In situ development of self-reinforced cellulose nanocrystals based thermoplastic elastomers by atom transfer radical polymerization

• Self-reinforced cellulose nanocrystals based thermoplastic elastomers (CTPEs) were developed.
• The compatibility between cellulose nanocrystals and thermoplastic elastomers was improved.
• Tensile strength and elastic recovery of CTPEs were improved.

Recently, the utilization of cellulose nanocrystals (CNCs) as a reinforcing material has received a great attention due to its high elastic modulus. In this article, a novel strategy for the synthesis of self-reinforced CNCs based thermoplastic elastomers (CTPEs) is presented. CNCs were first surface functionalized with an initiator for surface-initiated atom transfer radical polymerization (SI-ATRP). Subsequently, SI-ATRP of methyl methacrylate (MMA) and butyl acrylate (BA) was carried out in the presence of sacrificial initiator to form CTPEs in situ. The CTPEs together with the simple blends of CNCs and linear poly(MMA-co-BA) copolymer (P(MMA-co-BA)) were characterized for comparative study. The results indicated that P(MMA-co-BA) was successfully grafted onto the surface of CNCs and the compatibility between CNCs and the polymer matrix in CTPEs was greatly enhanced. Specially, the CTPEs containing 2.15 wt% CNCs increased Tg by 19.2 °C and tensile strength by 100% as compared to the linear P(MMA-co-BA).

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