Dielectric?Tailored Space Charge Layer and Ion Coordination Structure for High?Voltage Polymer All?Solid?State Lithium Batteries

This study presents a novel composite solid?state polymer electrolyte incorporated dielectric BaTiO3 nanofillers (PDB) for advanced high?voltage all?solid?state lithium batteries. The design achieves a tailored coordination structure, diminished space charge layer, improved ion transport, and enhanced oxidative stability, making this approach a promising strategy for practical long?cycling all?solid?state lithium batteries.The poor structural stability of polymer electrolytes and sluggish ion transport kinetics of interfaces with cathode limit the fundamental performance improvements of polymer all?solid?state lithium metal batteries under high voltages. Herein, it is revealed that by introducing dielectric BaTiO3 in an in?situ polymerized composite solid?state electrolyte, the generated interaction between the ether group of polymer electrolyte and dielectric material could effectively regulate the lithium?ion (Li+) coordination structure to achieve an oxidative potential higher than 5.2 V. The dielectric BaTiO3 with spontaneous polarization also weakens the space charge layer effect between the cathode and electrolyte, facilitating fast Li+ transport kinetics across the cathode/electrolyte interfaces. The all?solid?state LiNi0.8Co0.1Mn0.1O2/Li batteries with the dielectric composite solid?state electrolyte exhibit an ultra?long cycling life of 1800 and 1300 cycles at room temperature under high cut?off voltages of 4.6 and 4.7 V, respectively. This work highlights the critical role of dielectric materials in high?performance solid?state electrolytes and provides a promising strategy to realize high?voltage long?life all?solid?state lithium metal batteries.

» Publication Date: 27/03/2025

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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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