隨著物聯網技術快速發展，居家醫療診斷技術徹底改變了個人化醫療保健和無線遠醫療。可穿戴式汗液感測器的發展克服了傳統感測器的許多限制，使健康生理監測系統掌握更細緻之生理資訊，對長期慢性疾病患者的病情管理產生了極大之助益。然而，為了改善傳統生醫感測器應用於連續監控所面臨的問題，例如感測電極的壽命、複雜的電路設計以及長時間待機等；因此，以摩擦起電現象為基礎的摩擦起電感測器能有效解決上述等問題。藉由靜電感應和接觸起電的共軛效應，能使摩擦起電感測器能透過運動過程中收集能量轉換為電力進而實現自供電感測平台；且因結構簡單、材料選擇性多，使自供電摩擦起電感測器在未來的發展備受矚目。
乳酸是人體汗液中的主要代謝物，可作為監控人體運動時的生理狀態之關鍵因素。為了有效感測乳酸待測物，已具有專一性的酵素型感測器為目前應用最為廣泛的技術，然而其生物耐受性不佳與製造成本昂貴限制了此種感測器應用於穿戴式生醫感測平台的應用。為了解決上述問題，本論文的第四章設計出一種全新概念的分子模板修飾摩擦起電感測器，能以非侵入式的方法檢測人體汗液中的乳酸濃度並進一步的實現自供電穿戴式監控平台。分子模板修飾電極是使用PVDF/石墨烯柔性電極並藉由具乳酸分子模板結構之3-APBA進行表面修飾所製備。從實驗結果可證實分子模板電極可隨著人體汗液中乳酸濃度的變化而產生穩定的輸出信號變化，展示了分子模板電極在乳酸吸收後表面性質的改變。進一步將此種分子模板修飾電極引入摩擦起電感測器中，透過接觸/分離的過程中獲取機械能並轉換為電能訊號輸出。當檢測到高濃度的乳酸時，由於分子模板電極所吸附的乳酸量增加將會導致表面電荷下降而使訊號輸出降低。另外，分子模板修飾摩擦起電感測器可在無需外部供電下直接點亮多個LED燈，並且可透過亮度來推斷其乳酸濃度，驗證自供電可穿戴式摩擦起電感測器實現非侵入式監控人體生理狀態的可行性應用。
另一方面，葡萄糖是生物體內細胞活動的主要能量來源，對於維持適當濃度以避免糖尿病發生至關重要。儘管目前商業用葡萄糖監測系統種類繁多，但目前能實現長時間連續監控並以非侵入方式檢測體內葡萄糖濃度技術還是非常缺少的。有鑒於此，延續摩擦起電感測器與自供電穿戴式監控平台的優勢，本論文的第五章設計了一種具有自修復功能的葡萄糖響應性水凝膠並將其應用在摩擦起電感測器來檢測人體汗液中的葡萄糖濃度變化。具有生物相容性的PVA水凝膠可藉由葡萄糖氧化酵素酶(GOx)與β-環糊精的導入來達到具葡萄糖響應性；在葡萄糖水溶液環境下，水凝膠中的GOx與不同濃度的葡萄糖反應所產生的雙氧水將改變其水凝膠網絡性質並造成其電導率的變化。將葡萄糖響應性水凝膠集成到摩擦起電感測器中可以有效地分析人體汗液中的葡萄糖濃度，當檢測高葡萄糖濃度時，通過酶催化反應能增加離子強度導致的導電率和極化效應增強，使其輸出增加。從實驗結果也可證實葡萄糖響應性水凝膠摩擦起電感測器具有廣泛的葡萄糖感測應用，並且具有良好的選擇性、穩定性、可再現性和可重複性等優勢。此外，葡萄糖響應性水凝膠摩擦起電感測器在穿戴式檢測方面具有無需外部電源即可警示人體葡萄糖濃度含量過高的應用。另外，本研究也透過此平台分析膳食消耗前後對於真實人體汗液中葡萄糖濃度變化，進一步證實葡萄糖響應性水凝膠可應用於自供電連續監控人體汗液，讓糖尿病管理開闢了更多可能性。

The tremendous development of Internet of Things (IoT) Technology for point of care (POC) diagnostics potentially revolutionizes personalized healthcare and telemedicine. Recent progress in wearable sweat sensors had overcome numerous limitations of conventional sensors and provided methods of collecting molecular-level insight into the dynamics of human bodies. However, pioneering works in biosensors for biomarkers detection in sweat has been encountered major challenges such as noble material usage, immobile power supply, and complicated circuit connection to realize the compact sustainable sensing systems. Thus, these shortcomings encourage the development of emerging technology between energy harvester powering biosensors to realize the self-powered sensor. Triboelectric nanogenerator (TENG)-based sensors are capable of extracting biomechanical energy from human motion based on the conjugation of electrostatic induction and contact-electrification and sufficiently supply the power to the elaborate self-powered chemical sensors because of simple structure, extensive range of alternative and affordable materials.
Lactate, a major metabolite in human sweat, can serve as the critical limiting factor for continuing physical activity. In chapter 4, the self-powered molecular imprinted polymers-based triboelectric sensor (MIP-TES) was designed to offer a multifunctional noninvasive approach for specific and simultaneous lactate detection. Free-standing PVDF/graphene flexible electrode modified poly-3-aminophenyl boronic acid imprinted lactate molecule demonstrated the change of the surface properties after lactate absorption. MIP-modified electrode revealed the selective lactate sensing over non molecular imprinted polymers (NIP) electrode through the superior and stable signal change with variation of lactate concentration in human sweat. Moreover, MIP modified lactate sensor was further introduced in the triboelectric nanogenerator system to harvest mechanical energy from contact and separation into electrical output. The more adsorbed lactate led to lower energy barriers and decreasing electrical potential when detecting higher lactate concentration. Self-power triboelectric lactate sensor could directly power the number of LED lights without an external energy supply. Eventually, it was validated the feasible application of wearable sensors on human skin.
Moreover, Glucose is a major energy source of cellular activity in the living body which is crucial to maintaining a proper concentration to avoid diabetic complications. Despite the variety of available commercial glucose monitoring systems, the limitations of painless compact glucose sensors have been addressed by the burden of repeated blood collections, delamination of rigid layers, and complex power requirements. Therefore, in chapter 5, the self-healable glucose responsive hydrogel based triboelectric sensors (GRH-TES) was proposed to offer a biocompatible noninvasive approach for simultaneous glucose monitoring. Glucose-responsive PVA hydrogels can be used as an immobilization matrix for glucose oxidase enzyme (GOx) with the aid of beta-cyclodextrin (β-CD) inclusion complex. The alteration of dynamic hydrogel networks in the presence of variable glucose environments endows the changes in conductivity, which facilitates electrical performance. The integration of glucose-responsive hydrogel into a triboelectric nanogenerator offers effective energy conversion from motion-based glucose stimuli in human sweat into electrical output. The increasing TENG output was found when detecting higher glucose concentration due to the enhanced conductivity and polarization effect resulting from the increased ionic strength via enzymatic reaction. GRH-TES has the potential in medical aspects toward the excessive glucose level alarm without an external power supply. Eventually, GRH-TES validated the reliable self-powered glucose concentration from real human sweat associated with meal consumption. The proposed self-powered glucose-responsive hydrogel has opened more possibilities for diabetes management in terms of stand-alone highly selective, deformable, and stable real-time analysis of human perspiration.

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