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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Springer Nature
2018
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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]. |
first_indexed | 2024-09-23T15:10:40Z |
format | Article |
id | mit-1721.1/118596 |
institution | Massachusetts Institute of Technology |
last_indexed | 2024-09-23T15:10:40Z |
publishDate | 2018 |
publisher | Springer Nature |
record_format | dspace |
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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