Synergistic electronic-topological strategy enables spatiotemporal control of covalent adaptable networks

Covalent adaptable networks (CANs) hold considerable promise for combining the advantages of thermosets and thermoplastics. However, their use in high-speed melt spinning is restricted by insufficient dynamic bond reactivity at processing temperatures and the mismatch between network rearrangement kinetics and industrial requirements. Here, we establish a spatiotemporally regulated platform based on internally catalyzed oxime-urethane chemistry within a four-arm cross-linking topology. Neighboring urea groups provide internal catalysis that greatly accelerates oxime-urethane dissociation at 110°C, improving melt fluidity. During extrusion, the slight temperature drop rapidly drives bond recombination within…

• NN
  National Natural Science Foundation of China

  Awards: 52173117, 52203169, 52403163, U25A20251, 52473004
• SA
  Science and Technology Commission of Shanghai Municipality

  Awards: 20DZ2270800, 20DZ2254900
• SP
  Shanghai Pulmonary Hospital
• BA
  Basic and Applied Basic Research Foundation of Guangdong Province

  Award: 2023A1515110778