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研究生: 林大鈞
Lin, Da-Jun
論文名稱: 生醫用鎂鋅合金微觀組織及表面處理效應對生物降解特性及生物相容性之影響
Effects of Microstructure Modification and Surface Treatment on the Biodegradable Characteristics and Biocompatibility of Bio-Magnesium-Zinc alloy
指導教授: 洪飛義
Hung, Fei-Yi
學位類別: 博士
Doctor
系所名稱: 工學院 - 材料科學及工程學系
Department of Materials Science and Engineering
論文出版年: 2017
畢業學年度: 105
語文別: 中文
論文頁數: 205
中文關鍵詞: 鎂合金生醫材料生物降解
外文關鍵詞: Magnesium alloy, Biomaterial, Biodegradation
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  • 鎂金屬因具有適當的生物力學特性及生物可吸收(降解)性,降解過程中釋出的鎂離子可刺激細胞的生理活性,適合應用在短期植入的人工植體上,有機會導入低受力區的骨固定治療用途中,為近年的前瞻生醫金屬材料。但鎂合金由於高活性及低腐蝕阻抗,導致材料表面析氫速度過快,可能降低細胞及組織貼附及癒合的反應,因此必須運用材料組織及表面改質技術,使鎂合金的缺點獲得良好改善並提升其應用性。
    本研究考量生物安全性,以無毒的鎂鋅合金為素材,研究分三階段,首先使用熱處理進行組織調質研究,調控真空熱處理參數使材料內部產生迥異的質地特徵,並透過機械性質、腐蝕試驗及生物試驗得知均勻且細晶的微觀組織最適合應用於可降解鎂醫材中,最佳化組織的降解速率適中,於細胞層級可促進骨細胞快速增生及遷移,於實驗兔腿骨植入試驗中亦發現具有快速形成骨痂及骨質增厚的作用,證明其具有優異的骨傳導性。第二階段運用表面奈米氟晶沉積塗覆材料表面,材料鈍化且明顯降低析氫速度,由塗層解析中得知,奈米氟晶為奈米級氟化物複合介金屬化合物的雙相塗層,該塗層隨時間增長而增加厚度及緻密性,為其主要的表面鈍化機制;此塗層亦可透過表面光學測量得知其成膜品質,當塗層光反射率低於3.5%時,塗層的防護效率可達90%以上。第三階段研究以微晶化成形法進行骨科及牙科鎂醫材製備,本研究為首例採用微晶化成形製程開發出骨科鎂克氏針及牙科鎂再生膜,結果顯示微晶化組織具有更好的機械性質及耐蝕表現,導入前二階段之最佳化改質技術更有效提升材料耐用性,以骨科克氏針為例,長時間體外腐蝕-彎折強度仍可維持七成結構強度;以牙科再生膜為例,由預彎折-腐蝕試驗及大鼠植入試驗發現,微晶化及複合式改質材料具有最佳防蝕效果,可避免材料短時間內失效的疑慮,同時材料具有加速骨癒合的效果,於三個月植入期內即可完整修復大面積骨缺損區。由上述結果,本研究所研究之改質型鎂鋅合金及相關表面處理技術可有效應用於可降解性骨科及牙科植體。

    Magnesium(Mg) alloys are novel biodegradable materials which have been studied recently for temporary fixation. In addition, Mg is known to play an important role in the bone formation and mineralization, moreover, the degradation products of Mg alloy can stimulate bone cell and tissue for improving healing reaction. However, owing to high surface activity and hydrogen evolution rate, the healing situation might be seriously affected. Thus, microstructure modification and surface treatment are indispensable to improve anti-corrosion behavior and applicability.
    The attempt will be devoted to combine microstructure modification and surface treatment for obtaining well-functioned Mg-based orthopedic and dental implant (Kirschner pin and regeneration membrane). After optimized modification procedure, mechanical and anti-corrosion performance were significantly improved. The reliability tests showed that the duplex modification can maintain the mechanical integrity of Mg substrate. Furthermore, the biofunctionality of Mg implants was studied by using mouse cranial model. It was found that the well treated Mg alloy could accelerate new bone growth and heal almost 100% after 3 month implantation. It was concluded that the modified Mg-Zn alloy had good biocompatibility and can apply in orthopedic and dental field.

    第一章 緒論 1 第二章 文獻回顧 3 2-1生醫植體材料 3 2-2鎂金屬醫材的特性及優點 4 2-3鎂金屬醫材之缺點 7 2-4鎂合金腐蝕機理及腐蝕控制 9 2-5生醫鎂合金之合金組成 10 2-6鎂合金組織調質處理 13 2-6-1塑性加工對鎂合金的影響 13 2-6-2熱處理對鎂合金的影響 15 2-7鎂合金表面改質技術 16 2-8研究目的 18 第三章 高鋅與低鋅型鎂鋅合金之熱處理組織特性對其機械性質、腐蝕性及生物相容性之影響 20 3-1前言 20 3-2研究方法 21 3-3實驗結果與討論 31 3-3-1固溶熱處理效應對低鋅型鎂鋅合金之晶粒大小及均勻度影響 31 3-3-2固溶熱處理效應對低鋅型鎂鋅合金之腐蝕特性影響 32 3-3-3固溶熱處理效應對低鋅型鎂鋅合金之生物相容性影響 35 3-3-4不同熱處理效應對高鋅型鎂鋅合金之微觀組織調控 45 3-3-5晶粒大小與第二相分布形態對鎂鋅合金之機械性質影響 48 3-3-6晶粒大小與第二相分布形態對鎂鋅合金之體外降解特性影響 50 3-3-7高鋅型鎂鋅合金的組織效應對體外細胞相容性之影響 56 3-3-8鎂鋅合金的組織效應對骨缺損動物模型之修復成效 58 3-3-9鎂鋅合金的組織效應對表面生成氧化皮膜之影響 61 3-3-10高鋅半固態鎂合金之腐蝕破壞機制 65 3-4結論 67 第四章 鎂鋅合金組織改質效應對表面氟化塗層之成膜特性、耐蝕性及生物相容性的影響 90 4-1前言 90 4-2研究方法 91 4-3結果與討論 93 4-3-1組織改質型鎂鋅合金表面氟化處理之塗層特性評估 93 4-3-2氟化處理對組織改質型鎂鋅合金之體外腐蝕試驗影響 95 4-3-3氟化塗層表面耐蝕性及其光學特性 99 4-3-4氟化處理對組織改質型鎂鋅合金之骨細胞適應性分析 101 4-4結論 103 第五章 鎂鋅醫材(克氏針及再生膜) 組織微晶化及表面奈米氟晶沉積之複合處理效應 121 5-1前言 121 5-1-1前瞻性鎂基骨科克氏針 121 5-1-2前瞻性鎂基牙科再生膜 122 5-2 研究方法 127 5-3 實驗結果與討論 133 5-3-1微晶化成型製程對克氏針之微觀組織影響 133 5-3-2均質化熱處理對微晶化克氏針之微觀組織及機械性質影響 137 5-3-3微晶化克氏針之表面氟化塗層特性 140 5-3-4微晶化克氏針之體外降解試驗 141 5-3-5微晶化克氏針於模擬體液內之表面氧化行為 143 5-3-6微晶化克氏針於模擬體液內之彎折強度衰減 146 5-3-7微晶化再生膜及其熱處理與表面處理特性觀察 168 5-3-8微晶化再生膜之體外降解試驗 169 5-3-9微晶化再生膜之生物體植入試驗 173 5-4 結論 177 第六章 總結論 192 第七章 參考文獻 195

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