Abstract

AbstractNatural rubber is one of most famous self‐reinforced rubbers thanks to the phenomenon of strain‐induced crystallization. It is usually used in a vulcanized form to enhance the mechanical strength but this results in recycling issues. Herein a thermoplastic analogue of vulcanized natural rubber is obtained as a structural mimic. Terminally functionalized polyisoprene rubber B‐4A‐PIP was prepared by using tetra‐analine as physical crosslinking units. The strong binding of tetra‐analine groups gave B‐4A‐PIP a high tensile strength (15 MPa) and breaking strain of 890 %, which is much higher than those of undecorated copolymer B‐OH‐PIP. B‐4A‐PIP has a similar onset strain of crystallization and crystallization index to vulcanized natural rubber. Randomly functionalized polyisoprene R‐4A‐PIP showed a much lower mechanical strength and SIC properties although R‐4A‐PIP and B‐4A‐PIP possessed similar molecular weights and amounts of tetra‐analine groups.

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