Catalytic Functional Domain Enables Rapid Li⁺ Conduction in Polyether Electrolytes for Quasi-Solid-State Batteries.

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Polyether electrolytes (PEs) show promise for lithium (Li) metal batteries but suffer from low Li+ conduction due to poor Li+ dissociation and transport.
• Strong Li+-polymer coordination hinders ion mobility, limiting practical applications.

Purpose of the Study:

• To develop an innovative "catalytic functional domain" strategy to enhance Li+ conduction in PEs for high-performance quasi-solid-state batteries (QSSBs).

Main Methods:

• Incorporation of Ti4+-based catalytic sites with weak Lewis acidity and high-dielectric properties during in situ polymerization.
• Construction of catalytic functional regions to promote Li salt dissociation and weaken Li+-polymer coordination.

Main Results:

• Achieved ionic conductivity of 1.14 mS cm-1 at 25 °C and a Li+ transference number of 0.77.
• Demonstrated stable cycling (>2800 h) in Li||Li symmetric cells with dendrite-free Li deposition.
• Achieved high capacity retention (82.4% after 600 cycles) in Li||LiNi0.5Co0.2Mn0.3O2 cells and sustained cycling in high-voltage cells.

Conclusions:

• The catalytic functional domain strategy effectively accelerates Li+ conduction in PEs.
• This approach offers a new paradigm for designing advanced polymer electrolytes for high-performance QSSBs.