Improved LiTransport and Interfacial Stability in PEO-LiTFSI Solid Electrolytes via AlOCeramic Fillers at 20 °C
Source: PubMed Central Open Access, NCBI / U.S. National Library of Medicine
Incorporation of ceramic nanofillers (AlO, SiO, TiO) into PEO-based solid electrolytes is investigated to compare their effects on Litransport and address the low room-temperature conductivity of PEO by reducing polymer crystallinity and facilitating Limigration through the amorphous phase. Among the tested fillers, 5 wt % AlOreduces membrane crystallinity by ≈ 11% and increases ionic conductivity by ≈1.8-fold. Comparative analysis suggests that AlOstands out due to possible interactions with PEO ether oxygens, as supported by structural and spectroscopic analyses. These interactions generate interconnected Litransport pathways along polymer–filler interfaces, improving ionic conduction. Structural (XRD, FTIR, Raman) and thermal (TGA/DSC) analyses confirm an amorphous and thermally stable network. Electrochemical studies demonstrate that the AlO-containing membrane provides extended oxidation stability up to 5.22 V, with Litransference number and diffusion coefficient 2.58 and 8 times higher than those of the filler-free PEO-LiTFSI system, respectively. This membrane displays reduced overpotential and an almost 100% recovery ratio after current-step cycling, emphasizing superior interfacial compatibility. Stable Li plating/stripping for ≈780 h at 50 μA cmfurther confirms suppression of lithium dendrite growth, achieving a cycling lifetime 5.5 times longer. These findings highlight the role of AlOin promoting efficient low-temperature interfacial Liconduction, offering promisi
Abstract
Incorporation of ceramic nanofillers (AlO, SiO, TiO) into PEO-based solid electrolytes is investigated to compare their effects on Litransport and address the low room-temperature conductivity of PEO by reducing polymer crystallinity and facilitating Limigration through the amorphous phase. Among the tested fillers, 5 wt % AlOreduces membrane crystallinity by ≈ 11% and increases ionic conductivity by ≈1.8-fold. Comparative analysis suggests that AlOstands out due to possible interactions with PEO ether oxygens, as supported by structural and spectroscopic analyses. These interactions generate interconnected Litransport pathways along polymer–filler interfaces, improving ionic conduction. Structural (XRD, FTIR, Raman) and thermal (TGA/DSC) analyses confirm an amorphous and thermally stable network. Electrochemical studies demonstrate that the AlO-containing membrane provides extended oxidation stability up to 5.22 V, with Litransference number and diffusion coefficient 2.58 and 8 times higher than those of the filler-free PEO-LiTFSI system, respectively. This membrane displays reduced overpotential and an almost 100% recovery ratio after current-step cycling, emphasizing superior interfacial compatibility. Stable Li plating/stripping for ≈780 h at 50 μA cmfurther confirms suppression of lithium dendrite growth, achieving a cycling lifetime 5.5 times longer. These findings highlight the role of AlOin promoting efficient low-temperature interfacial Liconduction, offering promising insights for the design of solid polymer electrolytes. http://www.w3.org/1999/xlink abs1 float portrait ao6c03400_0017.jpg graphical http://www.w3.org/1999/xlink tgr1 not-for-print float portrait ao6c03400_0015.jpg toc-graphic