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  1. Free, publicly-accessible full text available July 1, 2024
  2. Integration of multiple types of dynamic linkages into one polymer network is challenging and not well understood especially in the design and fabrication of dynamic polymer nanocomposites (DPNs). In this contribution, we present facile methods for synthesizing flexible, healable, conductive, and recyclable thermoresponsive DPNs using three dynamic chemistries playing distinct roles. Dynamic hydrogen bonds account for material flexibility and recycling character. Thiol-Michael exchange accounts for thermoresponsive properties. Diels–Alder reaction leads to covalent bonding between polymer matrix and nanocomposite. Overall, the presence of multiple types of orthogonal dynamic bonds provided a solution to the trade-off between enhanced mechanical performance and material elongation in DPNs. Efficient reinforcement was achieved using <1 wt % multiwalled carbon nanotubes as nanocomposite. Resulting DPNs showed excellent healability with over 3 MPa increase in stress compared to unreinforced materials. Due to multiple responsive dynamic linkages, >90% stress–relaxation was observed with self-healing achieved within 1 h of healing time. Increased mechanical strength, electrical conductivity, and reprocessability were achieved all while maintaining material flexibility and extensibility, hence highlighting the strong promise of these DPNs in the rapidly growing fields of flexible compliant electrodes and strain sensors. 
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  3. The choice of chain transfer agent in reversible addition/fragmentation chain transfer polymerization has proven to be instrumental in modulating the dispersity of a certain polyphenyl vinyl ketone (PVK). The monomer, PVK, which can self-initiate when exposed to blue light, was used to synthesize homopolymers, block copolymers by extending with a different monomer and gradient polymers. Regardless of the polymer architecture or degree of polymerization, a consistent trend in polymer dispersity was quantified, with higher loadings of the less active chain transfer agent xanthate leading to higher dispersities. The dispersity could be further modulated by photodegradation of vinyl ketone polymers under UV irradiation. 
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