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Tuning the Degradation Profiles of Poly(L-lactide)-Based Materials through Miscibility
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.ORCID iD: 0000-0002-5850-8873
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology.
2014 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 15, no 1, 391-402 p.Article in journal (Refereed) Published
Abstract [en]

The effective use of biodegradable polymers relies on the ability to control the onset of and time needed for degradation. Preferably, the material properties should be retained throughout the intended time frame, and the material should degrade in a rapid and controlled manner afterward. The degradation profiles of polyester materials were controlled through their miscibility. Systems composed of PLLA blended with poly[(R,S)-3-hydroxybutyrate] (a-PHB) and polypropylene adipate (PPA) with various molar masses were prepared through extrusion. Three different systems were used: miscible (PLLA/a-PHB5 and PLLA/a-PHB20), partially miscible (PLLA/PPA5/comp and PLLA/PPA20/comp), and immiscible (PLLA/PPA5 and PLLA/PPA20) blends. These blends and their respective homopolymers were hydrolytically degraded in water at 37 degrees C for up to I year. The blends exhibited entirely different degradation profiles but showed no diversity between the total degradation times of the materials. PLLA presented a two-stage degradation profile with a rapid decrease in molar mass during the early stages of degradation, similar to the profile of PLLA/a-PHB5. PLLA/a-PHB20 presented a single, constant linear degradation profile. PLLA/PPA5 and PLLA/PPA20 showed completely opposing degradation profiles relative to PLLA, exhibiting a slow initial phase and a rapid decrease after a prolonged degradation time. PLLA/PPA5/comp and PLLA/PPA20/comp had degradation profiles between those of the miscible and the immiscible blends. The molar masses of the materials were approximately the same after 1 year of degradation despite their different profiles. The blend composition and topographical images captured at the last degradation time point demonstrate that the blending component was not leached out during the period of study. The hydrolytic stability of degradable polyester materials can be tailored to obtain different and predetermined degradation profiles for future applications.

Place, publisher, year, edition, pages
2014. Vol. 15, no 1, 391-402 p.
Keyword [en]
Hydrolytic Degradation, Atactic Poly(3-Hydroxybutyrate), Mechanical-Properties, Enzymatic Degradation, Aliphatic Polyesters, Poly(Dl-Lactic Acid), Poly(Lactic Acid), Phase-Structure, Blends, Polylactide
National Category
Biochemistry and Molecular Biology Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-141304DOI: 10.1021/bm401667bISI: 000329879800042Scopus ID: 2-s2.0-84892601347OAI: oai:DiVA.org:kth-141304DiVA: diva2:696485
Funder
Swedish Research Council, A0347801EU, European Research Council, 246776
Note

QC 20140214

Available from: 2014-02-14 Created: 2014-02-13 Last updated: 2017-12-06Bibliographically approved
In thesis
1. Macrostructural Design of Polylactide-based Materials for Improved Mechanical and Degradation Properties
Open this publication in new window or tab >>Macrostructural Design of Polylactide-based Materials for Improved Mechanical and Degradation Properties
2014 (English)Licentiate thesis, comprehensive summary (Other academic)
Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2014. 52 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2014:6
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-143542 (URN)978-91-7595-034-1 (ISBN)
Presentation
2014-04-04, K2, Teknikringen 28, Stockholm, 10:00 (English)
Opponent
Supervisors
Note

QC 20140324

Available from: 2014-03-24 Created: 2014-03-24 Last updated: 2014-03-24Bibliographically approved
2. Towards a retro-structural design of degradable aliphatic polyester-based materials
Open this publication in new window or tab >>Towards a retro-structural design of degradable aliphatic polyester-based materials
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The increasing amount of accumulated plastic waste has led to a continuous search for degradable materials for use in a variety of applications. This eco-friendly approach contemplates the use of degradable alternatives to the inert polymers (the main components in plastics) used today and further engineering of their degradation pathways. The most extensively investigated group of degradable polymers is the poly(α-esters), due to their tailorable thermo-mechanical properties and degradability. However, degradation of these polymers can be undesirable or desirable depending on the time of occurrence. Thus, by controlling the degradation process, it is possible to predict and, consequently, tailor the materials’ lifetime for specific needs.Herein, a methodology to allow for a retro-structural design of degradable materials based on aliphatic polyesters is presented. Insights into the degradation behavior of the systems were obtained and further translated to different levels of structural designs to achieve desired macroscopic properties in terms of performance and degradability. Several combinational strategies based on polymer morphology, polymer structure and block design, were developed. As a result, homopolymers and block copolymers with projected degradation for different instances were created. Apart from bulk modifications in the material, it was shown that it was possible to tailor degradation pathways by means of specific interactions between polymer pairs in block copolymers and also in polymer blends. Furthermore, well-defined structure-property relationships are crucial when designing materials with specific degradability properties. In light of this, degradable polyester-based particles with tunable crystalline structures and, hence, physical properties, were developed. These particles proved to function as reinforcing agents in the creation of “green” homocomposites. These composites are promising alternatives in the search for materials that are completely degradable and sustainable.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. 95 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:62
Keyword
Hydrolysis, polyesters, polylactide, hydrophobicity, crystallinity, miscibility, nanoparticles, stereocomplex, homocomposites
National Category
Polymer Chemistry
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-177187 (URN)978-91-7595-748-7 (ISBN)
Public defence
2015-12-11, Kollegiesalen, Brinellvägen 2, KTH, Stockholm, 13:30 (English)
Opponent
Supervisors
Note

QC 20151117

Available from: 2015-11-17 Created: 2015-11-17 Last updated: 2015-11-17Bibliographically approved

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