Waste rubber tires are an area of global concern in relation to reducing the consumption of petrochemical products and environmental pollution. Herein, eco-friendly high-performance thermoplastic polyurethane (PU) elastomers were successfully in-situ synthesized through the incorporation of ground tire rubber (GTR). The excellent wet-skid resistance of PU/GTR elastomer was achieved by using mixed polycaprolactone polyols with Mn = 1000 g/mol (PCL-1K) and PCL-2K as soft segments. More importantly, an efficient solution to balance the contradiction between dynamic heat build-up and wet-skid resistance in PU/GTR elastomers was that low heat build-up was realized through the limited friction between PU molecular chains, which was achieved with the help of the network structure formed from GTR particles uniformly distributed in the PU matrix. Impressively, the tanδ at 60 °C and the DIN abrasion volume (Δrel) of the optimal PU/GTR elastomer with 59.5% of PCL-1K and 5.0% of GTR were 0.03 and 38.5 mm3, respectively, which are significantly lower than the 0.12 and 158.32 mm3 for pure PU elastomer, indicating that the PU/GTR elastomer possesses extremely low rolling resistance and excellent wear resistance. Meanwhile, the tanδ at 0 °C of the above-mentioned PU/GTR elastomer was 0.92, which is higher than the 0.80 of pure PU elastomer, evidencing the high wet-skid resistance. To some extent, the as-prepared PU/GTR elastomer has effectively solved the "magic triangle" problem in the tire industry. Moreover, this novel research will be expected to make contributions in the upcycling of waste tires.
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