Hybrid solid electrolyte composition and hybrid solid electrolyte manufactured therefrom

Low-interfacial resistance electrolyte with ion channels formed by a co-continuous phase of photopolymerized gel and sulfide

This technology implements a co-continuous phase structure where sulfide-based solid electrolytes and gel polymer electrolytes each form continuous lithium-ion channels, maximizing ionic conductivity and reducing interfacial resistance.

Conventional inorganic solid electrolytes are brittle and suffer from high interfacial resistance with electrodes, which can lead to dendrite growth. Conversely, polymer electrolytes have low ionic conductivity, limiting their use as standalone solutions.

This technology involves mixing a gel polymer electrolyte precursor—composed of 1–15 wt% photopolymerizable monomer, LiFSI, and a glyme-based compound—with a sulfide-based solid electrolyte in a weight ratio of 1:9 to 3:7. It then undergoes photopolymerization and a 50–250 MPa surface compression process to form a co-continuous phase. Applicable to separator-replacement sheets or non-woven thin-film electrolyte layers in argyrodite-based all-solid-state batteries, it achieves ionic conductivity of over 10^-3 S/cm at room temperature while reducing process defects caused by brittleness.

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Key Features:

• Gel polymer electrolyte precursor solution containing a photopolymerizable monomer, lithium bis(fluorosulfonyl)imide, and a glyme-based compound
• Multifunctional (meth)acrylate-based photopolymerizable monomer included at 1 to less than 15 wt% of the total precursor solution weight
• Argyrodite crystal structure sulfide-based solid electrolyte forming a co-continuous phase with a gel polymer electrolyte having an elasticity of 10 to less than 220 MPa
• Step of forming a co-continuous phase by polymerizing the composition via light irradiation followed by surface compression

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This invention was developed with support from the Ministry of Science and ICT for a single-ion conductor-based multidimensional free-form power system.

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