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

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. Although it is desirable to understand how to tailor the macromolecular design of a polymer to play a passive or active role, d...

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Main Authors: Li, Longjun, Pascal, Tod A., Connell, Justin G., Meckler, Stephen M., Ma, Lin, Prendergast, David, Helms, Brett A., Fan, Frank Yongzhen, Chiang, Yet-Ming
Other Authors: Massachusetts Institute of Technology. Department of Materials Science and Engineering
Format: Article
Published: Springer Nature 2018
Online Access:http://hdl.handle.net/1721.1/118596
https://orcid.org/0000-0003-4244-0365
https://orcid.org/0000-0002-0833-7674
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author Li, Longjun
Pascal, Tod A.
Connell, Justin G.
Meckler, Stephen M.
Ma, Lin
Prendergast, David
Helms, Brett A.
Fan, Frank Yongzhen
Chiang, Yet-Ming
author2 Massachusetts Institute of Technology. Department of Materials Science and Engineering
author_facet Massachusetts Institute of Technology. Department of Materials Science and Engineering
Li, Longjun
Pascal, Tod A.
Connell, Justin G.
Meckler, Stephen M.
Ma, Lin
Prendergast, David
Helms, Brett A.
Fan, Frank Yongzhen
Chiang, Yet-Ming
author_sort Li, Longjun
collection MIT
description 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. Although 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. Here, 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 allow cells to be operated for >100 cycles with excellent rate capability using cathodes with areal sulfur loadings up to 8.1 mg cm[superscript -2].
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spelling mit-1721.1/1185962024-07-11T19:48:57Z Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes Li, Longjun Pascal, Tod A. Connell, Justin G. Meckler, Stephen M. Ma, Lin Prendergast, David Helms, Brett A. Fan, Frank Yongzhen Chiang, Yet-Ming Massachusetts Institute of Technology. Department of Materials Science and Engineering Fan, Frank Yongzhen Chiang, Yet-Ming 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. Although 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. Here, 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 allow cells to be operated for >100 cycles with excellent rate capability using cathodes with areal sulfur loadings up to 8.1 mg cm[superscript -2]. United States. Department of Energy. Office of Basic Energy Sciences (Joint Center for Energy Storage Research) 2018-10-18T13:13:06Z 2018-10-18T13:13:06Z 2017-12 2018-10-10T14:04:32Z Article http://purl.org/eprint/type/JournalArticle 2041-1723 http://hdl.handle.net/1721.1/118596 Li, Longjun, et al. “Molecular Understanding of Polyelectrolyte Binders That Actively Regulate Ion Transport in Sulfur Cathodes.” Nature Communications, vol. 8, no. 1, Dec. 2017. © 2017 The Authors https://orcid.org/0000-0003-4244-0365 https://orcid.org/0000-0002-0833-7674 http://dx.doi.org/10.1038/S41467-017-02410-6 Nature Communications Creative Commons Attribution 4.0 International License http://creativecommons.org/licenses/by/4.0/ application/pdf Springer Nature Nature
spellingShingle Li, Longjun
Pascal, Tod A.
Connell, Justin G.
Meckler, Stephen M.
Ma, Lin
Prendergast, David
Helms, Brett A.
Fan, Frank Yongzhen
Chiang, Yet-Ming
Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title_full Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title_fullStr Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title_full_unstemmed Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title_short Molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
title_sort molecular understanding of polyelectrolyte binders that actively regulate ion transport in sulfur cathodes
url http://hdl.handle.net/1721.1/118596
https://orcid.org/0000-0003-4244-0365
https://orcid.org/0000-0002-0833-7674
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