Journal
ENERGY STORAGE MATERIALS
Volume 49, Issue -, Pages 433-444Publisher
ELSEVIER
DOI: 10.1016/j.ensm.2022.04.035
Keywords
Solid electrolyte; Composite fiber network; Solid-state lithium battery; In-situ polymerization; 3D Li+ transport pathways
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The rational design of a unique solid electrolyte structure improves the ion conductivity and enhances the cycling performance and voltage endurance of batteries, resulting in excellent performance of lithium batteries.
Rational design of solid electrolyte is of great significance to meet the criterion for high-performance lithium batteries. Herein, a solid electrolyte containing Li+-percolated conduction network has been constructed through the in-situ polymerization of nonflammable polymer electrolyte inside silane modified-Li1.3Al0.3Ti1.7(PO4)(3) (Si@LATP)/poly (vinylidene fluoride) (PVDF) composite nanofiber membrane. Notably, the silane functionalization fully exposes the Lewis-acid sites of LATP, and the -NH3+ in polysiloxanes further enhances the anion adsorption ability of LATP based on electrostatic interaction. Characterizations and Density Function Theory (DFT) calculations suggest that the 3D Si@LATP/PVDF composite fiber network functions as an ion-regulative skeleton and facilitates the generation of continuous rapid Li+ conducting pathways. The resulting composite electrolyte integrates the features of superior ionic conductivity (1.06 mS cm(-1) at 25 C), near single-ion conducting characteristic (Li+ transference number=0.82), nanofiber backbone-reinforced interpenetrating polymer framework (tensile strength=15.3 MPa) and high-voltage endurance (4.86 V). Based on this mechanically robust composite electrolyte with regulated Li+ flux, symmetric Li cells exhibit outstanding Li stripping/plating reversibility. Benefitting from the in-situ solidification technique, continuous ionic conduction channels inside electrode and integrated electrode/electrolyte interface are guaranteed, rendering remarkable cycling performances for quasi-solid-state LiFePO4||Li cells (capacity retention of 99.9% after 200 cycles at 0.5C) and LiNi0.5Co0.2Mn0.3O2||Li cells.
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