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Dynamic covalent Diels–Alder chemistry was combined with multiwalled carbon nanotube (CNT) reinforcement to develop strong, tough and conductive dynamic materials. Unlike other approaches to functionalizing CNTs, this approach uses Diels–Alder bonds between diene pendant groups on the polymer and the CNT surface πσ bonds acting as dienophiles. Experimental and simulation data align with the CNT reinforcement coming from dynamic covalent bonds between the matrix and the CNT surface. The addition of just 0.9 wt% CNTs can lead to an almost 3-fold increase in strength and 6–7 order of magnitude increases in electrical conductivity, and materials with 0.45 wt% CNTs show excellent strength, self-healing and conductivity.
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