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Title: | 聚胺酯於生物製造與柔性電子之醫療應用研究 Polyurethane in Biofabrication and Flexible Electronics for Healthcare Applications |
Authors: | 吳欣達 Shin-Da Wu |
Advisor: | 徐善慧 Shan-hui Hsu |
Co-Advisor: | Horst Weller;Tobias Vossmeyer Horst Weller;Tobias Vossmeyer |
Keyword: | 聚胺酯,生物列印,智能水凝膠,自我修復,應變感測器,心臟晶片平台, Polyurethane,bioprinting,smart hydrogel,self-healing,strain sensor,heart-on-a-chip, |
Publication Year : | 2024 |
Degree: | 博士 |
Abstract: | 本篇論文呈現了涉及材料科學、生物製造、柔性電子和組織工程等多個領域的跨學科研究,其中特別焦點於聚胺酯材料於前瞻醫療應用革新扮演的重要角色。整個研究分為四個各具重點特色、相互關聯的主題,成功展示了創新智能性生物材料發展與新穎應變感測器製備方法及其應用。首先第一個主題介紹了一種由可生物降解聚胺酯與明膠基生物材料製成的多智能性水凝膠,具備之環境響應特性使其可用於高精度 (80微米) 3D生物列印,具備之自我修復特性使其可確保生物列印之結構具良好的結構一體性。此外,水凝膠具有之良好的堆疊性 (80層以上)、結構穩定性、彈性、生物相容性及可調整的機械模量 (1-60千帕) 使其可應用於各種組織工程發展。另外,此水凝膠還具有良好的形狀記憶特性及冷凍保存能力,可應用於4D生物列印、臨床微創手術、及生物銀行長期保存與運輸發展。第二個主題選擇探討與聚胺酯具結構相似性 (軟硬鏈段交替排列) 的重組蜘蛛絲水凝膠。研究結果發現此水凝膠具有自我修復特性與好的細胞相容性。透過原位小角度X光散射分析,揭示了其自我修復機制與結構內部之β摺疊奈米晶體的黏滑行為相關,此研究成果對自我修復水凝膠於生物醫學領域發展具重要意義。第三個主題將可生物降解聚胺酯薄膜與交聯之奈米金薄膜結合,朝向發展具環境保護特性之可穿戴應變感測器。在此,我發展了一種乾淨、簡易、快速且可擴展的接觸列印新方法,不需使用犧牲性高分子載體或有機溶劑即可完整地將圖案化之奈米金薄膜轉移至聚胺酯薄膜上。製作之奈米金-聚胺酯應變感測器具低楊氏模量 (~17.8兆帕)、高可拉伸性、良好應變穩定性與耐久性 (10000個週期)、及可降解特性。進一步發展之應變感測器陣列具時空間應變解析度,作為可穿戴感測器可實時監測人體的微小生理訊號或大範圍的肢體動作行為。第四個主題發展了一新的心臟晶片平台,其含人類誘導多能幹細胞衍生的3D心肌細胞球、具自我修復特性之水凝膠、及奈米金-聚胺酯懸臂式應變傳感器,作為人體外的心臟模型。第三個主題中開發的乾淨接觸列印方法在此被使用來製備奈米金-聚胺酯懸臂式應變傳感器以確保其生物相容性。製作之奈米金-聚胺酯懸臂式應變傳感器具高應變係數 (~50),可於發展的心臟晶片平台中有效監測心肌細胞球的收縮與舒張行為。 This dissertation presents interdisciplinary research at the intersection of material science, biofabrication, flexible electronics, and tissue engineering, specifically emphasizing the role of polyurethane (PU) in revolutionizing healthcare applications. Spanning four distinct but interrelated projects, this research not only demonstrates the development of smart biomaterials but also introduces novel fabrication methods and diverse applications for strain sensors. The first project introduces a novel smart hydrogel, comprising biodegradable PU and gelatin-based biomaterials. This hydrogel exhibited an environmental-responsive behavior, which makes it suitable for high-resolution (80 μm) three-dimensional (3D) bioprinting. Additionally, the hydrogel showed an ionomeric self-healing property, which is instrumental in ensuring the good structural integrity of bioprinted constructs. Further, the hydrogel demonstrated good stackability (> 80 layers), structural stability, elasticity, biocompatibility, and tunable modulus (1-60 kPa). These characteristics collectively underscore its vast potential in diverse tissue engineering applications. In addition, the shape memory and cryopreservation properties of the hydrogel make it a promising candidate for four-dimensional (4D) bioprinting in minimally invasive surgery and biobanking. The second project focuses on recombinant spider silk hydrogel, chosen due to its structural similarity with PU (i.e., alternating arrangement of soft and hard segments). This work showed the autonomous self-healing property and cytocompatibility of the recombinant spider silk hydrogel. In situ small-angle x-ray scattering (SAXS) analyses revealed that the self-healing mechanism was associated with the stick-slip behavior of the β-sheet nanocrystals. These results, first identified in my research, mark an important advancement in the biomedical field of self-healing hydrogels. The third project expands into advanced wearable eco-friendly electronics, integrating biodegradable PU films with crosslinked gold nanoparticle (GNP) films. A facile, clean, rapid, and scalable contact printing method with high reliability was developed for transferring the patterned GNP films onto the PU film, without the need of a sacrificial polymer carrier or organic solvents. The fabricated GNP-PU strain sensor with low Young''s modulus (~17.8 MPa) and high stretchability showed good stability and durability (10000 cycles) as well as degradability. The GNP-PU strain sensor arrays with spatiotemporal strain resolution are applied as wearable eco-friendly electronics for monitoring subtle physiological signals and large-strain actions. The fourth project introduces a heart-on-a-chip platform as the in vitro cardiac model, comprising the 3D human induced pluripotent stem cell (hiPSC)-derived cardiomyocyte spheroid-laden gel matrix and the GNP-PU cantilever-based strain sensor. The clean contact printing method developed in the third project was used for fabricating the GNP-PU cantilever-based strain sensor to preserve the biocompatibility. The fabricated cantilever-based GNP-PU strain sensor demonstrated a high gauge factor (~50). The developed heart-on-a-chip platform was capable of detecting the contractile behavior of the cardiomyocyte spheroids. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/92571 |
DOI: | 10.6342/NTU202400827 |
Fulltext Rights: | 同意授權(限校園內公開) |
Appears in Collections: | 高分子科學與工程學研究所 |
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