Abstract
The development of biodegradable and recyclable polymers having the desired material properties required in practical use has provided a partial solution for realizing a sustainable plastics economy. Naturally produced commercial poly(3-hydroxybutyrate) (P3HB), one of the much studied biodegradable polyhydroxyalkanoates (PHAs), is a stereoregular thermoplastic material with a high degree of crystallinity, significantly restricting its application due to the stiff and brittle characteristics. Therefore, it is of great significance to overcome the inherent brittleness through decreasing the crystallinity of P3HB. In this contribution, we present a powerful strategy to toughen P3HB via catalytic carbonylative terpolymerization of enantiopure epoxides with different long alkyl side chains and configurations using a binary trimetallic CrIII complex/carbonyl cobalt catalyst system. The structure and stereochemistry of epoxides significantly impact the properties of the resultant PHA copolymers, which spans from viscous oil to tough/ductile and brittle plastics. This study represents a rather rare example of a method to toughen the extensively studied P3HB with epoxide and CO as raw materials.
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