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Synthesis, characterization and 3D printing of linear and star-shaped poly(propylene fumarate) for medical applications

Luo, Yuanyuan
http://orcid.org/0000-0002-3256-229X
http://rave.ohiolink.edu/etdc/view?acc_num=akron156420129168176

Abstract Details

2019, Doctor of Philosophy, University of Akron, Polymer Science.
Advancements in additive manufacturing, or more commonly known as 3D printing techniques, and the development in synthetic polymers are enabling the fabrication of patient-matched medical devices. These are especially thriving in the regenerative medicine field where products with complex shapes are involved, such as cranial facial bone defect repair. However, before the release of such medical devices on market, they must be cleared by the Food and Drug Administration (FDA). The consistency of the starting material and final product built from 3D printing was incorporated into FDA’s concern to guarantee the safety and effectiveness of a medical device. Such material consistency requires material specifications, which usually depends on the type of materials and 3D printing techniques. For the example of polymers, the purity, molecular weight, molecular mass distribution (Dm), glass transition temperature properties are generally required. The failing to reliably and reproducibly produce a material may cause final device failure in tests like mechanical, biocompatible and/or pre-clinical animal studies, let alone to pass FDA regulations. Poly(propylene fumarate) (PPF) is a non-toxic, amorphous, degradable, crosslinkable polyester, with tunable mechanical and degradation properties for regenerative medicines. However, previous academic researchers reported some limitations of using 3D printed PPF for medical applications and research on these polymers had stopped at the stage of small animal studies. The drawbacks mainly came from unreliable molecular properties (e.g., Dm>2) and low yield (e.g., 35%) from traditional synthetic methods. Herein, a reaction system was developed as shown in this dissertation to generate PPF from ring-opening copolymerization (ROCOP) of maleic anhydride and propylene oxide followed by a base catalyzed isomerization reaction. Then a continuous improvement in the yield (e.g., 65%-90%), a more reproducible synthesis (up to 1kg/batch), a better control over the molecular mass distribution (e.g., 1.1-1.6) of PPF with various functionalities were achieved. The following sections start with the story of the first attempt to synthesize 3D printable PPF using a ROCOP method with detailed chemical and physical characterizations on these PPF materials (Chapter III). Then, the viscosity evaluations and 3D printing of these PPF based resins were further explored, followed by mechanical tests (Chapter IV). These results demonstrated the potential of using such PPF-based materials in high resolution 3D printing techniques, such as continuous digital light processing (cDLP) for bone repair applications. The most recent innovation in synthesis of star-shaped PPF made it possible to efficiently obtain higher molecular mass PPF, which also showed lower viscosity than their linear analogues. These significant improvements in star-shaped PPF over linear PPF analogs from synthetic speed, viscosity for 3D printing to mechanical properties were later disclosed (Chapter V). Currently, 3D printing of ROCOP synthesized PPF-based degradable resins with less solvent input, available functionalities for biological cues are possible, bringing a relatively wide range of mechanical and degradation properties of printed products. This work has been a preliminary study that has helped to gradually improve PPF properties to aid in 3D printing for patient and defect-matched regenerative medicine.
Matthew Becker (Advisor)
Bryan Vogt (Committee Member)
Eric Amis (Committee Member)
Toshikazu Miyoshi (Committee Member)
Chrys Wesdemiotis (Committee Member)
184 p.
Polymer Chemistry; Polymers

Recommended Citations

Citations

  • Luo, Y. (2019). Synthesis, characterization and 3D printing of linear and star-shaped poly(propylene fumarate) for medical applications [Doctoral dissertation, University of Akron]. OhioLINK Electronic Theses and Dissertations Center. http://rave.ohiolink.edu/etdc/view?acc_num=akron156420129168176

    APA Style (7th edition)

  • Luo, Yuanyuan. Synthesis, characterization and 3D printing of linear and star-shaped poly(propylene fumarate) for medical applications . 2019. University of Akron, Doctoral dissertation. OhioLINK Electronic Theses and Dissertations Center, http://rave.ohiolink.edu/etdc/view?acc_num=akron156420129168176.

    MLA Style (8th edition)

  • Luo, Yuanyuan. "Synthesis, characterization and 3D printing of linear and star-shaped poly(propylene fumarate) for medical applications ." Doctoral dissertation, University of Akron, 2019. http://rave.ohiolink.edu/etdc/view?acc_num=akron156420129168176

    Chicago Manual of Style (17th edition)

akron156420129168176
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© 2019, all rights reserved.
This open access ETD is published by University of Akron and OhioLINK.