近年來由於感測技術的快速進步，健康監測領域發生了重大的變化，尤其是在可穿戴生 物傳感器方面，這些具前瞻性的感測技術能讓使用者更有效率地獲取準確的健康信息並獲得 更佳的醫療效果，藉由通過連續監測更能讓使用者提前意識到疾病前兆進而採取更有效的預 防。可穿戴生物傳感器通常用於非侵入性監測人體液體(尿液，眼淚與汗液等)中的尿素、尿酸、 乳酸和葡萄糖等資訊，與傳統生物傳感器相比，它們具有即時測量以及非侵入性的特點，使 其在應用上更加多元化。而在這之中，基於汗液分析的可穿戴生物傳感器更成為了一種非常 熱門的研究議題，解決了必須通過血液樣本才能監測到生物標誌物的需求。
葡萄糖是人體中的一個重要生物標誌物，是監測多種疾病的關鍵指標，尤其是與血糖失 調相關的疾病(如糖尿病和半乳糖血症);而為了解決一般監測需要侵入式的血樣採集方法，透 過非侵入式並整合穿戴式電子器件來實現葡萄糖監測受到矚目，透過感測貼片就是一種有前 景的解決方案，不僅能夠無縫融入日常生活，也能同時實現連續監測。然而，感測電極的偵 測性能可能會在日常生活中劇烈且不規則的動作所造成的扭曲使其性能大打折扣，因此具有 高機械延展性的導電高分子材料變成為了一個可行的方案，而在這之中聚苯氨因為對雙氧水 具有電催化活性以及簡便的製程方法而脫穎而出，但聚苯氨對於中性溶液的低導電活性仍然 是一個待解決的問題。面對這種障礙，導入高導電能力的碳材料到聚苯氨中會是一個有效的 解決方案，其中碳化氮量子點因具有高反應表面積以及良好的電子傳導能力而著名，再加上 其特殊的 Pyridinic N 結構，能夠改善聚苯氨在中性環境中低導電能力的問題。有鑑於此，在 本論文的第四章提出設計了一種碳化氮量子點修飾聚苯胺電極應用於可饒曲穿戴式生物傳感 器。碳化氮量子點成功地促進了聚苯胺的電荷傳遞，從而顯著提高了靈敏度，在檢測雙氧水 時的靈敏度達到了 95.47 ± 1.31 μA mM−1 cm−2，超越了未經修飾的聚苯氨(45.06 ± 1.07 μA mM−1 cm−2)。此外，結合固定葡萄糖氧化酶技術，碳化氮量子點修飾聚苯胺電極在檢測人工 汗液中的葡萄糖靈敏度高達 49.71 ± 0.45 μA mM−1 cm−2。此外，而在經過連續彎曲測試 300 次 後，碳化氮量子點修飾聚苯胺電極在葡萄糖檢測中的靈敏度仍然保持在 94.88%，且沒有出現任何可見表面裂紋。因此，本研究所提出的碳化氮量子點修飾聚苯胺電極為開發高穩定柔性 感測電極的人體汗液葡萄糖監測系統，提供了一個極具潛力的解決方案。
為了使量子點修飾技術能夠更貼近商業化葡萄糖感測器的應用，在本研究進一步將其導 入在以普魯士藍作為感測材料之生物感測器來進一步提升穩定性與感測能力。普魯士藍是目 前商業化常應用於雙氧水感測材料，能夠在相當低的施加電位下進行雙氧水的還原反應，換 言之，在反應時可以避免氧氣或其他干擾物的反應影響測量結果，結合葡萄糖氧化酶便可成 為良好的葡萄糖生物傳感器。然而雙氧水對於普魯士藍感測層具有破壞性進而導致晶格崩塌 而造成電催化能力大幅降低，因此已經有非常多的研究著重於提升普魯士藍的穩定性。目前 已有許多文獻證明了導入普魯士藍衍生物保護層能夠彌補其感測電極的不穩定性，然而在提 升了穩定性的背後，隨之而來的是驟降的感測能力，這原因可能是低活性的普魯士藍衍生物 保護層覆蓋住普魯士藍感測層的活性位點。有鑑於此，本研究導入氮參雜石墨烯量子點修飾 普魯士藍衍生物保護層實現雙層感測電極結構，以提升普魯士藍感測電極之穩定性與感測能 力。氮參雜石墨烯量子點是個具有奈米及尺寸以及良好材料相容性的物質，其具有大量親水 性官能基，能成功地改善普魯士藍衍生物的結構大小以及親水性能力，進而降低待測物的擴 散阻力，進而顯著提高了靈敏度。使用雙層普魯士藍感測電極在檢測雙氧水時的靈敏度達到 了 221.29 ± 1.77 μA mM−1 cm−2，超越了單層普魯士藍感測電極(129.37 ± 4.57 μA mM−1 cm−2)， 此外，通過固定葡萄糖氧化酶於電極表面，雙層普魯士藍感測電極對於葡萄糖的感測靈敏度 高達 90.49 ± 1.08 μA mM−1 cm−2。更重要的是，雙層普魯士藍感測電極在連續操作 90 分鐘下 仍具有 87.37%的電流穩定性，其訊號穩定性比單層普魯士藍感測電極來得更加可靠。因此， 本研究所提出的的氮參雜石墨烯量子點修飾普魯士藍衍生物保護層，結合普魯士藍感測層的 雙層結構感測電極對於非侵入式連續監控葡萄糖濃度提供了一個新穎且可靠的路徑。

For diabetics, it is critical to comprehend the biomarker levels, particularly glucose, vary over time in order to guide early medication. Wearable sweat biosensors have received attention recently due to their continuously monitor the severity level and work in a non-invasive method. However, the primary problems are that the stiff electrocatalytic layer may cause unwanted metal cracking as a result of concatenated movements, which would reduce stability and sensitivity. In response to this issue, we designed a carbon nitride quantum dots (CNQDs) integrated polyaniline (PANI) nanocomposite layer as a flexible sensing electrode for wearable sweat biosensors with outstanding detection accuracy for non-invasive glucose monitoring in Chapter 4. The sensitivity of PANI is substantially enhanced by the high surface area and abundant edge structures of CNQDs, which facilitate charge transfer. Furthermore, the pyridinic N functional groups