近年來由於電子產品的蓬勃發展，使得電化學感測器應用於人體穿戴式感測裝置以及可
攜式環境監控平台逐漸受到重視，並且期盼能進一步結合無線遠距傳輸來達到遠端監控，以
實現同步整合多種生物資訊於未來備受矚目的人工智慧物聯網系統。然而，目前現有的電化
學感測器多半以貴金屬為電催化觸媒，但其成本較高且穩定性不佳，因此開發一高效且具有
高穩定性的電催化觸媒則為電化學感測器最重要的目標之一。
在人體穿戴式感測裝置中，以非侵入方式檢測人體體液中生物標記的穿戴式感測器備受
矚目，其待測物包含了乳酸、葡萄糖以及尿酸等物質，藉由穿戴式裝置提供的連續式監控將
有助於進行健康診斷來了解身體狀況，且能夠提早治療以防止病情惡化。在眾多體內待測物
中，尿酸是人體中普林經由新陳代謝而成的產物，一旦尿酸濃度過高即會引發高尿酸血症以
及痛風等疾病；因此第四章的研究目的旨在開發一種新型電催化材料透過無酵素電化學方法
來偵測汗液內的尿酸濃度以實現具長期穩定性的非侵入式穿戴式尿酸監控平台。本研究採用
兼具高導電度與電催化能力的奈米碳管為載體並導入硼摻雜石墨烯量子點作為電化學活性位
點來實現非酵素型尿酸電催化觸媒，研究結果顯示經由硼摻雜石墨烯量子點修飾之奈米碳管
於尿酸濃度範圍 0 至 50 M 之感測靈敏度(8.92±0.22 A M-1 cm-2)遠高於未經修飾之奈米碳
管(4.24±0.24 A M-1 cm-2)，其主要原因在於硼摻雜石墨烯量子點除了能提供額外的電化學活
性表面積外，且經由理論計算結果可得知硼對尿酸有較佳的吸附能力，使其在尿酸氧化中亦
有較好的表現。硼摻雜石墨烯量子點修飾奈米碳管除了具有良好的選擇性，在經過 28 天的長
期操作下仍擁有 91.28%的回覆率，指出其擁有絕佳的穩定性；此外，本研究更進一步將其導
入軟性電極實現穿戴式感測裝置，在人工汗液下測試其尿酸濃度的準確度高達 98%，其靈敏
度為 35.1±1.5 A M-1 cm-2。
在可攜式環境監控平台方面，溶氧量感測為水質監測非常重要的指標之一，透過監控水
體溶氧量將有益於穩定水產養殖產值以及監測廢水處理等產業的發展。其工作機制仰賴電極
表面的氧氣還原反應進而推估水體中的氧氣濃度，使得開發一高效氧氣還原之電催化觸媒為
一大挑戰。基於第四章研究結果已知硼摻雜石墨烯量子點修飾碳材表面能大幅提升其電催化
能力，因此第五章以此材料概念為基礎來更進一步開發一種全新具有硼氮共摻雜碳材，首先
將氮摻雜至奈米碳管後再利用 π-π stacking 效應將硼摻雜石墨烯量子點吸附其表面，如此一來
便可有效降低 B-N 鍵結比例來大幅提升其氧氣還原之催化能力。從研究結果顯示出硼摻雜石
墨烯量子點修飾氮摻雜奈米碳管的氧氣還原的起始電位為 0.91 V (vs. RHE)，遠高於奈米碳管
的 0.81 V (vs. RHE)。本研究進一步結合可攜式水質監測裝置搭配遠距數據傳輸技術實現連續
式即時監控溶氧平台，能將即時監測溶氧結果透過 wifi 上傳至雲端數據庫。在人造海水條件
下實際測試，其偵測溶氧量於 0 至 18 ppm 可達 0.011 mA/cm2 ppm 的高靈敏度，證實了本研究
提供了一個低成本且高效能的非貴金屬電催化材料應用於遠端線上監控溶氧量感測平台。
綜合本論文之研究結果證實硼摻雜石墨烯量子點之複合碳材確實能夠有效提高整體電催
化能力並成功應用於感測尿酸以及溶氧量等電化學感測，更重要的是具有高穩定特性與良好
電催化特性的硼摻雜石墨烯量子點複合碳材可提高穿戴式/可攜式電化學式感測裝置的可靠
性來有效實現長期連續式監控並結合遠端傳輸的人工智慧物聯網系統願景。

Wearable biosensing devices and portable environmental monitoring platforms via
electrochemical technics have attracted much attention since the widespread of electronic devices could provide useful insights into the performance and health of individuals. Moreover, it is expected to combine with wireless communication to achieve the goal of remote monitoring, realizing the prospect of artificial intelligent Internet of Things (AIoT) system. However, electrochemical biosensors rely on noble metals, which are high cost and low stability. Thus, developing highly efficient electrocatalysts to overcome the sluggish reaction rate of the reduction-oxidation reaction of analytes is a crucial issue.
