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Tunable thermal characteristics of biodegradable copolymer inks for additive manufacturing of implantable therapeutic depots

  • 정윤근 (Jeong Yun Geun, 아주대학교 일반대학원)

초록/요약

A significant challenge impeding the widespread use of three-dimensional (3D) printing for personalized drug delivery is the scarcity of polymers that offer both low-temperature processability and adjustable biodegradation rates. This research addresses this gap by detailing the systematic development, synthesis, and evaluation of a series of poly(ε-caprolactone-ran-lactide) (CL) copolymer inks. By strategically varying the molar percentage of poly(lactide) (PLA) from 1 % to 20 % within the poly(ε-caprolactone) structure, we successfully tailored the we successfully engineered the material's thermomechanical properties. This modification was essential to meet the distinct criteria required for the 3D printing process and for stable performance in a biological environment. Analysis via differential scanning calorimetry verified a direct correlation: a higher proportion of PLA resulted in a systematic decrease of the melting point, dropping from 57 °C to 40 °C. This ability to tune the thermal behavior was critical for optimizing printability and ensuring the structural integrity of the final depot. Rheological and printing tests, performed under fine-tuned conditions, confirmed the material's superior filament consistency and layer-by-layer fabrication fidelity. Based on their thermal stability above 40 °C, the CL1–CL3 variants were chosen for in-depth analysis. To validate their therapeutic potential, these polymers were used to fabricate dexamethasone-loaded depots (DCL). These depots demonstrated high drug encapsulation efficiencies (over 90 %) and provided sustained release for more than 30 days in both laboratory and animal models. Critically, the DCL3 variant, with its lower melting point, showed faster release kinetics, validating that PLA content is an effective tool for controlling degradation and release profiles. In vivo experiments revealed excellent biocompatibility, with prolonged drug retention at the implantation site and minimal inflammatory response, as verified by histological examination. Overall, this work establishes these CL copolymer inks as a highly adaptable and safe framework for the additive manufacturing of implantable therapeutic systems, which are distinguished by their controllable degradation profiles and dependable clinical efficacy. Keywords: 3D printing; Biocompatibility; Biodegradability; Drug delivery; Polymer inks; Printability

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목차

1. Introduction 1

2. Experimental 5
2.1. Materials 5
2.2. Synthesis and Formulation of CL Copolymers 5
2.3. Assessment of thermal integrity for CL copolymers 8
2.4. Analysis of rheological properties for CL copolymers 8
2.5. Analysis of in vitro biodegradation 9
2.6. Formulation of dexamethasone-loaded (DCL) copolymers 10
2.7. Printing process and evaluation of fabrication accuracy 11
2.8. Manufacturing and subsequent evaluation of DCL depots 12
2.9. Determination of encapsulation efficiency and in vitro dexamethasone release 14
2.10. In vivo study procedures for implanted depots 16
2.11. Analysis of in vivo morphology and drug release for DCL depots 17
2.12. Analysis of host response by histological and immunohistochemical methods 18
2.13. Statistical analysis 20

3. Results & Discussion 21
3.1. Synthesis and initial characterization of CL copolymers 21
3.2. Thermal characterization of CL copolymers for FDM applications 22
3.3. Thermal integrity of CL copolymers during FDM processing 23
3.4. Rheological properties of CL copolymers under FDM conditions 27
3.5. Assessment of printing fidelity and structural characteristics for CL copolymers in FDM fabrication 29
3.6. Assessment of in vitro biodegradation for CL copolymers 33
3.7. Preparation and characterization of 3D-printed DCL depots 35
3.8. Analysis of in vitro dexamethasone release from 3D-printed DCL depots 39
3.9. In vivo performance and Dex release profile of 3D-printed DCL depots 41
3.10. Analysis of in vivo host response to implanted 3D-printed DCL depots 45

4. Conclusion 52
REFERENCES 53
LIST OF PUBLICATIONS 59
LIST OF PRESENTATIONS 60

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