Abstract

Novel green classes of biodegradable polylactide-based triblock polyurethane (TBPU) polymers were synthesized. Owing to their tailored mechanical properties, improved degradation rates, and the enhance cell attachment potential compared with polylactide-homopolymer, they tested for biomedical applications. Triblock copolymers (TB) of different lactide and polyethylene glycol composition were first fabricated by ring-opening polymerization using tin octoate as catalyst. Afterwich polycaprolactone diole (PCL-diole) is reacted with TB copolymers using 1,4-butane diisocyanate (BDI) as nontoxic chain extender to form the final TBPUs. Final composition, molecular weight, thermal properties, hydrophilicity and biodegradation of the obtained TB and TBPU were studied and characterized using 1H-NMR, GPC, FTIR, DSC, SEM and contact angle measurements. Results obtained from the high molecular weight members of TBPUs showed improved hydrophilicity and degradation rates along with tailored mechanical properties. Nanocomposites obtained by reinforcing TBPU3 with 7% (w/w) BCNW showed ~16% increase in tensile strength and 330% in % elongation compared with PL-homopolymer. Those polymers and their nanocomposites demonstrated promising potential to be used as bone cement, and in regenerative medicin.

Highlights

  • The triblock polyurethane (TBPU) of low molecular weight can be utilized as drug delivery carriers and implantable membranes where fast degradation and drug stability are required, whereas the TBPUs of higher molecular weights can be used in fabrication of porous scaffold that are used in tissue engineering scaffolds

  • The results showed that the cell attachment efficiency on Multi-PLE 4/1(4/1 refers to the molar ratio of lactidyl units to ethylene oxide units) films was close to that on PLLA film, while the cell proliferation on Multi-PLE4/1 and Multi-PLE2/1 scaffolds was better than that on PLLA scaffold, which was closely related to the improved hydrophilicity of Multi-PLE copolymers due to the incorporation of poly(ethylene glycol) (PEG) in comparison with pure PLLA [76]

  • Results obtained from the mechanical properties study carried out by Qu et al [134] showed that both tensile strength and elongation at break significantly improved and reached a maximum in the composite obtained by blending poly(lactic acid) (PLA)/PEG when cellulose nanofibril of 3% content was added to the blend, and decreased with further increase of cellulose nanofibrils

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Summary

Overview and Background

Biodegradable polymers are used in an increasingly large number of biomedical applications. To overcome the current limitations that confront the use of the previously mentioned biodegradable homopolymers, the current project focus on the synthesis of wide range of molecular weights of green nontoxic biodegradable triblock polyurethanes (TBPUs) that have improved hydrophilicity, degradation rate and cell attachment abilities over the pure homopolymers PLA and PCL Those newly designed polyurethane can be used either for rapid drug delivery system and MRI contrast agent, as well as in tissue engineering scaffolds. The new BCNW/TBPUs nanocomposite will be envisioned, from one side, to show improved interfacial adhesion with the newly generated cells due to the presence of hydrophilic PEG and BCNW in the hydrophobic polymer matrix, and from the other side to improve the mechanical strength and biodegradation rate This project is a multifaceted challenge, since obtaining a new group of materials with a given set of mechanical and physical properties, to be used in biomedical applications, is conditional upon being biocompatible and biodegradable

Problem Statement
Objectives and Specific Aims
Research Plan
Chemical Modification of PLA through Copolymerization with PEG: A Review
Chemical Modification of PLA through Chain Extension/Chain Linker Using Urethane Reactions: A Review
Synthesis of Poly(ester-urethane)
Hydrolytic Degradation of Poly(ester-urethane)
Cellulose Nanowhiskers
Nanocomposites of BCNW with Biodegradable Polymers
Micromechanical
Mechanical Properties of PL Based Poly(ester-urethane)
Mechanical Properties of PL based/cellulose Nanocomposites
Results
Bacterial Strain and Culture Growth Conditions Gluconoacetobacter
Production of BC Nanofibers Bacterial
Purification and Recovery of TB Copolymers
Preparation of Polymer Films
Determination of Degree of Polymerization and Molecular Weight
Biodegradation
3.4.10 Mechanical Testing
Synthesis of Triblock (PL-PEG-PL) and PUs
FTIR-ATR Spectra
C H2 g C H2 O O
Water Absorption and Contact Angle Testing of TB Copolymer and TBPUs
Mechanical Properties of TB and TBPUs
Statistical Analysis and Error Calculations
CHAPTER 5 – CONCLUSION AND FUTURE WORK
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