Synthesis of poly(lactic acid) multiblock copolymers with improved properties using 3-hydroxybutyrate diol

Yoshida, Konosuke; Hsu, Yu I.; Sugimoto, Masayuki et al.

Polymer Degradation and Stability, 2025, 241, 111570

Number of Access:31（2025-10-28 06:13 Counts）

Identifier to cite or link to this item: https://hdl.handle.net/11094/102779

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Title
Synthesis of poly(lactic acid) multiblock copolymers with improved properties using 3-hydroxybutyrate diol
Creator
CreatorName
Yoshida, Konosuke
NRID
1000010757678 1000010757678
ORCID
0000-0002-4533-7200 0000-0002-4533-7200
researchmap permalink
yuihsu yuihsu
Scopus Author ID
55389981500 55389981500
CreatorName
Hsu, Yu I.
CreatorName
Sugimoto, Masayuki
NRID
1000070203594 1000070203594
ORCID
0000-0002-8587-2507 0000-0002-8587-2507
researchmap permalink
read0168389 read0168389
Scopus Author ID
7102108908 7102108908
CreatorName
Uyama, Hiroshi
Subject
(R)-3-Hydroxybutyrate (3HB) diol
Biodegradable polymer
Copolymer
Enzymatic degradation
Poly(lactic acid) (PLA)
Structure-property relationship
Description
Yoshida K., Hsu Y.I., Sugimoto M., et al. Synthesis of poly(lactic acid) multiblock copolymers with improved properties using 3-hydroxybutyrate diol. Polymer Degradation and Stability 241, 111570 (2025); https://doi.org/10.1016/j.polymdegradstab.2025.111570.
Abstract
The increasing accumulation of persistent plastic waste in terrestrial and marine environments has heightened the demand for high-performance, biodegradable alternatives. Poly(lactic acid) (PLA) is a widely used renewable polyester, yet its intrinsic brittleness and limited degradability under ambient conditions continue to impede broader application. In this work, a fully synthetic strategy was developed to address these limitations through the design of (R)-3-hydroxybutyrate (3HB)-Poly(lactic acid) (PLA) multiblock copolymers incorporating structurally tailored 3HB diols. Structurally distinct 3HB diols were synthesized via nucleophilic substitution between chemically derived 3HB and either a linear dihalide or a cyclic ditosylated compound, yielding diols in which two 3HB units are connected by a linear or cyclic linker. These diols were subsequently copolymerized with L-lactide via ring-opening polymerization, followed by chain extension using hexamethylene diisocyanate (HDI) to obtain alternating multiblock copolymers. The resulting materials exhibited significantly enhanced mechanical properties, with linear 3HB diols notably improving toughness and elongation at break. Differential scanning calorimetry revealed that 3HB incorporation reduced the glass transition temperature, while variation in PLA segment length modulated crystallinity. Enzymatic degradation assays showed substantially faster degradation rates compared to neat PLA, confirming improved biodegradability. These results demonstrate that incorporating chemically modified 3HB diols into PLA enables concurrent enhancement of mechanical performance and environmental biodegradability. Furthermore, the tunability of material properties through control of 3HB architecture and PLA segment length highlights the versatility of this copolymer design strategy for developing sustainable polymer systems.
Publisher
Elsevier Ltd
Source Title
Polymer Degradation and Stability
Volume (Issue)
241
Page
111570
Date of Issued
2025-11-01
Language
English
Handle URL
https://hdl.handle.net/11094/102779
PISSN
01413910
Relation.isIdenticalTo
DOI (Publisher Version)
https://doi.org/10.1016/j.polymdegradstab.2025.111570
Access Rights
open access
CopyRight
This article is licensed under a Creative Commons Attribution-NonCommercial-NoDerivatives 4.0 International License.
© 2025 The Authors
oaire:version
Version of Record
Category
学術雑誌論文 Journal Article