in CNQDs improve the low conductivity of PANI in neutral solutions and help PANI retain its protons by introducing negative charges to the PANI surface, thereby enhancing the charge mobility of component. The effect resulting in a remarkable enhancement in sensitivity with a value of 95.47 ± 1.31 and 45.06 ± 1.07 μA mM−1 cm−2 in detecting H2O2, surpassing pristine PANI. Furthermore, through the strategic immobilization of glucose oxidase (GOx) within a flexible electrode, significant effectiveness was observed in detecting glucose in artificial sweat. This flexible electrode, followed by continuous bending test, maintained an impressive sensitivity to glucose detection to 94.88%, without any visible cracks in the nanocomposite layer's morphology. In regard to this, our CNQDs/PANI nanocomposite offers a promising solution for developing a dependable monitoring system with sturdy electrodes for non-invasive human sweat glucose monitoring via wearable biosensors. In Chapter 5, improvements to the preciseness and dependability of wearable biosensors for diabetic tracking are necessary for enhancing the quality of the results for patients. The consumption of pristine Prussian Blue (PB) or the combination with its analogues (PBA) has been the subject of numerous studies that have evaluated glucose sensor. However, the first approach is confronted with obstacles as the consequence of the low stability that arises from the reaction with hydrogen peroxide, whereas the other is afflicted by diminished sensitivity as an effect of obstructed active sites. We addressed these issues by incorporating nitrogen-doped graphene quantum dots (NGQDs) into the protective layer of PBA, in conjunction with a PB sensing layer, to develop a wearable biosensor that possesses exceptional stability and accuracy in detection. The surface properties of PBA were successfully improved by NGQDs, resulting in a substantial rise in the overall sensor sensitivity. The sensitivity of 221.29 ± 1.77 μA mM−1 cm−2 was achieved while detecting H2O2, which is comparable to the pristine PB with acceptable sensing capabilities. Furthermore, the glucose detection sensitivity was significantly enhanced by the strategic immobilization of GOx on the electrode (90.49 ± 1.08 μA mM−1 cm−2). More importantly, this nanomaterial demonstrated outstanding stability. The current density retention rate reached 87.37 % through long-term operation at a specific concentration, and the sensitivity remained at 88.17 % with continuous repeated use. Therefore, our NGQDs/PBA/PB nanocomposite provides a prospective solution for the development of a dependable monitoring system with durable electrodes that is appropriate for the non-invasive monitoring of glucose in human sweat through wearable biosensors.

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