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Mapping the Mechanical Properties of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Banded Spherulites by Nanoindentation.

ABSTRACT: Nanoindentation provides clear evidence that spherulite banding can be associated with a continuous modulation of mechanical properties from the more compliant peaks to the stiffer valleys. The structural arrangement in polymer-banded spherulites has intrigued scientists for many decades, and the debate has been recently intensified with the advent of new experimental evidence. The present paper approaches this issue by exploring the local mechanical properties of poly(3-hydroxybutyrate-co-3-hydroxyvalerate)-ringed spherulites via nanoindentation and discussing the confidence of the results. It was found that storage modulus and hardness across the banding morphology can be described as a sequence of regular oscillations with a periodicity that exactly matches the one observed using optical and atomic force microscopy. Results are consistent with the model of regular twisting of the lamellae, with flat-on arrangement in the low regions and edge-on lamellae in the crests.

SUBMITTER: Enrique-Jimenez P

PROVIDER: S-EPMC6432475 | biostudies-literature | 2016 Oct

REPOSITORIES: biostudies-literature

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Mapping the Mechanical Properties of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Banded Spherulites by Nanoindentation.

Enrique-Jimenez Patricia P Vega Juan F JF Martínez-Salazar Javier J Ania Fernando F Flores Araceli A

Polymers 20161012 10

Nanoindentation provides clear evidence that spherulite banding can be associated with a continuous modulation of mechanical properties from the more compliant peaks to the stiffer valleys. The structural arrangement in polymer-banded spherulites has intrigued scientists for many decades, and the debate has been recently intensified with the advent of new experimental evidence. The present paper approaches this issue by exploring the local mechanical properties of poly(3-hydroxybutyrate-co-3-hyd ...[more]

PMID: 30974634

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Project description:Poly(hydroxybutyrate-co-hydroxyhexanoate) [P(HB-co-HHx)] and poly(hydroxybutyrate-co-hydroxyvalerate-co-hydroxyhexanoate) [P(HB-co-HV-co-HHx)] demonstrate interesting mechanical and thermal properties as well as excellent biocompatibility, making them suitable for multiple applications and notably biomedical purposes. The production of such polymers was described in Rhodospirillum rubrum, a purple nonsulfur bacteria in a nutrient-lacking environment where the HHx synthesis is triggered by the presence of hexanoate in the medium. However, the production of P(HB-co-HHx) under nutrient-balanced growth conditions in R. rubrum has not been described so far, and the assimilation of hexanoate is poorly documented. In this study, we used proteomic analysis and a mutant fitness assay to demonstrate that hexanoate assimilation involve β-oxidation and the ethylmalonyl-coenzyme A (CoA) (EMC) and methylbutanoyl-CoA (MBC) pathways, both being anaplerotic pathways already described in R. rubrum. Polyhydroxyalkanoate (PHA) production is likely to involve the de novo fatty acid synthesis pathway. Concerning the polymer composition, HB is the main component of the polymer, probably as acetyl-CoA and butyryl-CoA are intermediates of hexanoate assimilation pathways. When no essential nutrient is lacking in the medium, the synthesis of PHA seems to help maintain the redox balance of the cell. In this framework, we showed that the fixation of CO2 is required to sustain the growth. An increase in the proportion of HHx in the polymer was observed when redox stress was engendered in the cell under bicarbonate-limiting growth conditions. The addition of isoleucine or valerate in the medium also increased the HHx content of the polymer and allowed the production of a terpolymer of P(HB-co-HV-co-HHx). IMPORTANCE The use of purple bacteria, which can assimilate volatile fatty acids, for biotechnological applications has increased, since they reduce the production costs of added-value compounds such as PHA. P(HB-co-HHx) and P(HB-co-HV-co-HHx) have demonstrated interesting properties, notably for biomedical applications. In a nutrient-lacking environment, R. rubrum is known to synthesize such polymers when hexanoate is used as the carbon source. However, their production in R. rubrum in non-nutrient-lacking growth conditions has not been described so far, and the assimilation of hexanoate is poorly documented. As the carbon source and its assimilation directly impact the polymer composition, we studied under non-nutrient-lacking growth conditions the assimilation pathway of hexanoate and PHA production in R. rubrum. Proteomic analysis and mutant fitness assays allowed us to explain PHA production and composition. An increase in HHx content of the polymer and production of P(HB-co-HV-co-HHx) was possible using the knowledge gained on metabolism under hexanoate growth conditions.

Dataset Information

Mapping the Mechanical Properties of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Banded Spherulites by Nanoindentation.

Publications

Mapping the Mechanical Properties of Poly(3-hydroxybutyrate-co-3-hydroxyvalerate) Banded Spherulites by Nanoindentation.

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