Tailoring electrolyte coordination structure for high-rate polymer-based solid-state batteries.

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Solid-state batteries (SSBs) promise enhanced safety and energy density over conventional batteries.
• Polymer-based solid-state electrolytes (SSEs) offer processing advantages but suffer from low ionic conductivity and limited stability.
• Overcoming these limitations is crucial for advancing high-performance SSBs.

Purpose of the Study:

• To develop a novel solvation-tailoring strategy for polymer-based solid-state electrolytes.
• To enhance ionic conductivity and electrochemical stability in SSBs.
• To improve the rate capability and overall performance of polymer-based SSBs.

Main Methods:

• Embedding zirconium-based metal-organic framework (MOF808) nanofillers into a polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) matrix.
• Utilizing MOF808's strong solvent adsorption to alter the Li+ solvation sheath and promote anion-rich configurations.
• Quantifying changes in solvation environment and Li+ transport kinetics via computational analysis.

Main Results:

• The novel PLM-3 electrolyte demonstrated significantly enhanced Li+ transport kinetics by reducing desolvation energy by 15.8%.
• Cells utilizing the PLM-3 electrolyte and a SC-NCM83 cathode exhibited excellent rate capability (182.8 mAh g-1 at 5C).
• The PLM-3 electrolyte maintained 93.73% capacity retention after 200 cycles at 1C with a 4.3 V cutoff voltage.

Conclusions:

• The proposed solvation-tailoring strategy effectively enhances ion transport in polymer-based SSEs.
• This approach redefines performance limits for polymer-based SSBs, enabling high-power and high-energy applications.
• The findings pave the way for developing industrially viable, high-performance solid-state batteries.