Approximately 4.8–12.7 million tons of plastic waste has been estimated to be discharged into marine environments annually by wind and river currents. The Ellen MacArthur Foundation warns that the total weight of plastic waste in the oceans will exceed the total weight of fish in 2050 if the environmental runoff of plastic continues at the current rate. Hence, biodegradable plastics are attracting attention as a solution to the problems caused by plastic waste. Among biodegradable plastics, polyhydroxyalkanoates (PHAs) and poly(ε-caprolactone) (PCL) are particularly noteworthy because of their excellent marine biodegradability. In this review, the biosynthesis of PHA and cutin, a natural analog of PCL, and the biodegradation of PHA and PCL in carbon cycles in marine ecosystems are discussed. PHA is biosynthesized and biodegraded by various marine microbes in a wide range of marine environments, including coastal, shallow-water, and deep-sea environments. Marine cutin is biosynthesized by marine plants or obtained from terrestrial environments, and PCL and cutin are biodegraded by cutin hydrolytic enzyme-producing microbes in broad marine environments. Thus, biological carbon cycles for PHA and PCL exist in the marine environment, which would allow materials made of PHA and PCL to be quickly mineralized in marine environments.
Exploiting biomass as an alternative to petrochemicals for the production of commodity plastics is vitally important if we are to become a more sustainable society. Here, we report a synthetic route for the production of terephthalic acid (TPA), the monomer of the widely used thermoplastic polymer poly(ethylene terephthalate) (PET), from the biomass-derived starting material furfural. Biobased furfural was oxidised and dehydrated to give maleic anhydride, which was further reacted with biobased furan to give its Diels-Alder (DA) adduct. The dehydration of the DA adduct gave phthalic anhydride, which was converted via phthalic acid and dipotassium phthalate to TPA. The biobased carbon content of the TPA was measured by accelerator mass spectroscopy and the TPA was found to be made of 100% biobased carbon.
Poly(3-hydoxybutyrate-co-4-hydroxybutyrate) [P(3HB-co-4HB)] was biosynthesized by Comamonas acidovorans with mixed carbon sources of n-butyric acid and 1,4-butanediol. P(3HB) and P(3HB-co-94 mol% 4HB) were obtained by fermentation with sole carbon source of n-butyric acid and 1,4-butanediol, respectively. The content of 4HB component in P(3HB-co-4HB) increased as the composition of 1,4-butanediol in mixed carbon sources increased. These biosynthesized copolymers are not homogeneous, but mixtures of copolymers having different 4HB contents. Fractionation was carried out to obtain fractionated copolymers having a narrower distribution of composition. The change in structural and physical properties of the fractionated copolymers were investigated against the 4HB contents. Crystallinities of P(3HB-co-4HB)s were estimated using density values and the heat of fusion of P(3HB) measured was 125 J g 21 and that of P(4HB) was 76 J g 21 . q
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