skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes

Abstract

Polymer binders in battery electrodes may be either active or passive. This distinction depends on whether the polymer influences charge or mass transport in the electrode. Though it is desirable to understand how to tailor the macromolecular design of a polymer to play a passive or active role, design rules are still lacking, as is a framework to assess the divergence in such behaviors. We reveal the molecular-level underpinnings that distinguish an active polyelectrolyte binder designed for lithium-sulfur batteries from a passive alternative. The binder, a cationic polyelectrolyte, is shown to both facilitate lithium-ion transport through its reconfigurable network of mobile anions and restrict polysulfide diffusion from mesoporous carbon hosts by anion metathesis, which we show is selective for higher oligomers. These attributes then allow cells to be operated for > 100 cycles with excellent rate capability using cathodes with areal sulfur loadings up to 8.1 mg cm -2 .

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3];  [4];  [5];  [1];  [4]; ORCiD logo [6]; ORCiD logo [6]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Joint Center for Energy Storage Research
  4. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Materials Science and Engineering
  5. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  6. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Joint Center for Energy Storage Research, Molecular Foundry
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
SC-22.2 USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1417620
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 25 ENERGY STORAGE; batteries; polymer characterization

Citation Formats

Li, Longjun, Pascal, Tod A., Connell, Justin G., Fan, Frank Y., Meckler, Stephen M., Ma, Lin, Chiang, Yet-Ming, Prendergast, David, and Helms, Brett A. Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes. United States: N. p., 2017. Web. doi:10.1038/s41467-017-02410-6.
Li, Longjun, Pascal, Tod A., Connell, Justin G., Fan, Frank Y., Meckler, Stephen M., Ma, Lin, Chiang, Yet-Ming, Prendergast, David, & Helms, Brett A. Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes. United States. doi:10.1038/s41467-017-02410-6.
Li, Longjun, Pascal, Tod A., Connell, Justin G., Fan, Frank Y., Meckler, Stephen M., Ma, Lin, Chiang, Yet-Ming, Prendergast, David, and Helms, Brett A. Fri . "Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes". United States. doi:10.1038/s41467-017-02410-6. https://www.osti.gov/servlets/purl/1417620.
@article{osti_1417620,
title = {Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes},
author = {Li, Longjun and Pascal, Tod A. and Connell, Justin G. and Fan, Frank Y. and Meckler, Stephen M. and Ma, Lin and Chiang, Yet-Ming and Prendergast, David and Helms, Brett A.},
abstractNote = {Polymer binders in battery electrodes may be either active or passive. This distinction depends on whether the polymer influences charge or mass transport in the electrode. Though it is desirable to understand how to tailor the macromolecular design of a polymer to play a passive or active role, design rules are still lacking, as is a framework to assess the divergence in such behaviors. We reveal the molecular-level underpinnings that distinguish an active polyelectrolyte binder designed for lithium-sulfur batteries from a passive alternative. The binder, a cationic polyelectrolyte, is shown to both facilitate lithium-ion transport through its reconfigurable network of mobile anions and restrict polysulfide diffusion from mesoporous carbon hosts by anion metathesis, which we show is selective for higher oligomers. These attributes then allow cells to be operated for > 100 cycles with excellent rate capability using cathodes with areal sulfur loadings up to 8.1 mg cm -2 .},
doi = {10.1038/s41467-017-02410-6},
journal = {Nature Communications},
number = 1,
volume = 8,
place = {United States},
year = {Fri Dec 22 00:00:00 EST 2017},
month = {Fri Dec 22 00:00:00 EST 2017}
}

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

Citation Metrics:
Cited by: 4 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Structural Factors of Sulfur Cathodes with Poly(ethylene oxide) Binder for Performance of Rechargeable Lithium Sulfur Batteries
journal, January 2002

  • Cheon, Sang-Eun; Cho, Ji-Hoon; Ko, Ki-Seok
  • Journal of The Electrochemical Society, Vol. 149, Issue 11, p. A1437-A1441
  • DOI: 10.1149/1.1511187

Application of gelatin as a binder for the sulfur cathode in lithium–sulfur batteries
journal, October 2008


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

A highly ordered nanostructured carbon–sulphur cathode for lithium–sulphur batteries
journal, May 2009

  • Ji, Xiulei; Lee, Kyu Tae; Nazar, Linda F.
  • Nature Materials, Vol. 8, Issue 6, p. 500-506
  • DOI: 10.1038/nmat2460

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