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Constructing high-ionic-conductivity solid-state electrolytes with improved interface stability by rapid laser processing
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DOI：10.1016/j.jechem.2025.06.062.png)
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Abstract
En 中文
All-solid-state batteries (ASSBs) with Li or Si anodes promise enhanced safety and high energy densities but face challenges with complex fabrication, stringent storage requirements, and pressure-dependent operation. Polyethylene oxide (PEO)-based composite solid electrolytes (CSEs) enable easy processing and flexible interfaces, supporting pressure-free operation and reducing costs. However, their low ionic conductivity remains a key limitation. Here, we present a rapid (∼5 min) and eco-friendly laser modification strategy for post-synthesized PEO CSEs, achieving enhanced ionic conductivity while retaining the attributes of simple fabrication and compatibility with Li and Si anodes under pressure-free operation. Laser engineering reduces PEO crystallinity, introduces additional Li+ coordination sites, and improves interfacial stability through tailored solid electrolyte interphases. The laser-modified electrolyte enables LiFePO4//Li cells to retain 142.4 mAh g−1 after 800 cycles with 99.8% Coulombic efficiency at 1 C and 60 °C. Moreover, without stack pressure, a Si anode paired with the laser-modified electrolyte delivers a high capacity of 1710.3 mAh g−1 with 56% retention at 0.5 A g−1 after 50 cycles at 60 °C. Beyond performance enhancements, this work establishes a link between fluorescence emission and Li+ transport in CSEs. Specifically, fluorescence shifts to shorter wavelengths correspond to shorter molecular chain lengths and lower coordination bonds, supported by time-dependent density functional theory calculations. These factors give rise to improved Li+ transport. This optical probe offers a non-destructive approach for rapidly assessing electrolyte properties and enriching electrolyte design. Overall, this work demonstrates laser engineering as a practical post-synthetic strategy and highlights fluorescence as a practical indicator for advancing next-generation ASSBs.
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