Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries

The growing requirements for electrified applications entail exploring alternative battery systems. Lithium-sulfur batteries (LSBs) have emerged as a promising, cost-effective, and sustainable solution; however, their practical commercialization is impeded by several intrinsic challenges. With the a...

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Autores: Castillo Ruiz de Azua, Julen, Soria Fernández, Asier, Rodríguez Peña, Sergio, Rikarte, Jon, Robles Fernández, Adrián, Aldalur Ceberio, Itziar, Cid Barreno, Rosalía, González Marcos, José Antonio, Carrasco Rodríguez, Javier, Armand, Michel, Santiago Sánchez, Alexander, Carriazo, Daniel
Tipo de documento: artigo
Data de publicação:2024
País:España
Recursos:Universidad del País Vasco
Repositório:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/67339
Acesso em linha:http://hdl.handle.net/10810/67339
Access Level:Acceso aberto
Palavra-chave:2D graphene-based sulfur cathodes
electrolyte additives
electrolyte engineering
lithium metal anodes
lithium-sulfur batteries
pouch cells
solid electrolyte interphases
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spelling Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype BatteriesCastillo Ruiz de Azua, JulenSoria Fernández, AsierRodríguez Peña, SergioRikarte, JonRobles Fernández, AdriánAldalur Ceberio, ItziarCid Barreno, RosalíaGonzález Marcos, José AntonioCarrasco Rodríguez, JavierArmand, MichelSantiago Sánchez, AlexanderCarriazo, Daniel2D graphene-based sulfur cathodeselectrolyte additiveselectrolyte engineeringlithium metal anodeslithium-sulfur batteriespouch cellssolid electrolyte interphasesThe growing requirements for electrified applications entail exploring alternative battery systems. Lithium-sulfur batteries (LSBs) have emerged as a promising, cost-effective, and sustainable solution; however, their practical commercialization is impeded by several intrinsic challenges. With the aim of surpassing these challenges, the implementation of a holistic LSB concept is proposed. To this end, the effectiveness of coupling a high-performing 2D graphene-based sulfur cathode with a well-suited sparingly solvating electrolyte (SSE) is reported. The incorporation of bis(fluorosulfonyl)imide (LiFSI) salt to tune sulfolane and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether based SSE enables the formation of a robust and compact lithium fluoride-rich solid electrolyte interphase. Consequently, the lithium compatibility is improved, achieving a high Coulombic efficiency (CE) of 98.8% in the Li||Cu cells and enabling thin and dense lithium depositions. When combined with a high-performing 2D graphene-based sulfur cathode, a symbiotic effect is shown, leading to high discharge capacities, remarkable rate capability (2.5 mAh cm−2 at C/2), enhanced cell stability, and wide temperature applicability. Furthermore, the scalability of this strategy is successfully demonstrated by assembling high-performing monolayer prototype cells with a total capacity of 93 mAh, notable capacity retention of 70% after 100 cycles, and a high average CE of 99%.J.C. is a beneficiary of the Predoctoral Program from the Education Department of the Basque Government. The authors want to acknowledge GRAPHENEA for supplying graphene oxide. Chunmei Li is acknowledged for fruitful discussion. Hegoi Manzano at the University of the Basque Country is thanked for providing technical advice and access to facilities throughout computational work. This work was funded by the European Union's Horizon 2020 research and innovation program Graphene Flagship Core Project 3 (GrapheneCore3) under grant agreement 881603.WileyEuropean Commission202420242024info:eu-repo/semantics/articleapplication/pdfhttp://hdl.handle.net/10810/67339reponame:Addi. Archivo Digital para la Docencia y la Investigacióninstname:Universidad del País VascoInglésinfo:eu-repo/grantAgreement/EC/H2020/881603https://onlinelibrary.wiley.com/doi/full/10.1002/aenm.202302378info:eu-repo/semantics/openAccesshttp://creativecommons.org/licenses/by-nc-nd/3.0/es/© 2023 The Authors. Advanced Energy Materials published by Wiley-VCH GmbH This is an open access article under the terms of the Creative Commons Attribution-NonCommercial-NoDerivs License, which permits use and distribution in any medium, provided the original work is properly cited, the use is non-commercial and no modifications or adaptations are made.Atribución-NoComercial-SinDerivadas 3.0 Españaoai:addi.ehu.eus:10810/673392026-06-18T09:23:17Z
dc.title.none.fl_str_mv Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
title Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
