隨著物聯網和穿戴式電子產品的快速發展，可提供持續且穩定的電源問題變得越來越重要。自供電系統不僅可以減少電子元件對電池的依賴，亦可以提供穩定的能源輸出進而成為次世代電子科技發展的未來趨勢。以摩擦起電現象為基礎的摩擦奈米發電機可有機會實現可持續自供電的穿戴式電子元件系統，藉由接觸起電與靜電感應的共軛效應，可輕鬆地透過人體運動過程中以機械能轉變成可用電能，且因材料選擇性多，結構簡單，使自供電的摩擦奈米發電機在未來的發展備受矚目。
摩擦奈米發電機常使用物理沉積技術來製備金屬導電薄膜電極；然而，金屬薄膜電極容易在空氣中被氧化且在人體運動過程中容易斷裂破損導致耐用性及導電性下降，因此開發具可撓性的非金屬薄膜電極為將摩擦奈米發電機導入穿戴式電子元件的重要課題。故本論文於第四章設計出了一種以石墨烯聚偏二氟乙烯複合薄膜來實現兼具導電層與摩擦層的雙功能薄膜電極並應用於可撓式摩擦奈米發電機；本研究也首度提出透過石墨烯誘導聚偏二氟乙烯進行自組裝轉變成具有高極化的晶相並將其用於提高摩擦奈米發電機的輸出表現，透過表面界達電位分析能證明具自組裝晶相聚偏二氟乙烯的表面電位(-41.35 mV)高於一般聚偏二氟乙烯(-33.47 mV)。另一方面，具高導電性的石墨烯能於複合薄膜中形成具高機械強度與柔韌性的非金屬導電層，透過簡易有效的鍍膜策略能使其能有效附著於複合薄膜中。通過導入不同比例的石墨烯與製模參數來有效調整石墨烯聚偏二氟乙烯雙功能複合電極的導電性與自極化來進一步提升其應用於軟性摩擦奈米發電機的輸出。本研究所提出的石墨烯聚偏二氟乙烯複合電極在連續彎曲測試下並不會因外力而改變形貌及性能，甚至能將此薄膜塗布在不規則形狀物體上來實現摩擦起電感測器的功能，顯示此複合薄膜有潛力被導入到自供電系統中實現可穿戴式電子元件的願景。
另一方面，具有材料多樣性及結構簡易的摩擦起電感測器在近年來蓬勃發展，能夠有效克服傳統壓電感測器的靈敏度不足及材料選擇受限等缺點。然而，如何提升摩擦層表面電荷成為實現高靈敏摩擦起電壓力感測器的一大瓶頸。有鑒於此，本論文第五章設計出了一種以氮摻雜還原氧化石墨烯修飾聚偏二氟乙烯複合薄膜作為電荷捕捉層來提升摩擦性能並應用於摩擦發電壓力感測器；本研究提出通過導入具有高比表面積和豐富自由電荷載流子密度的氮摻雜還原氧化石墨烯作為電荷捕捉材料使其成為電荷儲存位點，透過改變燒結溫度調控氮摻雜還原氧化石墨烯中的氮含量變化以調控電荷儲存位點進而提升摩擦發電的輸出性能，其摩擦電荷輸出結果亦證實導入氮摻雜還原氧化石墨烯作為電荷捕捉層的表面電荷(80 nC)高於一般聚偏二氟乙烯(40 nC)。此外，電荷捕捉層除了可以有效的屏蔽摩擦電荷向下擴散至下方電極所感應出的電荷結合，也可增益層與層間的極化效應來提升輸出性能。因此，導入氮摻雜還原氧化石墨烯電荷捕捉層的摩擦起電壓力感測器之靈敏度(15.68 V/kPa)遠高於傳統聚偏二氟乙烯（5.63 V/kPa），顯示了導入氮摻雜還原氧化石墨烯作為電荷捕捉層具有強大的潛力應用於穿戴式自供電摩擦起電式壓力感測元件。
綜合本論文之研究結果證實石墨烯修飾聚偏二氟乙烯複合薄膜具有高機械強度與柔韌性，能有效提升摩擦奈米發電的性能應用於軟性摩擦奈米發電機與高靈敏摩擦起電壓力感測元件，能有效實現自供電摩擦起電感測器應用於穿戴型連續監測人體生理狀況的願景。

With the booming development of the Internet of Things and wearable electronics, a continuous and sustainable power supply apparently become a crucial issue. Self-powered systems can provide a stable energy output and reduce the dependence of electronic components such as batteries. Triboelectric nanogenerators are the promising next-generation of energy harvester based on the triboelectrification for converting the mechanical energy of human movement into electrical energy. Moreover, the self-powered triboelectric nanogenerators have attracted much attention due to the abundant material choices and simple structure.
Conventionally the triboelectric nanogenerators will use metal conductive thin film electrodes. However, two main difficulties including the oxidized metal electrodes in the air and easy damage caused by human movement result in the loss of durability and conductivity. The metal-free film electrodes turn into the alternatives utilizing in wearable triboelectric nanogenerators devices. Therefore, in Chapter 4, a graphene-modified polyvinylidene fluoride (Gr/PVDF) composite film is designed to realize a bifunctional film electrode in flexible triboelectric nanogenerator. The graphene is introduced as the frictional layer to induce the PVDF transformation into a highly polarized β-phase which improved TENG output performance. Solid surface analysis was investigated by electrokinetic analyzer. The findings demonstrated that the surface potential (-41.35 mV) of the self-assembled β-phase PVDF was higher than the pristine PVDF (-33.47 mV). Graphene is also renowned for its high electrical conductivity, high mechanical strength and flexibility to simply fabricate as the conductive layer in metal-free electrode. By introducing the different ratio of graphene and molding parameters, self-polarization graphene/PVDF bifunctional composite electrode could rival the use of metal electrode. Furthermore, there are the retained TENG performance and electrode morphology under continuous bending test. Surprisingly, the graphene/PVDF film can be coated on irregularly shaped objects which would be adventurous for self-powered wearable and flexible electronics.
On the other hand, diverse materials and simple structures in triboelectric sensors can effectively overcome the shortcomings of traditional piezoelectric sensors such as insufficient sensitivity and limited material selection. However, surface charge improvement on triboelectric layer has become a major bottleneck in the realization of a highly sensitive triboelectric pressure sensor. Therefore, in Chapter 5, a N-doped reduced graphene oxide modified polyvinylidene fluoride (N-rGO/PVDF) composite film was designed as a charge trapping layer and further introduced into the triboelectric pressure sensor. N-rGO with high specific surface area and abundant free charge carrier density as a charge-trapping material served the charge storage site. The output performance is significant enhanced by modulating the N content in N-rGO by changing the pyrolysis temperature in the synthesis process. The surface charge (80 nC) of the N-rGO/PVDF trapping layer was higher than that of pristine PVDF (40 nC). In addition, the charge trapping layer can not only shield the triboelectric charges diffusion, but also increase the polarization effect in between the layers to improve the output performance. Therefore, the sensitivity of the triboelectric pressure sensor (15.68 V/kPa) had significant enhanced with the introduction of N-rGO/PVDF compared to the traditional PVDF (5.63 V/kPa), indicating that N-rGO has strong potential to improve the performance of wearable self-powered triboelectric pressure sensor as a result of charge storage site.
Graphene/PVDF composite film with high mechanical strength and flexibility can effectively improve the output performance of triboelectric nanogenerators in course of enhanced conductivity and charge storage ability. Thus, graphene/PVDF composite can be utilized into the wearable self-powered sensor for continuous monitoring in various human physiological conditions.

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