“智能水凝膠(smart hydrogels)”的研究備受矚目。智能水膠是由混合(hybrid)高分子鏈段組成的三維網狀交聯結構，同時具有特殊組成和卓越設計的水膠，其性能和結構能夠響應各種環境而改變。智能水凝膠已在生物醫學領域具有優越的突破性進展於開發“自我修復(self-healing)"和“分解響應(solubility response)”的先進材料(advanced materials)，其自愈性水膠可以延長材料的壽命以及減少維修費用，可逆響應水膠易於製備並且對生物組織有最小的侵入性。為實現其在生物醫學中的可行性，穩定的微觀結構和適用的機械強度是水凝膠的基礎，因此，複合水凝膠系統是有前景的系統能夠將兩種材料進行互補，從而產生協同效應具有優異的性能。主要重點是在複合水凝膠中開發具有單一或多重外部刺激響應的動態網絡結構。“自我修復”和“可逆響應”的智能複合水凝膠是將其無機或有機材料嵌入至軟性高分子水膠中組成，應用於特性分析，並傳遞生長因子以促進傷口癒合。
本論文具有兩個獨立的研究系統:第一項研究由聚乙烯醇（PVA）和氮化硼納米片（BNNSs）構成兩個互穿的交聯網絡，形成具有熱響應(thermo-responsive)的水凝膠系統。其此水凝膠具有熱自修復性(thermal-healing)以及增強機械性能(enhanced mechanical)的同時不會影響自愈的效能。結果顯示添加氮化硼納米片的聚乙烯醇水凝膠顯著增加水凝膠的玻璃化轉變溫度（Tg）和脹溶程度隨著溫度而成相依性(temperature-dependent swelling)，證實這兩種材料之間的相容性佳，且對外部熱刺激具有敏感性。添加氮化硼納米片的聚乙烯醇水凝膠在熱自修復能力方面優於單網絡的聚乙烯醇水凝膠。當溫度高於玻璃化轉變溫度（Tg）時，水凝膠的熱能增加與水分流失，導致分子鏈段有較高的熱遷移率(thermal mobility)和自由體積(free volume)有利於斷裂處再次形成新的氫鍵。水凝膠中獨特的雙網絡結構賦予較高的水含量與優越的機械性能，由於水凝膠在變形期間，第二個網絡能夠有效地分散另一個網絡的能量與承載力量。總結，我們的研究設計聚乙烯醇水凝膠與氮化硼納米片結合，證實此系統結構能夠發揮加成效果於水凝膠的熱修復性能。
第二部分的研究，開發新型具有可逆、智能的互穿網絡水凝膠（IPN），由熱交聯網絡的泊洛沙姆407(Pluronic F127)作為鈣離子交聯網絡的藻酸鹽模板，可調控水膠的構像。此柔軟而有彈性的互穿網絡水凝膠即使吸收了大量傷口的組織液也能保持其形狀不被破壞，且水凝膠的外部是由較硬的藻酸鹽-鈣離子交聯網絡所組成，使其維持水凝膠的型態，以及促進包覆血管內皮生長因子（VEGF）的穩定性並且局部控制其釋放於傷口。拉曼光譜法證實了水凝膠的層狀結構，其結構在使用冷的磷酸鹽緩衝對傷口進行適度沖洗後具有可逆性。總結，上述結果證實這樣研究中所開發的互穿網絡水凝膠是有前瞻性的生長因子輸送系統和加速傷口癒合的智能敷。

There is growing research interest in "smart hydrogels". In general, smart hydrogels are 3D networks composed of hybrid cross-linked polymer chains. Meanwhile, the intelligent hydrogel with a specific composition and prominent design can undergo alternation of structures and property responding in the various environments. Intelligent hydrogels have found a breakthrough role in feasibility application in biomedical, including advanced materials further developed "self-healing" and "solubility response". The former can prolong the lifetime of materials and low-cost, the behind is in favor of easy fabrication and minimally invasive for biological tissue. To realize their feasibility application in biomedical, the stable microstructure and applicable mechanical strength are the foundation of hydrogels. Thus, composite hydrogel systems are the potential promising platform since complimentary of both materials while eliminating individual disadvantages, resulting in the generation of synergetic effects in desired superior properties. The main focus is to develop the dynamic network construction within the composite hydrogel that can respond to single or multiple external stimuli. A smart, "self-healing" and " solubility response" composite hydrogels composed of inorganic or organic materials embedded in soft polymer hydrogels for characteristic analysis, and delivery of growth factor for wound healing activity.
This dissertation is organized on the basis of two separate sections: the first section study, we aimed to create a thermo-responsive hydrogel that possessed thermal-healing and enhanced mechanical properties, without losing its self-healing capabilities, by employing two interpenetrating cross-linked networks of polyvinyl alcohol (PVA) and boron nitride nanosheets (BNNSs). We observed that addition of BNNSs significantly increased the glass transition temperature (Tg) and temperature-dependent swelling of PVA hydrogels, indicating a high compatibility between these two materials and a high thermal response to external stimuli. Our results suggest that PVA hydrogels combined with BNNSs outperform single-network PVA hydrogels in terms of thermal-healing capacity. As above Tg, the thermal energy gained during moisture loss leads to an increase in the thermal mobility of the polymer chains and in the free volume available for new hydrogen bonds at the fracture surface. This unique structure increases water content and confers better mechanical properties. Interestingly, this structure of the second network benefits the first PVA network during deformation by effectively dissipating energy and bearing force, and contrarily to single network PVA hydrogels. Taken together, our results show that combining PVA and BNNSs to create a hybrid structure, exerts a synergistic effect and successfully improves the thermal-healing performance of wet hydrogels.
In the section study, the aim of this study was to develop a novel, solubility, smart, interpenetrating polymeric network (IPN) by utilizing the thermosensitive network of pluronic F127 (PF127) as a template to regulate the conformation of calcium-ion-cross-linked alginate. We found that the IPN hydrogels formed soft and elastic thermosensitive networks, retaining their form even after absorbing a large amount of wound exudate. The exterior of the hydrogels was made up of a rigid calcium alginate network that supported the entire hydrogel, promoting the stability of the vascular endothelial growth factor (VEGF) payload and controlling its release when the hydrogel was applied topically to wounds. Raman spectroscopy confirmed the layered structure of the hydrogel, which was found to easily disintegrate even after moderate rinsing of the wound with cold phosphate-buffered saline. Taken together, these results show that the IPN hydrogel developed in this study could be a promising delivery platform for growth factors to accelerate wound-healing.

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