具連續監控與操作簡易優勢的穿戴型生醫感測器和遠距環境監測平台隨著智慧型裝置深入日常生活中逐漸受到重視。隨著物聯網技術飛速演進，將感測平台與無線遠距傳輸技術結合能實現同步收集多種生物資訊的人工智慧物聯網系統是未來備受矚目的科技技術。迄今為止，使用稀缺性高與製造成本昂貴的貴金屬觸媒做為電極材料仍為目前商業化電化學感測器所不可取代的一塊；因此發展兼具低成本與高穩定性優勢的非貴金屬電催化觸媒則為實現將電化學感測器整合於人工智慧物聯網系統的關鍵技術之一。
近年來穿戴式生醫感測裝置從連續追蹤體能活動中的生理訊號逐漸擴展至疾病管理，透過非侵入式的方法分析人體生理狀況帶來極高的便利性。在眾多人體生理液體中，汗液不僅含有豐富的待測物能反應其生理狀態且具有在不同部位提供連續監測的獨特優勢。然而，不規則且劇烈的運動可能會導致穿戴式裝置內的感測電極因長時間外力所產生形變並影響其感測準確性與可靠度；有鑒於此，本論文的第四章著重於設計具機械耐久性的氮摻雜石墨烯量子點修飾聚苯胺導電高分子做為新型電催化電極來偵測汗液內葡萄糖濃度來實現具長期穩定性的穿戴型血糖監控平台。由於聚苯胺的電催化活性在中性電解質下會大幅降低，故本研究採用氮摻雜石墨烯量子點來提升其感測能力；透過合成時改變氨水添加量可有效調控氮摻雜石墨烯量子點之氮含量，也可進一步使其表面含氮官能基組成產生變化。將最適化之氮摻雜石墨烯量子點修飾於聚苯胺後證明其對雙氧水範圍0至1 mM之感測靈敏度(68.1 ± 1.11 uA mM-1 cm-2)高於未經修飾之聚苯胺(44.06±2.1 uA mM-1 cm-2)，其原因在於石墨烯量子點上的吡啶氮能有效降低電荷轉移阻力，進而改善聚苯胺之電催化活性並提升感測靈敏度。在導入葡萄糖氧化酵素於電極表面可使其電極在人體汗液葡萄糖濃度範圍(50~500 uM)內的感測靈敏度達到28.2±0.62 uA mM-1 cm-2並同時兼具極佳的選擇率、連續操作穩定性與重複使用性。本研究更進一步將其導入軟性電極來偵測人工汗液中葡萄糖濃度變化，此電極在連續彎曲測試的靈敏度保留率可達93.2%，顯示本研究所提出的具機械耐久性的氮摻雜石墨烯量子點修飾聚苯胺導電高分子電極可以承受日常運動所造成的應力破壞進而達到長期可靠的穩定監控。
 
在遠距環境監控平台方面，水中的溶氧量為水質監測之重要衡量指標，更在漁業養殖與環境廢水處理等產業扮演極具重要的監控參數。電化學溶氧感測器仰賴電極表面的氧氣還原反應推估水體中的溶氧度；然而，電極長時間浸於水體中會出現生物膜附著表面之問題，進而導致感測器之感測靈敏度降低而失去其監測功能與數據品質。基於第四章的結果，本論文的第五章設計出兼具溶氧感測能力與自清潔能力之雙功能電催化觸媒並首度提出一種具自主抗生物附著溶氧感測器的概念。從研究結果證實氮摻雜還原氧化石墨烯在中性電解質能成功催化兩個電子轉移之氧氣還原反應來產生雙氧水，透過改變燒結溫度可調控氮摻雜還原氧化石墨烯中的氮含量變化也同時影響氮官能基組成。從X光吸收光譜觀察到其中的石墨氮光子能階偏移，進一步證實石墨烯量子點上的π電子會由碳轉移至石墨氮上並進而提升其催化以兩個電子轉移為反應路徑之氧氣還原能力。為了驗證雙氧水用於自主抗生物附著於電極表面之效果，於真實水體中連續操作48小時測試結果中可觀察到相比於商用白金電極(留存率= 24.01%)，氮摻雜還原氧化石墨烯表現良好的抗生物膜附著之性能(留存率= 73.29%)。為了進一步驗證氮摻雜還原氧化石墨烯被應用於實際場域之連續式溶氧監測之能力，導入遠端溶氧監測裝置並用於監控人工海水之動態調整溶氧濃度，從數據平台中的即時溶氧量與商用光學溶氧計之數據比較後證實了此研究開發出兼具高效能且自清潔的非貴金屬電催化材料應用於遠距監控溶氧量感測平台。
綜合上述結果，本論文成功證實透過氮摻雜效應能大幅提升氮摻雜碳材複合材料之電催化能力並導入開發可撓曲人體汗液監控元件與自主抗生物附著溶氧感測器中，具高機械耐久性與良好使用穩定性之高效能電催化氮摻雜碳材複合材料實現了對連續式監測生理檢測/水質監控的願景。

