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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Detalles Bibliográficos
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 recurso: artículo
Fecha de publicación:2024
País:España
Institución:Universidad del País Vasco
Repositorio:Addi. Archivo Digital para la Docencia y la Investigación
OAI Identifier:oai:addi.ehu.eus:10810/67339
Acceso en línea:http://hdl.handle.net/10810/67339
Access Level:acceso abierto
Palabra clave:2D graphene-based sulfur cathodes
electrolyte additives
electrolyte engineering
lithium metal anodes
lithium-sulfur batteries
pouch cells
solid electrolyte interphases
Descripción
Sumario: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%.