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Selective degradation in aliphatic block copolyesters by controlling the heterogeneity of the amorphous phase
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.ORCID iD: 0000-0002-5850-8873
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology.
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2015 (English)In: Polymer Chemistry, ISSN 1759-9954, E-ISSN 1759-9962, Vol. 6, no 17, 3271-3282 p.Article in journal (Refereed) Published
Abstract [en]

Controlling the course of the degradation of aliphatic polyesters is a key question when designing new degradable materials. It is shown herein that it is possible to predetermine the degradation path of aliphatic block copolyesters by controlling the heterogeneity of the amorphous phase, which in turn regulates the availability of the hydrolyzable groups in the polyester backbone. To demonstrate these processes, we synthesized a set of degradable materials based on poly(l-lactide) (PLLA), poly(ε-decalactone) (PεDL) and poly(ε-caprolactone) (PCL) with varying compositions. The materials were subjected to hydrolysis for a six months period. The materials composed of PLLA and PεDL exhibited a heterogeneous amorphous phase, whereas the materials composed of PCL and PεDL presented a more homogeneous phase. The kinetics of the degradation indicated that the slowest degradation rate was observed for the more homogeneous compositions. The degradation path of the heterogeneous amorphous phase materials was driven by a random chain scission process, whereas the more homogeneous composition presented a degradation path driven by a more selective chain scission. The confinement of the amorphous phase by the more hydrolytically stable PεDL permitted a selective degradation of the available hydrolyzable groups. The random and more selective chain scission processes were further verified by using previously determined molecular modeling based on Monte Carlo procedures. Topographical images and thermal analyses of the materials under different degradation periods correlated with the proposed degradation paths. Detailed insights and the ability to predetermine the degradation pathways of aliphatic polyesters will continue to expand the great potential of renewable materials and their use in specific applications for a future sustainable society.

Place, publisher, year, edition, pages
2015. Vol. 6, no 17, 3271-3282 p.
Keyword [en]
Chains, Degradation, Organic polymers, Polyesters, Thermoanalysis, Aliphatic polyester, Degradation pathways, Homogeneous composition, Monte Carlo procedures, Poly (epsiloncaprolactone), Random chain scissions, Selective degradation, Topographical images, Amorphous materials
National Category
Polymer Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-167775DOI: 10.1039/c5py00136fISI: 000353348700010Scopus ID: 2-s2.0-84928485535OAI: oai:DiVA.org:kth-167775DiVA: diva2:814170
Funder
Swedish Research Council, A0347801EU, European Research Council, 246776
Note

QC 20150526

Available from: 2015-05-26 Created: 2015-05-22 Last updated: 2017-12-04Bibliographically approved
In thesis
1. 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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