Improving Ionic Conformality Across Polymer Electrolyte|Electrode Interfaces

Polymer electrolytes typically form physically intimate electrode interfaces but often fail to maintain continuous ionic pathways, critically limiting battery performance. Through strategic compositional design, this study introduces a molecular ionic composite electrolyte that effectively reduces interfacial ionic depletion, ensuring consistent ion transport. Enhanced ionic conformality is directly visualized, improving cycling stability in solid?state lithium batteries.Maintaining uniform ionic transport at electrode|electrolyte interfaces, i.e., ionic conformality, remains challenging in polymer electrolyte (PE)?based solid?state batteries. Morphological conformality does not necessarily imply ionic conformality. In PEs, which typically consist of a mechanically supporting component and distinct ionically conductive components, the rearrangement or depletion of mobile ion?conductive domains at interfaces can disrupt ionic transport pathways. Such localized ionic depletion contributes to interfacial instability and capacity degradation in high?voltage lithium?metal batteries. Herein, an electrolyte design approach aimed at minimizing interfacial heterogeneities is demonstrated through compositional adjustments, characterized by spatially resolved structural and chemical X?ray techniques and NMR diffusometry to elucidate ion transport dynamics. This approach improves ionic conformality at electrode interfaces, enhancing cycling stability in Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) coin and pouch cells cycled at high voltages. These results contribute to understanding interfacial behaviors in multiphase PEs and inform strategies for improving stability across solid?state battery interfaces.

» Publication Date: 21/12/2025

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This project has received funding from the European Union's Horizon 2020 research and innovation programme under grant agreement Nº 768737


                   




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