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Thermoplastic elastomers (TPEs) derived from sustainable cellulose and its derivatives have attracted a great deal of attention, because of their abundance, renewable nature, rigid backbone and good mechanical properties. To fabricate TPEs with tunable performance, a series of sustainable ethyl cellulose (EC)-grafted poly(methyl methacrylate (MMA)) (EC-g-P(MMA)) and poly(MMA-co-butyl methacrylate (BMA)) (EC-g-P(MMA-co-BMA)) were fabricated by way of atom-transfer radical polymerization (ATRP). By tuning the molar ratio of MMA/BMA in the copolymer side chains, tunable performance of TPEs with tunable glass transition temperatures (118–47.8°C) was achieved. The chemical structures of EC-bromide and EC graft copolymers were identifiable by Fourier transform infrared spectroscopy and hydrogen-1 (1H) nuclear magnetic resonance spectroscopy. The EC graft copolymers exhibited a higher molecular weight and good thermal stability and mechanical properties. These results suggested that these tunable-performance copolymers with a sustainable cellulose backbone and an acrylate side chain were potential candidates for service as TPEs in some applications.

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