Synergistic Composite Solid Electrolyte Based on Multifunctional Polymer Networks for High-Performance Lithium Metal...

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Polymer-based solid-state electrolytes (SPEs) are crucial for high energy density lithium-metal batteries (LMBs).
• Conventional poly(ethylene oxide) (PEO)-based SPEs exhibit low ionic conductivity at room temperature and poor lithium dendrite suppression.
• These limitations stem from anion-solvate structures that reduce Li-ion transference number (LITN) and impede ion transport.

Purpose of the Study:

• To design a self-healing composite polymer electrolyte with enhanced Li-ion transport and dendrite suppression capabilities.
• To overcome the limitations of conventional PEO-based electrolytes for improved LMB performance.
• To develop a scalable strategy for creating advanced SPEs for next-generation batteries.

Main Methods:

• Incorporation of iminoboronate-functionalized networks into a polymer matrix.
• Addition of succinonitrile (SN) to create an anion-trapping polymer matrix.
• Fabrication of the self-healing iminoboronate-based polymer electrolyte (I-SHPE) and SN-embedded I-SHPE (I-SN-SHPE).

Main Results:

• The I-SN-SHPE demonstrated enhanced LITN and preserved ionic conductivity (IC).
• The electrolyte facilitated rapid, selective, and uniform Li-ion transport, enabling stable LMB operation at 1 C for 480 cycles with 88% capacity retention.
• The I-SHPE exhibited significant self-healing capacity, reinforcing mechanical properties and improving overall electrolyte stability.

Conclusions:

• The developed SN-embedded I-SHPE offers a synergistic combination of high IC, anion-capture ability, and rapid self-healing.
• This strategy effectively overcomes the intrinsic limitations of conventional PEO-based electrolytes.
• The I-SN-SHPE presents a promising pathway toward safer and more durable lithium-metal batteries.