本論文以熱可塑性聚胺基甲酸酯膜(Thermoplastic polyurethane, TPU)為基材，利用臭氧活化方式，進行表面接枝聚合反應，使膜表面產生-COOH 或-NH2基團，然後利用硫酸化葡聚糖 (dextran sulfate, DS)與水溶性幾丁聚醣(water-soluble chitosan, WSC)以共價結合固定於TPU表面。 或以層接式自我組裝方法形成多層聚集，其中並包覆有奈米銀膠體，分別探討其表面改質後抗菌性、生物分解性、與L929纖維母細胞成長之影響，並且分析血液相容性，以作為血液導管或血管支架填充材之應用。
所得改質前後之TPU膜將以XPS、接觸角、Zeta Potential、FE-SEM與AFM等表面分析來確定聚電解層固定化改質後材料特性，並以測定接觸角來判定其親水性及表面自由能。分別測試材料改質前、後之凝血蛋白原(fibrinogen)和血小板吸附性質，及其凝血時間以探討其血液相容性。最後測試表面固定化多層結構之TPU 之抗菌性，以期獲得生物相容性最佳之生化膜材。並加以評估其長期穩定性及有效性，以便未來運用於組織培養或人工臟器等應用。
結果顯示過氧化物量及聚丙烯酸接枝密度在臭氧處理20分鐘達到最高值。以WSC作為延伸鏈，可大幅提高硫酸化葡聚糖的接枝密度。另外在表面性質，其接觸角隨硫酸性葡聚糖接枝密度而下降表示親水性因此而提高。隨著硫酸性葡聚糖的接枝密度之增加，APTT 顯著延長，血小板吸附量與凝血蛋白原吸附量下降。這些結果顯示硫酸性葡聚糖的接枝可增加TPU 薄膜之親水性、血液相容性使其具有抗菌性。並且細胞相容性獲得大幅改善。
另外由UV光譜、SEM 及Zeta-scattering 粒徑分析，我們發現利用硫酸化葡聚糖當為奈米銀穩定劑及以葡萄糖當為還原劑，可得到粒徑更小及穩定均勻分散奈米銀膠體。由反應動力學得知其反應速率隨硫酸化葡聚糖量及溫度成正比關係。
層接式(Later-by-layer, LBL)自我組裝改質方式係利用物種帶正、負電荷的性質，經由靜電力互相吸引而自組合，形成多層聚電解質的結構。由FE-SEM 及AFM觀察可知聚電解質多層結構厚度隨改質次數增加而增加但粗糙度並沒顯著增加。 由XPS及染料確認可得知chitosan 及 dextran sulfate 量也隨固化層增加有線性增加趨勢。由接觸角與Zeta電位量測可知第四層結構已成功完全披附於TPU表面。如此更使親水性提高。由抗菌性實驗可確認奈米銀加入可彌補幾丁聚醣因硫酸化葡聚糖減少之缺點 而且由於硫酸化葡聚糖量增加更降低TPU膜蛋白質與血小板吸附進而增長血液凝血時間。由凝血時間長期實驗得知，當固化層大於三層時，其APTT時間在4週內並無明顯變化，表示有優良穩定性。
整體而言，層接式自我組裝改質方式具有方便性、經濟性、可控制性更是無毒性之表面改質方法，改質後TPU膜在血液接觸性生醫材用途深具潛力。

In the study, the improvement of antibacterial activity, cytocompatibility and haemocompatibility of thermoplastic polyurethane (TPU) film was developed using surface modification of polyelectrolyte complexes (PECs) immobilization. The presented work was divided into three parts to study. Part 1 investigated the covalent binding of PECs biomaterials via pre-ozone irritation and graft copolymerization. The PECs of water-soluble chitosan (WSC)/ dextran sulfate (DS) was covalently immobilized onto the surface of TPU membranes by poly(acrylic acid) (PAA) graft polymerization, thereby improving the hydrophilicity, antibacterial activity, and cytocompatibility and blood compatibility. Part 2 fabricated the DS-stabilized nanosized silver colloid. The effect of concentration of DS and reducing agent of dextrose on the mechanism and kinetics of chemical reduction of silver were studied. Part 3 constructed the acid-soluble chitosan (CS)/silver-encapsulated dextran sulfate (DSS) PEC multilayers immobilized on TPU film via layer-by-layer (LBL) self-assembly of technique.
The obtained results showed that the surface density of peroxides generated and PAA-grafted reached the maximum value at 20min of ozone treatment. It was found that the WSC- and DS-immobilized amount increased with pH and the molecular weight of WSC. The as-prepared membrane/water interfacial free energy increased with PAA-grafting and PEC-immobilization, indicating the increasing wettability of TPU membrane. The adsorption of human plasma fibrinogen (HPF) on TPU-PEC membranes could be effectively curtailed and exhibited the unfavorable adsorption. Moreover, the PEC immobilization could effectively reduce the platelet adhesion and prolong the blood coagulation time. After WSC- and PEC-immobilizing modification, the TPU membranes possess the antibacterial activity . According to L929 fibroblast cell grow inhibition index, the resulted TPU membranes exhibited non-cytotoxic. In addition, the in-vitro evaluation of L929 fibroblasts attachment, proliferation and viability of PEC-immobilized TPU membranes could be ascertained superior to those of immobilized WSC alone or native TPU. Therefore, PEC immobilization could not only improve the hydrophilicity, cytocompatibility and hemocompatibility of TPU film, but also endow the antibacterial activity.
Macromolecular and polyanionic Dextran sulfate (DS, MW = 500,000) were tested in this work for their ability to stabilize silver colloids obtained from chemical reduction by dextrose. Our results indicated that their effects against agglomeration would depend to a great extent on the dosage of DS used for the promotion of reduction reaction. It was found that the values of rate constant from silver kinetics were proportional to the quantity of DS added and reaction temperature at the beginning of these reactions, thereby indicating the conversion of silver nanoparticle indicated quicker than that in the absence of DS. Therefore, the simple, rapid and non-toxic formation method of stabilized silver colloid (DSS) should be promising and potential for the biomedical application.
In the other project, TPU film was aminolyzed via ozone treatment, graft polymerization of N-vinylformamide (NVF), and hydrolysis to introduce an amino-group bearing surface. It was found the PEC multilayer consisting of CS (as a positive-charged and antibacterial agent) and DSS (as a negative-charged and anti-adhesive agent) were successfully prepared on the aminolyzed TPU film in a layer-by-layer (LBL) self-assembly manner. The obtained results showed that the contact angle decreased with the layer number of PEMs, however, reached to the steady value at 4 layer of coating, hence proving the full coverage of coating with PEM layers was achieved only after the deposition layers of TPU-DSS(CS/DSS)4. Furthermore, we could find the three-dimensional and porous structure on the surface. The results of antibacterial activity against MRSA elucidated effective on TPU-DSS(CS/DSS)5. Although chitosan could be antibacterial agent, the antibacterial activity could reduced due to the formation of PEMs layer. Therefore, the silver nanoparticle-encapsulated multilayer is essential. The static platelet adhesion and static clotting time experiments indicated that the PEMs-deposited stainless steel could resist the platelet adhesion and prolong the blood coagulation times effectively. The APTT data revealed that the multilayer coating was stable in pH 7.4 buffer saline (PBS) for 28 days with more than 3 biolayer immobilization. Overall result demonstrated that such an easy processing and rapid and non-toxic method should have good potential for surface modification of TPU in the application of blood-contacting devices, such as cardiovascular stent or blood vessels.

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