How Regiochemistry Influences Aggregation Behavior and Charge Transport in Conjugated Organosulfur Polymer Cathodes for Lithium–Sulfur Batteries
[Image: see text] For lithium–sulfur (Li–S) batteries to become competitive, they require high stability and energy density. Organosulfur polymer-based cathodes have recently shown promising performance due to their ability to overcome common limitations of Li–S batteries, such as the insulating nat...
Autores principales: | , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10141565/ https://www.ncbi.nlm.nih.gov/pubmed/37014093 http://dx.doi.org/10.1021/acsnano.3c01523 |
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author | Schütze, Yannik Gayen, Diptesh Palczynski, Karol de Oliveira Silva, Ranielle Lu, Yan Tovar, Michael Partovi-Azar, Pouya Bande, Annika Dzubiella, Joachim |
author_facet | Schütze, Yannik Gayen, Diptesh Palczynski, Karol de Oliveira Silva, Ranielle Lu, Yan Tovar, Michael Partovi-Azar, Pouya Bande, Annika Dzubiella, Joachim |
author_sort | Schütze, Yannik |
collection | PubMed |
description | [Image: see text] For lithium–sulfur (Li–S) batteries to become competitive, they require high stability and energy density. Organosulfur polymer-based cathodes have recently shown promising performance due to their ability to overcome common limitations of Li–S batteries, such as the insulating nature of sulfur. In this study, we use a multiscale modeling approach to explore the influence of the regiochemistry of a conjugated poly(4-(thiophene-3-yl)benzenethiol) (PTBT) polymer on its aggregation behavior and charge transport. Classical molecular dynamics simulations of the self-assembly of polymer chains with different regioregularity show that a head-to-tail/head-to-tail regularity can form a well-ordered crystalline phase of planar chains allowing for fast charge transport. Our X-ray diffraction measurements, in conjunction with our predicted crystal structure, confirm the presence of crystalline phases in the electropolymerized PTBT polymer. We quantitatively describe the charge transport in the crystalline phase in a band-like regime. Our results give detailed insights into the interplay between microstructural and electrical properties of conjugated polymer cathode materials, highlighting the effect of polymer chain regioregularity on its charge transport properties. |
format | Online Article Text |
id | pubmed-10141565 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-101415652023-04-29 How Regiochemistry Influences Aggregation Behavior and Charge Transport in Conjugated Organosulfur Polymer Cathodes for Lithium–Sulfur Batteries Schütze, Yannik Gayen, Diptesh Palczynski, Karol de Oliveira Silva, Ranielle Lu, Yan Tovar, Michael Partovi-Azar, Pouya Bande, Annika Dzubiella, Joachim ACS Nano [Image: see text] For lithium–sulfur (Li–S) batteries to become competitive, they require high stability and energy density. Organosulfur polymer-based cathodes have recently shown promising performance due to their ability to overcome common limitations of Li–S batteries, such as the insulating nature of sulfur. In this study, we use a multiscale modeling approach to explore the influence of the regiochemistry of a conjugated poly(4-(thiophene-3-yl)benzenethiol) (PTBT) polymer on its aggregation behavior and charge transport. Classical molecular dynamics simulations of the self-assembly of polymer chains with different regioregularity show that a head-to-tail/head-to-tail regularity can form a well-ordered crystalline phase of planar chains allowing for fast charge transport. Our X-ray diffraction measurements, in conjunction with our predicted crystal structure, confirm the presence of crystalline phases in the electropolymerized PTBT polymer. We quantitatively describe the charge transport in the crystalline phase in a band-like regime. Our results give detailed insights into the interplay between microstructural and electrical properties of conjugated polymer cathode materials, highlighting the effect of polymer chain regioregularity on its charge transport properties. American Chemical Society 2023-04-04 /pmc/articles/PMC10141565/ /pubmed/37014093 http://dx.doi.org/10.1021/acsnano.3c01523 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Schütze, Yannik Gayen, Diptesh Palczynski, Karol de Oliveira Silva, Ranielle Lu, Yan Tovar, Michael Partovi-Azar, Pouya Bande, Annika Dzubiella, Joachim How Regiochemistry Influences Aggregation Behavior and Charge Transport in Conjugated Organosulfur Polymer Cathodes for Lithium–Sulfur Batteries |
title | How
Regiochemistry Influences Aggregation Behavior
and Charge Transport in Conjugated Organosulfur Polymer Cathodes for
Lithium–Sulfur Batteries |
title_full | How
Regiochemistry Influences Aggregation Behavior
and Charge Transport in Conjugated Organosulfur Polymer Cathodes for
Lithium–Sulfur Batteries |
title_fullStr | How
Regiochemistry Influences Aggregation Behavior
and Charge Transport in Conjugated Organosulfur Polymer Cathodes for
Lithium–Sulfur Batteries |
title_full_unstemmed | How
Regiochemistry Influences Aggregation Behavior
and Charge Transport in Conjugated Organosulfur Polymer Cathodes for
Lithium–Sulfur Batteries |
title_short | How
Regiochemistry Influences Aggregation Behavior
and Charge Transport in Conjugated Organosulfur Polymer Cathodes for
Lithium–Sulfur Batteries |
title_sort | how
regiochemistry influences aggregation behavior
and charge transport in conjugated organosulfur polymer cathodes for
lithium–sulfur batteries |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10141565/ https://www.ncbi.nlm.nih.gov/pubmed/37014093 http://dx.doi.org/10.1021/acsnano.3c01523 |
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