Abstract

The intrinsic drawbacks of electrolytes and the growth of lithium dendrites limit the development of commercial lithium batteries. To address the aforementioned challenges, a novel biomimetic brain-like nanostructure (BBLN) solid polymer electrolyte was created by manipulating the shape of the incorporated nanoparticles. Our designed BBLN solid polymer electrolyte was created by incorporating spherical core-shell (UIO-66@67) fillers into polymer electrolyte, which is significantly different from traditional polymer-based composite electrolytes. UIO-66@67 spherical nanoparticles are highly favorable to eliminating polymer electrolyte stress and deformation during solidification, indicating a great potential for fabricating highly uniform BBLN solid polymer electrolytes with a substantial number of continuous convolutions. Furthermore, spherical nanoparticles can significantly reduce the crystalline structure of polymer electrolytes, improving polymer chain segmental movement and providing continuous pathways for rapid ion transfer. As a result, BBLN solid polymer electrolyte shows excellent ionic conductivity (9.2 × 10−4 S cm−1), a high lithium transference number (0.74), and outstanding cycle stability against lithium electrodes over 6500 h at room temperature. The concept of biomimetic brain-like nanostructures in this work demonstrates a novel strategy to enhance ion transport in polymer-based electrolytes for solid-state batteries.

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