John D.
  • Journal of the American Chemical Society, Vol. 77, Issue 14
  • DOI: 10.1021/ja01619a008

Decoupling Bulk Mechanics and Mono- and Multivalent Ion Transport in Polymers Based on Metal–Ligand Coordination
journal, July 2018


Highly conductive solvent-free polymer electrolyte membrane for lithium-ion batteries: Effect of prepolymer molecular weight
journal, January 2016


Elastic and Wearable Wire-Shaped Lithium-Ion Battery with High Electrochemical Performance
journal, June 2014

  • Ren, Jing; Zhang, Ye; Bai, Wenyu
  • Angewandte Chemie International Edition, Vol. 53, Issue 30
  • DOI: 10.1002/anie.201402388

A stretchable and biodegradable strain and pressure sensor for orthopaedic application
journal, May 2018

  • Boutry, Clementine M.; Kaizawa, Yukitoshi; Schroeder, Bob C.
  • Nature Electronics, Vol. 1, Issue 5
  • DOI: 10.1038/s41928-018-0071-7

Poly(allylamine). Chelating properties and resins for uranium recovery from seawater
journal, December 1985

  • Kobayashi, Shiro; Tokunoh, Masazumi; Saegusa, Takeo
  • Macromolecules, Vol. 18, Issue 12
  • DOI: 10.1021/ma00154a004

Highly Conductive and Thermally Stable Ion Gels with Tunable Anisotropy and Modulus
journal, January 2016


Effect of Anions on Lithium Ion Conduction in Poly(ethylene carbonate)-based Polymer Electrolytes
journal, January 2015

  • Tominaga, Yoichi; Yamazaki, Kenta; Nanthana, Vannasa
  • Journal of The Electrochemical Society, Vol. 162, Issue 2
  • DOI: 10.1149/2.0211502jes

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


Structure–Conductivity Relationship for Peptoid-Based PEO–Mimetic Polymer Electrolytes
journal, June 2012

  • Sun, Jing; Stone, Gregory M.; Balsara, Nitash P.
  • Macromolecules, Vol. 45, Issue 12
  • DOI: 10.1021/ma300775b

Syringe-injectable electronics
journal, June 2015

  • Liu, Jia; Fu, Tian-Ming; Cheng, Zengguang
  • Nature Nanotechnology, Vol. 10, Issue 7
  • DOI: 10.1038/nnano.2015.115

Bring on the bodyNET
journal, September 2017

  • Chu, Bryant; Burnett, William; Chung, Jong Won
  • Nature, Vol. 549, Issue 7672
  • DOI: 10.1038/549328a

Stretching-induced interconnect delamination in stretchable electronic circuits
journal, December 2010


Toughening stretchable fibers via serial fracturing of a metallic core
journal, February 2019

  • Cooper, Christopher B.; Joshipura, Ishan D.; Parekh, Dishit P.
  • Science Advances, Vol. 5, Issue 2
  • DOI: 10.1126/sciadv.aat4600

Epidermal Electronics
journal, August 2011


A solid future for battery development
journal, September 2016


Flexible and stretchable power sources for wearable electronics
journal, June 2017

  • Zamarayeva, Alla M.; Ostfeld, Aminy E.; Wang, Michael
  • Science Advances, Vol. 3, Issue 6
  • DOI: 10.1126/sciadv.1602051

Nanocomposite polymer electrolytes for lithium batteries
journal, July 1998

  • Croce, F.; Appetecchi, G. B.; Persi, L.
  • Nature, Vol. 394, Issue 6692
  • DOI: 10.1038/28818

Stretchable gold conductors on elastomeric substrates
journal, April 2003

  • Lacour, Stephanie Perichon; Wagner, Sigurd; Huang, Zhenyu
  • Applied Physics Letters, Vol. 82, Issue 15, p. 2404-2406
  • DOI: 10.1063/1.1565683

All-Printed, Stretchable Zn-Ag 2 O Rechargeable Battery via Hyperelastic Binder for Self-Powering Wearable Electronics
journal, December 2016


Flexible and Stretchable Energy Storage: Recent Advances and Future Perspectives
journal, November 2016


Effect of monomer structure on ionic conductivity in a systematic set of polyester electrolytes
journal, June 2016


Polymer electrolytes—Some principles, cautions, and new practices
journal, October 2017


Fully Integrated Design of a Stretchable Solid‐State Lithium‐Ion Full Battery
journal, September 2019


Towards greener and more sustainable batteries for electrical energy storage
journal, November 2014


Dynamic supramolecular poly(isobutylene)s for self-healing materials
journal, January 2012

  • Herbst, Florian; Seiffert, Sebastian; Binder, Wolfgang H.
  • Polymer Chemistry, Vol. 3, Issue 11
  • DOI: 10.1039/c2py20265d

High-performance stretchable electrodes prepared from elastomeric current collectors and binders
journal, January 2017

  • Zhou, Ao; Sim, Richard; Luo, Yingwu
  • J. Mater. Chem. A, Vol. 5, Issue 40
  • DOI: 10.1039/C7TA07185J

An All-Stretchable-Component Sodium-Ion Full Battery
journal, April 2017


Quadruple H-Bonding Cross-Linked Supramolecular Polymeric Materials as Substrates for Stretchable, Antitearing, and Self-Healable Thin Film Electrodes
journal, March 2018

  • Yan, Xuzhou; Liu, Zhiyuan; Zhang, Qiuhong
  • Journal of the American Chemical Society, Vol. 140, Issue 15
  • DOI: 10.1021/jacs.8b01682

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


Towards Dynamic but Supertough Healable Polymers through Biomimetic Hierarchical Hydrogen-Bonding Interactions
journal, September 2018

  • Song, Yan; Liu, Yuan; Qi, Tao
  • Angewandte Chemie International Edition, Vol. 57, Issue 42
  • DOI: 10.1002/anie.201807622

Tough adhesives for diverse wet surfaces
journal, July 2017


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

  • Choudhury, Snehashis; Mangal, Rahul; Agrawal, Akanksha
  • Nature Communications, Vol. 6, Issue 1
  • DOI: 10.1038/ncomms10101

Stretchable batteries with self-similar serpentine interconnects and integrated wireless recharging systems
journal, February 2013

  • Xu, Sheng; Zhang, Yihui; Cho, Jiung
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms2553

Dip-coating processed sponge-based electrodes for stretchable Zn-MnO2 batteries
journal, February 2018


Supramolecular Regulation of Anions Enhances Conductivity and Transference Number of Lithium in Liquid Electrolytes
journal, July 2018

  • Qiao, Bo; Leverick, Graham M.; Zhao, Wei
  • Journal of the American Chemical Society, Vol. 140, Issue 35
  • DOI: 10.1021/jacs.8b05915

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


Design, Synthesis, and X-ray Crystal Structure of a Potent Dual Inhibitor of Thymidylate Synthase and Dihydrofolate Reductase as an Antitumor Agent 1
journal, October 2000

  • Gangjee, Aleem; Yu, Jianming; McGuire, John J.
  • Journal of Medicinal Chemistry, Vol. 43, Issue 21
  • DOI: 10.1021/jm000200l