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Synthesis and Structure–Property Relationships of PLLA-Based ABA Triblock Copolymers with Bio-Based Soft Segments.

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Title: Synthesis and Structure–Property Relationships of PLLA-Based ABA Triblock Copolymers with Bio-Based Soft Segments.
Authors: Ristić, Ivan1 (AUTHOR) vesnateofilovic@uns.ac.rs, Krstić, Marija1,2 (AUTHOR) tamara.erceg@uns.ac.rs, Cakić, Suzana2,3 (AUTHOR), Nikolić, Ljubiša1,2 (AUTHOR), Teofilović, Vesna1,2 (AUTHOR), Erceg, Tamara1,3 (AUTHOR), Mićić, Vladan3 (AUTHOR)
Source: Polymers (20734360). Feb2026, Vol. 18 Issue 4, p428. 21p.
Subjects: Block copolymers, Phase separation, Thermophysical properties, Ring-opening polymerization, Polymers, Biodegradable plastics
Abstract: The development of biodegradable ABA-type triblock copolymers with tailored thermo-mechanical performance requires precise control over polymer architecture and phase behavior. In this study, PLLA-based ABA triblock copolymers were synthesized using two structurally distinct, fully bio-based soft segments: poly(methyl ricinoleate) (PMR) and poly(1,3-propanediol) (PPD). To the best of our knowledge, this is the first report on PLLA triblock copolymers incorporating PMR as a renewable soft middle block. Hydroxyl-terminated PMR and PPD were employed as macroinitiators for the controlled ring-opening polymerization of L-lactide, enabling systematic variation in block composition and molecular weight. Structural characterization confirmed successful block formation, while thermal and mechanical analyses revealed pronounced differences in phase separation and structure–property relationships. Copolymers containing PMR exhibited enhanced phase separation, increased crystallinity of PLLA domains, and significantly improved elongation at break, attributed to the presence of pendant chains in the soft segment. In contrast, PPD-based copolymers showed reduced phase separation and more PLA-like mechanical behavior. These results demonstrate that the chemical architecture of bio-based soft segments plays a decisive role in governing the thermo-mechanical performance of PLLA-based triblock copolymers. [ABSTRACT FROM AUTHOR]
Copyright of Polymers (20734360) is the property of MDPI and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Synthesis and Structure–Property Relationships of PLLA-Based ABA Triblock Copolymers with Bio-Based Soft Segments.
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  Data: <searchLink fieldCode="AR" term="%22Ristić%2C+Ivan%22">Ristić, Ivan</searchLink><relatesTo>1</relatesTo> (AUTHOR)<i> vesnateofilovic@uns.ac.rs</i><br /><searchLink fieldCode="AR" term="%22Krstić%2C+Marija%22">Krstić, Marija</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<i> tamara.erceg@uns.ac.rs</i><br /><searchLink fieldCode="AR" term="%22Cakić%2C+Suzana%22">Cakić, Suzana</searchLink><relatesTo>2,3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Nikolić%2C+Ljubiša%22">Nikolić, Ljubiša</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Teofilović%2C+Vesna%22">Teofilović, Vesna</searchLink><relatesTo>1,2</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Erceg%2C+Tamara%22">Erceg, Tamara</searchLink><relatesTo>1,3</relatesTo> (AUTHOR)<br /><searchLink fieldCode="AR" term="%22Mićić%2C+Vladan%22">Mićić, Vladan</searchLink><relatesTo>3</relatesTo> (AUTHOR)
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  Data: <searchLink fieldCode="JN" term="%22Polymers+%2820734360%29%22">Polymers (20734360)</searchLink>. Feb2026, Vol. 18 Issue 4, p428. 21p.
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  Data: <searchLink fieldCode="DE" term="%22Block+copolymers%22">Block copolymers</searchLink><br /><searchLink fieldCode="DE" term="%22Phase+separation%22">Phase separation</searchLink><br /><searchLink fieldCode="DE" term="%22Thermophysical+properties%22">Thermophysical properties</searchLink><br /><searchLink fieldCode="DE" term="%22Ring-opening+polymerization%22">Ring-opening polymerization</searchLink><br /><searchLink fieldCode="DE" term="%22Polymers%22">Polymers</searchLink><br /><searchLink fieldCode="DE" term="%22Biodegradable+plastics%22">Biodegradable plastics</searchLink>
– Name: Abstract
  Label: Abstract
  Group: Ab
  Data: The development of biodegradable ABA-type triblock copolymers with tailored thermo-mechanical performance requires precise control over polymer architecture and phase behavior. In this study, PLLA-based ABA triblock copolymers were synthesized using two structurally distinct, fully bio-based soft segments: poly(methyl ricinoleate) (PMR) and poly(1,3-propanediol) (PPD). To the best of our knowledge, this is the first report on PLLA triblock copolymers incorporating PMR as a renewable soft middle block. Hydroxyl-terminated PMR and PPD were employed as macroinitiators for the controlled ring-opening polymerization of L-lactide, enabling systematic variation in block composition and molecular weight. Structural characterization confirmed successful block formation, while thermal and mechanical analyses revealed pronounced differences in phase separation and structure–property relationships. Copolymers containing PMR exhibited enhanced phase separation, increased crystallinity of PLLA domains, and significantly improved elongation at break, attributed to the presence of pendant chains in the soft segment. In contrast, PPD-based copolymers showed reduced phase separation and more PLA-like mechanical behavior. These results demonstrate that the chemical architecture of bio-based soft segments plays a decisive role in governing the thermo-mechanical performance of PLLA-based triblock copolymers. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Polymers (20734360) is the property of MDPI and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.3390/polym18040428
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        Text: English
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      – SubjectFull: Phase separation
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      – SubjectFull: Thermophysical properties
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      – TitleFull: Synthesis and Structure–Property Relationships of PLLA-Based ABA Triblock Copolymers with Bio-Based Soft Segments.
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              M: 02
              Text: Feb2026
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              Y: 2026
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