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Printed solid polymer electrolytes for high-performance solid-state lithium-ion battery

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Resumo:Energy storage systems (ESSs) play a key role in energy security and the digital revolution, strongly associated with mobility, where the intensive demand for portable electronic devices stimulates the development of new, improved, safer and more sustainable ESSs with higher energy and power density, in which solid polymer electrolytes (SPE) are considered a promising technology to overcome these challenges in the near future. Thus, this work developed printed SPE produced by Direct-Ink Writing (DIW). The SPEs are based on poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)), clinoptilolite zeolite (CPT) and 1-methyl-1- propylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([PMPyr][TFSI]) ionic liquid. Furthermore, the conventional solvent of PVDF based polymers, N-dimethylformamide (DMF), is replaced by more sustainable and environmentally friendly solvents such as dimethyl sulfoxide (DMSO), acetone, and N-methyl-2-pyrrolidone (NMP). Rheological properties play a key role in the printability of materials and the produced inks must have a non-Newtonian performance, so they can be effectively extruded and maintain the desired membrane shape after coming into contact with the substrate. The different types of solvents have an impact on the samples' mechanical characteristics and polymer phase. They also have a significant impact on electrochemical parameters including lithium-transference number, and ionic conductivity value. The SPE produced with acetone solvent presents the best ionic conductivity (1.5 × 10− 5 S cm− 1 ) and lithium ion transference number (0.45). Excellent performance was shown in the charge and discharge testing of batteries at C/10, with values of 135 mAh.g− 1 for SPE prepared with acetone solvent after 60 cycles. This study shows the importance of the solvent in the formulation of ternary SPE to maximize the performance of solid-state batteries. The effect of the solvent on printed SPE for solid-state batteries is thus proven for the first time. The obtained results demonstrate the viability of DIW printing technique and environmentally friendly solvents, for a new generation of all printed and sustainable solid-state batteries.
Autores principais:Pinto, Rafael Santos
Outros Autores:Barbosa, J.; Fidalgo Marijuan, A.; Hilliou, L.; Gonçalves, Renato Ferreira; Costa, Carlos Miguel Silva; Lanceros-Mendez, S.
Assunto:Solid polymer electrolytes Printing techniques Solid-state batteries
Ano:2026
País:Portugal
Tipo de documento:artigo
Tipo de acesso:acesso restrito
Instituição associada:Universidade do Minho
Idioma:inglês
Origem:RepositóriUM - Universidade do Minho
Descrição
Resumo:Energy storage systems (ESSs) play a key role in energy security and the digital revolution, strongly associated with mobility, where the intensive demand for portable electronic devices stimulates the development of new, improved, safer and more sustainable ESSs with higher energy and power density, in which solid polymer electrolytes (SPE) are considered a promising technology to overcome these challenges in the near future. Thus, this work developed printed SPE produced by Direct-Ink Writing (DIW). The SPEs are based on poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)), clinoptilolite zeolite (CPT) and 1-methyl-1- propylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([PMPyr][TFSI]) ionic liquid. Furthermore, the conventional solvent of PVDF based polymers, N-dimethylformamide (DMF), is replaced by more sustainable and environmentally friendly solvents such as dimethyl sulfoxide (DMSO), acetone, and N-methyl-2-pyrrolidone (NMP). Rheological properties play a key role in the printability of materials and the produced inks must have a non-Newtonian performance, so they can be effectively extruded and maintain the desired membrane shape after coming into contact with the substrate. The different types of solvents have an impact on the samples' mechanical characteristics and polymer phase. They also have a significant impact on electrochemical parameters including lithium-transference number, and ionic conductivity value. The SPE produced with acetone solvent presents the best ionic conductivity (1.5 × 10− 5 S cm− 1 ) and lithium ion transference number (0.45). Excellent performance was shown in the charge and discharge testing of batteries at C/10, with values of 135 mAh.g− 1 for SPE prepared with acetone solvent after 60 cycles. This study shows the importance of the solvent in the formulation of ternary SPE to maximize the performance of solid-state batteries. The effect of the solvent on printed SPE for solid-state batteries is thus proven for the first time. The obtained results demonstrate the viability of DIW printing technique and environmentally friendly solvents, for a new generation of all printed and sustainable solid-state batteries.

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