spellingShingle Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
Castillo Ruiz de Azua, Julen
2D graphene-based sulfur cathodes
electrolyte additives
electrolyte engineering
lithium metal anodes
lithium-sulfur batteries
pouch cells
solid electrolyte interphases
title_short Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
title_full Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
title_fullStr Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
title_full_unstemmed Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
title_sort Graphene-Based Sulfur Cathodes and Dual Salt-Based Sparingly Solvating Electrolytes: A Perfect Marriage for High Performing, Safe, and Long Cycle Life Lithium-Sulfur Prototype Batteries
dc.creator.none.fl_str_mv Castillo Ruiz de Azua, Julen
Soria Fernández, Asier
Rodríguez Peña, Sergio
Rikarte, Jon
Robles Fernández, Adrián
Aldalur Ceberio, Itziar
Cid Barreno, Rosalía
González Marcos, José Antonio
Carrasco Rodríguez, Javier
Armand, Michel
Santiago Sánchez, Alexander
Carriazo, Daniel
author Castillo Ruiz de Azua, Julen
author_facet Castillo Ruiz de Azua, Julen
Soria Fernández, Asier
Rodríguez Peña, Sergio
Rikarte, Jon
Robles Fernández, Adrián
Aldalur Ceberio, Itziar
Cid Barreno, Rosalía
González Marcos, José Antonio
Carrasco Rodríguez, Javier
Armand, Michel
Santiago Sánchez, Alexander
Carriazo, Daniel
author_role author
author2 Soria Fernández, Asier
Rodríguez Peña, Sergio
Rikarte, Jon
Robles Fernández, Adrián
Aldalur Ceberio, Itziar
Cid Barreno, Rosalía
González Marcos, José Antonio
Carrasco Rodríguez, Javier
Armand, Michel
Santiago Sánchez, Alexander
Carriazo, Daniel
author2_role author
author
author
author
author
author
author
author
author
author
author
dc.contributor.none.fl_str_mv European Commission
dc.subject.none.fl_str_mv 2D graphene-based sulfur cathodes
electrolyte additives
electrolyte engineering
lithium metal anodes
lithium-sulfur batteries
pouch cells
solid electrolyte interphases
topic 2D graphene-based sulfur cathodes
electrolyte additives
electrolyte engineering
lithium metal anodes
lithium-sulfur batteries
pouch cells
solid electrolyte interphases
description The growing requirements for electrified applications entail exploring alternative battery systems. Lithium-sulfur batteries (LSBs) have emerged as a promising, cost-effective, and sustainable solution; however, their practical commercialization is impeded by several intrinsic challenges. With the aim of surpassing these challenges, the implementation of a holistic LSB concept is proposed. To this end, the effectiveness of coupling a high-performing 2D graphene-based sulfur cathode with a well-suited sparingly solvating electrolyte (SSE) is reported. The incorporation of bis(fluorosulfonyl)imide (LiFSI) salt to tune sulfolane and 1,1,2,2-tetrafluoroethyl-2,2,3,3-tetrafluoropropylether based SSE enables the formation of a robust and compact lithium fluoride-rich solid electrolyte interphase. Consequently, the lithium compatibility is improved, achieving a high Coulombic efficiency (CE) of 98.8% in the Li||Cu cells and enabling thin and dense lithium depositions. When combined with a high-performing 2D graphene-based sulfur cathode, a symbiotic effect is shown, leading to high discharge capacities, remarkable rate capability (2.5 mAh cm−2 at C/2), enhanced cell stability, and wide temperature applicability. Furthermore, the scalability of this strategy is successfully demonstrated by assembling high-performing monolayer prototype cells with a total capacity of 93 mAh, notable capacity retention of 70% after 100 cycles, and a high average CE of 99%.
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv http://hdl.handle.net/10810/67339
url http://hdl.handle.net/10810/67339
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv info:eu-repo/grantAgreement/EC/H2020/881603
https://onlinelibrary.wiley.com/doi/full/10.1002/aenm.202302378
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
http://creativecommons.org/licenses/by-nc-nd/3.0/es/
Atribución-NoComercial-SinDerivadas 3.0 España
eu_rights_str_mv openAccess
rights_invalid_str_mv http://creativecommons.org/licenses/by-nc-nd/3.0/es/
Atribución-NoComercial-SinDerivadas 3.0 España
dc.format.none.fl_str_mv application/pdf
dc.publisher.none.fl_str_mv Wiley
publisher.none.fl_str_mv Wiley
dc.source.none.fl_str_mv reponame:Addi. Archivo Digital para la Docencia y la Investigación
instname:Universidad del País Vasco
instname_str Universidad del País Vasco
reponame_str Addi. Archivo Digital para la Docencia y la Investigación
collection Addi. Archivo Digital para la Docencia y la Investigación
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