Closed-Loop Recyclable Lithium and Sodium Conducting Covalent Adaptable Networks

Area of Science:

• Polymer Chemistry
• Materials Science
• Electrochemistry

Background:

• Covalent adaptable networks (CANs) are advanced polymers merging thermoset and thermoplastic properties.
• Existing CANs with charged side chains are limited, with few featuring negatively charged backbones.
• Integrating permanent charge into polymer backbones can unlock novel applications.

Purpose of the Study:

• To introduce a new class of aliphatic spiroborate-linked ionic covalent adaptable networks (ICANs).
• To develop dynamic ionomer thermosets with permanently charged backbones.
• To explore their potential as flexible solid-state electrolytes.

Main Methods:

• Synthesis of ICANs using a catalyst-free, scalable, and eco-friendly approach.
• Incorporation of lithium or sodium as counter cations.
• Fabrication and testing of a device utilizing the ICANs as solid-state electrolytes.

Main Results:

• ICANs exhibited promising ion conductivity without plasticizers.
• The spiroborate linkages enabled rapid reprocessing and recycling under moderate conditions.
• Demonstrated robust conducting performance in a device under extreme physical deformation, alongside self-healing capabilities.

Conclusions:

• Aliphatic spiroborate-linked ICANs represent a novel category of dynamic ionomer thermosets.
• These materials offer a sustainable and versatile platform for flexible electronic devices.
• The study highlights new possibilities for developing advanced dynamic ionomer thermosets.