Atomic and Molecular Structure Regulated In Situ Cross-Linked Polyurethane Gel Electrolyte for High-Performance...

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Conventional electrolytes hinder lithium metal battery (LMB) performance due to incompatibility with high-voltage cathodes and lithium metal anodes.
• Developing stable electrolytes is crucial for advancing high-energy-density battery technologies.

Purpose of the Study:

• To design and synthesize an in situ cross-linked polyurethane gel electrolyte (G-P3 AR) for high-performance LMBs.
• To regulate atomic and molecular structures for enhanced electrochemical stability and ion transport.

Main Methods:

• Atomic and molecular structure regulation of polyurethane.
• Synthesis of a cross-linked gel electrolyte (G-P3 AR).
• Electrochemical characterization including stability window, rate capability, and cycling performance in Li||NCM811 cells.

Main Results:

• The G-P3 AR electrolyte exhibits an extended electrochemical stability window of 4.97 V, compatible with NCM811 cathodes.
• Enhanced Li+ transport with a transference number of 0.78 due to immobilized anions and reduced desolvation barrier.
• Achieved high rate capability (157.7 mAh g-1 at 2 C) and excellent cycling stability (81.7% capacity retention after 500 cycles).

Conclusions:

• The designed G-P3 AR electrolyte offers a viable strategy for high-performance lithium metal batteries.
• Atomic and molecular structure control is key to overcoming electrolyte limitations in advanced battery systems.
• This work paves the way for safer and more efficient energy storage solutions.