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Covalent adaptable networks (CANs) represent a novel class of polymeric materials crosslinked by dynamic covalent bonds. Since their first discovery, CANs have attracted great attention due to their high mechanical strength and stability like conventional thermosets under service conditions and easy reprocessability like thermoplastics under certain external stimuli. Here, we report the first example of ionic covalent adaptable networks (ICANs), a type of crosslinked ionomers, consisting of negatively charged backbone structures. More specifically, two ICANs with different backbone compositions were prepared through spiroborate chemistry. Given the dynamic nature of the spiroborate linkages, the resulting ionomer thermosets display rapid reprocessability and closed-loop recyclability under mild conditions. The materials mechanically broken into smaller pieces can be reprocessed into coherent solids at 120 °C within only 1 min with nearly 100% recovery of the mechanical properties. Upon treating the ICANs with dilute hydrochloric acid at room temperature, the valuable monomers can be easily chemically recycled in almost quantitative yield. This work demonstrates the great potential of spiroborate bonds as a novel dynamic ionic linkage for development of new reprocessable and recyclable ionomer thermosets.
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This content will become publicly available on April 17, 2026
Closed‐Loop Recyclable Lithium and Sodium Conducting Covalent Adaptable Networks
Abstract Within the past two decades, covalent adaptable networks (CANs) have emerged as a novel class of dynamically crosslinked polymers, combining the benefits of thermosets and thermoplastics. Although some CANs with charged side chains have been reported, CANs with negatively charged backbones remain very limited. The integration of permanent charge into the backbones upon their formation could open up important new applications. Here, we introduce a series of aliphatic spiroborate‐linked ionic covalent adaptable networks (ICANs), representing a new category of dynamic ionomer thermosets. These ICANs were synthesized using a catalyst‐free, scalable, and environment‐friendly method. Incorporating lithium or sodium as counter cations in these networks yielded promising ion conductivity without the need of plasticizers. The dynamic nature of the spiroborate linkages in these materials allows for rapid reprocessing and recycling under moderate conditions. Furthermore, their potential as flexible solid‐state electrolytes is demonstrated in a device that maintained robust conducting performance under extreme physical deformation, coupled with effective self‐healing properties. This research opens new possibilities for future development of dynamic ionomer thermosets and their potential applications in flexible electronic devices.
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- PAR ID:
- 10596653
- Publisher / Repository:
- Wiley-VCH GmbH
- Date Published:
- Journal Name:
- Angewandte Chemie International Edition
- Volume:
- 64
- Issue:
- 17
- ISSN:
- 1433-7851
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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