Recent advances in non-invasively bioanalytical sensors have received enormous attention in the early diagnosis of a range of diseases. In the past few years, sweat is considered as the most popular choice for developing wearable devices due to lots of information in human sweat, including glucose, uric acid and urea. Uric acid (UA) is the main end product of purine in human sweat, exhibiting a high relationship with gout, hyperuricemia, and Lesch-Nyhan syndrome. Therefore,
developing a wearable device to monitor the UA levels in the sweat non-invasively has drawn enormous attention. To design the enzyme-free wearable sensor to monitor the concentration of UA in human sweat, boron-doped graphene quantum dots anchored on carbon nanotubes (BGQD/CNTs) was synthesized as noble-metal free electrocatalyst in Chapter 4. From the results, BGQD/CNTs exhibit ultra-high sensitivity of 8.92±0.22 A M-1 cm-2 for UA detection in comparison to pristine CNTs (4.24±0.24 A M-1 cm-2). Moreover, the DFT calculation indicates that the B atom could
increase the adsorption energy of UA to facilitate the following oxidation reaction. Also, BGQD/CNTs demonstrate outstanding selectivity and superior stability for 30 days with the current retention of 91.28%, suggesting that the B-GQDs could improve their electrocatalytic ability. Notably, BGQD/CNTs can be easily integrated into flexible electrodes, providing constant measurement under bending with a sensitivity of 35.1±0.15 A M-1cm-2, suggesting its potential for utilizing in enzymefree electrochemical UA wearable biosensor with reliable and stable performance.
Dissolved oxygen (DO) is an essential indicator for evaluating water quality, the exquisitely sensitive electrochemical DO sensor could accurately record DO response quickly which the working mechanism based on oxygen reduction reaction (ORR) with a sluggish reaction rate. Thus, highefficient ORR electrocatalysts are urgently needed for broad applications. Based on the previous results in Chapter 4, this work attempt to fabricate a B-N co-doped electrocatalyst in Chapter 5 to further improve its electrocatalytic activity without the presence of B-N bonding. This research design a strategy to solve this problem; despite substantial efforts, this study shows a metal-free BGQD/NCNTs electrode significantly influences ORR catalytic activity due to the synergistic effect and abundant active sites. BGQD/NCNTs exhibits an excellent ORR performance in alkaline medium with onset potential of 0.91 V (vs. RHE), exceeding most previously reported GQDs-introduced
catalysts, it also outperformed the commercial electrocatalyst Pt/C in terms of methanol interference and long-term stability. Furthermore, BGQD/NCNTs exhibit ultra-high sensitivity of 0.011 mA/cm2 ppm in DO sensing in seawater. Additionally, this study measures DO using an online detection platform, accomplishing the aim of continuous monitoring via a wireless connection.The results elucidate the prepared BGQDs composites as noble metal-free electrocatalysts are inexpensive and highly efficient electrocatalysts for replacing noble-metal based electrocatalysts.
Moreover, BGQDs composites could be utilized in wearable UA biosensors and DO remote monitoring sensing platforms with reliable data, which may be capable to realize the prospect of AIoT system. Importantly, this synthetic strategy would provide novel inspiration for the fabrication of various highly efficient carbon-based electrocatalysts for diverse applications.

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