Recently, high-performance self-healing electromagnetic interference (EMI) shielding materials with superior electrical conductivity, excellent shielding efficiency, and effective selfrepairing ability have gained great attention. However, the practical development of such systems still encounters considerable challenges. In this study, a highly efficient EMI shielding selfhealing nanocomposite system composed of multiple components of multiwalled carbon nanotubes (MWCNTs), graphene nanosheets (GNSs), and Fe 3 O 4 nanoparticles was developed by integrating a novel amphiphilic poly(ethylene glycol)-block-poly-(caprolactone-co-furfuryl glycidyl ether) block copolymer (PEG-b-PCLF) with 1,1′-(methylenedi-4,1-phenylene)bismaleimide and nanofillers via Diels−Alder (DA) chemistry and molecular affinity. Within this composite system, MWCNTs were distributed within the GNSs and served as connecting bridges across adjacent GNSs. Simultaneously, Fe 3 O 4 nanoparticles were uniformly interspersed in the space around the MWCNT/GNS staggered framework due to good affinity with the hydrophilic PEG block, thereby forming MWCNT/GNS/Fe 3 O 4 tricontinuous networks. Upon heating, the retro-DA mechanisms endowed the material system with excellent reprocessability and self-repairability. More importantly, the MWCNT/GNS/Fe 3 O 4 tricontinuous networks not only provided efficient channels for charge transport but also served as an electromagnetic framework that synergistically endowed the material system with excellent EMI shielding properties. Accordingly, a favorable electrical conductivity of 18.5 S m −1 and an extremely high shielding effectiveness of 92.7 dB in the X-band were achieved. Additionally, the material system also possessed sufficient performances in the recovery of mechanical properties and shielding efficiency after repair, thereby leading to a prolonged service life. This study offers a promising strategy for the effective integration of multiple electromagnetic nanofillers into a self-healing polymeric system, which leads to highly efficient electrical and EMI shielding properties as well as remarkable self-repairability. We believe that these results can guide the development of advanced, durable EMI shielding applications.
In this study, a novel self-healing material with a dual-network composed of cross-linked structure by Diels–Alder (DA) chemistry interconnected with self-assembled π-conjugated polymer nanofibrils was developed for application in electromagnetic...
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