Carbohydrates as Hard Segments for Sustainable Elastomers:
Carbohydrates Direct the Self-Assembly and Mechanical Properties of
Fully Bio-Based Block Copolymers
Posted on 2020-06-16 - 13:34
A series of fully bio-based block
copolymers (BCPs) consisting
of maltooligosaccharides (maltose, maltotriose, maltotetraose, and
maltohexaose; A block) and poly(δ-decanolactone) (PDL; B block),
with ABA-, A2BA2-, A3BA3-, A(BA)2-, and A2(BA)2-type architectures,
were synthesized to demonstrate the potential of oligosaccharides
as novel hard segments for bio-based elastomers. To understand the
correlation between the BCP molecular structure and material properties,
the BCPs were designed to have comparable molecular weights (ca. 12K)
and total numbers of glucose units (12). Morphological analysis revealed
the formation of body-centered-cubic sphere and hexagonally close-packed
cylinder (HEX) morphologies depending on the branched architecture
(interdomain distance 9.7–14.4 nm). While the PDL homopolymer
is a viscous liquid due to its low Tg and
amorphous nature, all BCPs exhibited elastomeric properties, confirming
that the oligosaccharide blocks segregated to form the hard domains
to cross-link the rubbery PDL chains. Tensile testing revealed that
the mechanical properties of the BCPs were mainly determined by the
microphase-separated structure and less affected by the length of
each oligosaccharide chain. The HEX-forming A2BA2- and A3BA3-type BCPs exhibited Young’s
moduli of ∼6 MPa, which is comparable to well-known styrene-based
thermoplastic elastomers. Furthermore, a readily available polydisperse
maltooligosaccharide was employed to synthesize an A2BA2-type BCP with a higher molecular weight PDL block (20K),
which exhibited a Young’s modulus of ∼6 MPa and an elongation
at break of ∼700%. These results demonstrate that oligosaccharides
are a sustainable alternative to the petroleum-derived synthetic hard
segments (e.g., polystyrene), thereby opening up a new avenue for
fully bio-based soft material design.
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Isono, Takuya; Nakahira, Saki; Hsieh, Hui-Ching; Katsuhara, Satoshi; Mamiya, Hiroaki; Yamamoto, Takuya; et al. (2020). Carbohydrates as Hard Segments for Sustainable Elastomers:
Carbohydrates Direct the Self-Assembly and Mechanical Properties of
Fully Bio-Based Block Copolymers. ACS Publications. Collection. https://doi.org/10.1021/acs.macromol.0c00611