Solid-state electrolytes (SSEs) could represent the key to solve safety issues of lithium-ion batteries (LIBs). Among them, those obtained by homogenously dispersing inorganic nanofillers into a polymer matrix combine advantages of all SSE typologies. In this work, high-entropy (Cr,Mn,Fe,Co,Ni) oxide (HEO) with different morphology (nanoparticles or nanofibers) are evaluated as passive fillers for the preparation of composite polyethylene oxide (PEO)-based SSEs. By varying their preparation conditions (calcination at 400 or 800 ◦C for 0.5 or 2 h, followed by rapid cooling) different size and crystallization degree of the oxide grains are obtained. The results of the electrochemical testing of the PEO/HEO composites evidence the crucial role of the filler microstructure and morphology. The best results in terms of electrolyte resistance (22.5 Ω), electrochemical stability window (4.7 V), Li+transference number (0.37) and ionic conductivity (3.0⋅10− 4 S cm− 1 at 65 ◦C) are obtained by using well crystallized HEO nanofibers with highly defective surface. The suitability of the most promising composite for practical applications is validated by successfully using it in full cell with commercial high-voltage cathode materials.

Evaluation of high-entropy (Cr, Mn, Fe, Co, Ni)-oxide nanofibers and nanoparticles as passive fillers for solid composite electrolytes

Patriarchi, Asia;Minnetti, Luca;Nobili, Francesco
;
2025-01-01

Abstract

Solid-state electrolytes (SSEs) could represent the key to solve safety issues of lithium-ion batteries (LIBs). Among them, those obtained by homogenously dispersing inorganic nanofillers into a polymer matrix combine advantages of all SSE typologies. In this work, high-entropy (Cr,Mn,Fe,Co,Ni) oxide (HEO) with different morphology (nanoparticles or nanofibers) are evaluated as passive fillers for the preparation of composite polyethylene oxide (PEO)-based SSEs. By varying their preparation conditions (calcination at 400 or 800 ◦C for 0.5 or 2 h, followed by rapid cooling) different size and crystallization degree of the oxide grains are obtained. The results of the electrochemical testing of the PEO/HEO composites evidence the crucial role of the filler microstructure and morphology. The best results in terms of electrolyte resistance (22.5 Ω), electrochemical stability window (4.7 V), Li+transference number (0.37) and ionic conductivity (3.0⋅10− 4 S cm− 1 at 65 ◦C) are obtained by using well crystallized HEO nanofibers with highly defective surface. The suitability of the most promising composite for practical applications is validated by successfully using it in full cell with commercial high-voltage cathode materials.
2025
High-entropy oxides, Nanofibers, Nanoparticles, Poly(ethylene oxide), Solid composite electrolytes, Lithium-ion batteries
262
File in questo prodotto:
Non ci sono file associati a questo prodotto.

I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11581/487471
 Attenzione

Attenzione! I dati visualizzati non sono stati sottoposti a validazione da parte dell'ateneo

Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus ND
  • ???jsp.display-item.citation.isi??? ND
social impact