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...

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Autores principales: Schütze, Yannik, Gayen, Diptesh, Palczynski, Karol, de Oliveira Silva, Ranielle, Lu, Yan, Tovar, Michael, Partovi-Azar, Pouya, Bande, Annika, Dzubiella, Joachim
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
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.
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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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