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A reduction-oxidation reaction is commonly called a redox reaction. In a redox reaction, electrons are transferred from one species to another rather than being shared between or among atoms. The reducing agent or reductant is the species that loses electrons and gets oxidized in the process. The species that gains electrons and gets reduced in the process is the oxidizing agent or oxidant. Redox reactions are represented as two separate equations called half-reactions, where one equation...
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Covalent Adaptable Networks Mediated by Redox-Responsive Neighboring-Group-Participating Transalkylation.

Wenyu Dong1, Yuxin Luo1, Junlu Zhang1

  • 1School of Materials Science & Engineering, Beijing Institute of Technology, Beijing, 100081, China.

Angewandte Chemie (International Ed. in English)
|April 17, 2025
PubMed
Summary
This summary is machine-generated.

This study introduces catalyst-free covalent adaptable networks (CANs) using bicyclo[3.3.1]nonane (BCN) crosslinkers and selenium-based neighboring-group-participation (NGP). These dynamic networks offer efficient recycling, repair, and reprocessing with tunable properties.

Keywords:
Covalent adaptable networksDynamic covalent chemistryNeighboring‐group‐participationRedox responsivenessSelenium

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Organic Chemistry

Background:

  • Covalent adaptable networks (CANs) often rely on external catalysts for crosslinker exchange, hindering reprocessability due to catalyst leaching and degradation.
  • Developing catalyst-free dynamic polymer networks is crucial for sustainable materials and advanced applications.

Purpose of the Study:

  • To develop a novel catalyst-free dynamic polymer network system.
  • To investigate the use of selenium-based neighboring-group-participation (NGP) to facilitate efficient crosslinker exchange in CANs.
  • To explore the chemical recyclability, repairability, and tunable dynamic behavior of the developed network.

Main Methods:

  • Employed a bicyclo[3.3.1]nonane (BCN) bis-alkyl halide crosslinker designed to utilize selenium-based NGP.
  • Investigated thermally mediated C─N alkyl exchange for bond dissociation and association.
  • Characterized the flow behavior and dynamic properties of the resulting ionic network.

Main Results:

  • Achieved efficient crosslinker exchange without external catalysts, enabling rapid bond exchange and flow.
  • Demonstrated that the ionic network possesses intrinsic antimicrobial properties.
  • Successfully recycled, repaired, and reprocessed the network under mild conditions.
  • Showcased the ability to regulate network dynamics via the reversible redox responsiveness of selenium atoms.

Conclusions:

  • A novel NGP-based catalyst-free CAN was successfully developed using a BCN crosslinker and selenium.
  • The developed CAN exhibits excellent reprocessability, recyclability, and repairability under mild conditions.
  • The network's dynamic behavior can be modulated through selenium's redox activity, offering potential for high-performance, tunable dynamic materials.