Understanding the levels change in biomarker over time, especially glucose, is crucial for diabetics to inform the early therapy. Recently, wearable sweat biosensors which operate in a non-invasive way have raised attention, providing continuous monitoring of the severity level. Nevertheless, the key challenges are that multiplexed motions may result in undesirable metal cracking by the rigid electrocatalytic layer, leading in decreased sensitivity and stability. To realize a reliable wearable sweat biosensor for monitoring glucose levels, in chapter 4, selecting flexible material such as polyaniline (PANI) would be needed. Additionally, introducing carbon materials, such as N-doped graphene quantum dots (N-GQDs) owing to their great electron mobility can level up it electroactivity. In this work, we designed an N-GQDs anchored PANI matrix to realize flexible wearable biosensors with high detection accuracy. Upon the enhanced electron transfer by N-GQDs, N-GQDs/PANI nanocomposite offers greater sensitivity in H2O2 detection compared to pristine PANI, resulting in sensitivity of 68.1±1.11 and 44.06±2.1 uA mM-1 cm-2, respectively. Moreover, after the glucose oxidase (GOx) immobilization, GOx/N-GQDs/PANI based biosensor had shown excellent sensitivity, selectivity, repeatability, and long-term stability for glucose detection in artificial sweat. Precise glucose detection was also maintained after integrating into a flexible electrode, the sensitivity of GOx/N-GQDs/PANI based biosensor had retained 93.2% with no apparent cracks in the morphology of nanocomposite layer, compared to GOx/Pt based one (71.3%) toward glucose detection after continuously bending test. Thus, N-GQDs/PANI nanocomposite layer can provide reliable long-term monitoring with robust electrodes for non-invasive human sweat glucose monitoring on wearable biosensor.
Dissolved oxygen (DO) reflects the self-regulating state of the water environment. The electrochemical DO sensor measured the dynamic DO values via oxygen reduction reaction (ORR). However, the unwanted biofilm growth on the electrode surface may impact the sensitivity and stability of DO sensors in practical applications. The reactive oxygen species (ROS) such as H2O2 had been used for degrading the biofilm attached to the electrode due to its simplicity and free from contamination. Therefore, creating high-efficiency electrocatalysts of ORR with self-anti-biofouling is crucial. In chapter 5, N-doped reduced graphene oxide (N-rGO) was used to promote the two-electron pathway of ORR for generating H2O2 in a neutral medium. After modulating the pyrolysis temperature, the N content and its configuration in N-rGO can be adjusted. In the soft X-ray absorption spectrum (XAS), the photo energy of graphitic N was shifted, which confirmed that the π electrons are moving from C atom to graphitic N, resulting in the remarkable H2O2 selectivity. To identify the effect of self-anti-biofuling via H2O2 formation, N-rGO exhibits extraordinary stability with current retention of 73.29% for 48 hr in the actual sample. A remote DO monitoring device was introduced to examine the feasibility of N-rGO for continuous DO measurement in fish raising, and DO concentration was dynamically adjusted in artificial seawater. The comparison of DO value between data storage platform and commercial optical DO meter confirmed that this research has developed an electrocatalyst integrated a with remote DO monitoring with self-antibiofouling strategy.
Last but not least, the research shed light on the role of N doping in developing carbon-based electrocatalysts, which were introduced in wearable robust glucose biosensors and the DO remote monitoring sensing platforms with high durability and reliable stability in continuous monitoring.

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