Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries
Abstract The growing demand for advanced energy storage systems requires the development of next‐generation battery technologies with superior energy density and cycle stability, with lithium–sulfur (Li–S) batteries representing a promising solution. Sulfur‐containing polyacrylonitrile cathodes (SPA...
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Wiley
2025-04-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202415436 |
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| author | Robin Moschner Martina Gerle Timo Danner Esther Kezia Simanjuntak Peter Michalowski Arnulf Latz Maryam Nojabaee Arno Kwade K. A. Friedrich |
| author_facet | Robin Moschner Martina Gerle Timo Danner Esther Kezia Simanjuntak Peter Michalowski Arnulf Latz Maryam Nojabaee Arno Kwade K. A. Friedrich |
| author_sort | Robin Moschner |
| collection | DOAJ |
| description | Abstract The growing demand for advanced energy storage systems requires the development of next‐generation battery technologies with superior energy density and cycle stability, with lithium–sulfur (Li–S) batteries representing a promising solution. Sulfur‐containing polyacrylonitrile cathodes (SPAN) for Li–S batteries are a significant advancement for this next‐generation battery chemistry, addressing the major issue of limited cycle life encountered in conventional carbon/sulfur composite cathodes. In the presented study, the influence of available ionic and electronic conduction pathways within the cathode on the electrochemical performance of SPAN‐based Li–S batteries is studied in details. To this end, a series of SPAN cathodes with different microstructures is prepared by adapting the compression degree of calendering. Mechanical and morphological characterizations confirm a pronounced springback effect due to a characteristic elastic deformation behavior of SPAN. Electrochemical impedance spectroscopy (EIS) shows increased cathode impedance values with multiple overlapping processes in the high‐ to mid‐frequency region in highly compressed SPAN cathodes. Moreover, while the (first) discharge capacity is unaffected, the subsequent charge capacity decreases substantially for highly compressed cathodes. The electrochemical experiments and electrochemical continuum simulations confirm that this phenomenon is mainly due to the disturbance of the electronic percolation pathways caused by the springback behavior during calendering. |
| format | Article |
| id | doaj-art-25d12646161c410399bf8f9eba024507 |
| institution | OA Journals |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-04-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-25d12646161c410399bf8f9eba0245072025-08-20T02:17:28ZengWileyAdvanced Science2198-38442025-04-011215n/an/a10.1002/advs.202415436Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur BatteriesRobin Moschner0Martina Gerle1Timo Danner2Esther Kezia Simanjuntak3Peter Michalowski4Arnulf Latz5Maryam Nojabaee6Arno Kwade7K. A. Friedrich8Institute for Particle Technology Technische Universität Braunschweig Volkmaroder Straße 5 D‐38104 Braunschweig GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyInstitute for Particle Technology Technische Universität Braunschweig Volkmaroder Straße 5 D‐38104 Braunschweig GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyInstitute for Particle Technology Technische Universität Braunschweig Volkmaroder Straße 5 D‐38104 Braunschweig GermanyInstitute of Engineering Thermodynamics German Aerospace Center (DLR) Pfaffenwaldring 38‐40 D‐70569 Stuttgart GermanyAbstract The growing demand for advanced energy storage systems requires the development of next‐generation battery technologies with superior energy density and cycle stability, with lithium–sulfur (Li–S) batteries representing a promising solution. Sulfur‐containing polyacrylonitrile cathodes (SPAN) for Li–S batteries are a significant advancement for this next‐generation battery chemistry, addressing the major issue of limited cycle life encountered in conventional carbon/sulfur composite cathodes. In the presented study, the influence of available ionic and electronic conduction pathways within the cathode on the electrochemical performance of SPAN‐based Li–S batteries is studied in details. To this end, a series of SPAN cathodes with different microstructures is prepared by adapting the compression degree of calendering. Mechanical and morphological characterizations confirm a pronounced springback effect due to a characteristic elastic deformation behavior of SPAN. Electrochemical impedance spectroscopy (EIS) shows increased cathode impedance values with multiple overlapping processes in the high‐ to mid‐frequency region in highly compressed SPAN cathodes. Moreover, while the (first) discharge capacity is unaffected, the subsequent charge capacity decreases substantially for highly compressed cathodes. The electrochemical experiments and electrochemical continuum simulations confirm that this phenomenon is mainly due to the disturbance of the electronic percolation pathways caused by the springback behavior during calendering.https://doi.org/10.1002/advs.202415436calenderingelectrochemical characterizationelectrochemical impedance spectroscopyLithium–sulfur batterymechanical characterizationnumerical simulation |
| spellingShingle | Robin Moschner Martina Gerle Timo Danner Esther Kezia Simanjuntak Peter Michalowski Arnulf Latz Maryam Nojabaee Arno Kwade K. A. Friedrich Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries Advanced Science calendering electrochemical characterization electrochemical impedance spectroscopy Lithium–sulfur battery mechanical characterization numerical simulation |
| title | Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries |
| title_full | Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries |
| title_fullStr | Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries |
| title_full_unstemmed | Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries |
| title_short | Impact of the Sulfurized Polyacrylonitrile Cathode Microstructure on the Electrochemical Performance of Lithium–Sulfur Batteries |
| title_sort | impact of the sulfurized polyacrylonitrile cathode microstructure on the electrochemical performance of lithium sulfur batteries |
| topic | calendering electrochemical characterization electrochemical impedance spectroscopy Lithium–sulfur battery mechanical characterization numerical simulation |
| url | https://doi.org/10.1002/advs.202415436 |
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