Key Findings
The prelithiated PU/LAGP (PLAP) composite electrolyte achieves a room-temperature ionic conductivity of 3.8 × 10⁻⁴ S/cm. In symmetrical cell testing, the electrolyte demonstrated stable cycling for 750 hours at an ultrahigh current density of 10 mA cm-2. When integrated into LiFePO4(LFP)|PLAP|Li full cells, the system maintained capacity retentions of 95.7%, 91%, and 87.8% during cycles at 0.2 C, C, and 2C, respectively.
Technical Details
The PLAP electrolyte utilizes a customized soft-hard segmented architecture combining a prelithiated polyurethane (PU) matrix with Li1.5Al0.5Ge0.5P3O12 (LAGP) fillers. This structure provides significant mechanical strength, specifically a tensile strength of 5.47 MPa and 192.4% elongation.
Computational and spectroscopic analyses indicate that terminal-group prelithiation (−OH →−OLi) reduces the interfacial Li⁺ binding energy from 1.01 eV to 0.55 eV. This reduction is proposed to liberate trapped Li⁺ ions, facilitating faster ion transport. These results were validated by comparing the PLAP electrolyte against a non-prelithiated −OH-terminated PU/LAGP baseline under identical formulation and testing conditions.
Background & Context
The practical deployment of all-solid-state lithium batteries (ASSLBs) has been hindered by two primary factors: the compromise between mechanical robustness and ionic conductivity, and sluggish interfacial transport caused by “ion trapping.” The development of the PLAP electrolyte specifically targets these bottlenecks by integrating a rigid-flexible network with a chemical modification to the polymer matrix.
Significance & Outlook
By utilizing a prelithiation-driven design to attenuate binding energy and liberate trapped ions, this approach provides a viable pathway for the development of highly durable, fast-charging, and liquid-free all-solid-state lithium-metal batteries.
Source: https://www.frontiersin.org/journals/chemistry/articles/10.3389/fchem.2026.1908013/full
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