近年來隨著全球人口增長與極端氣候，水與能源短缺的問題日趨嚴峻，儘管已有許多方法可以產生水資源與能源。但幾乎都需要消耗額外的資源，如水資源的有效利用與處理需要大量電能，電能的生產過程亦需要大量水資源，這導致兩者之間有著密切的關連，無法單一考量。因此，大量的研究致力於發展低能耗的水處理方法、新的能源生產方案以及同時獲取水與能源的新型技術。
薄膜科技是解決這些複雜議題最有效且可行的方法之一，本研究提出一種石墨烯-聚偏二氟乙烯 (Polyvinylidene fluoride, PVDF) 壓電薄膜，透過太陽能蒸餾與壓電效應同時獲取乾淨水與能源以克服前述的難題。藉由石墨烯(Graphene)添加以靜電作用力誘導PVDF高分子從非極性α相轉換至壓電性β相。透過海浪驅動薄膜將機械能轉換為電能，在模擬海浪1 Hz下薄膜可獲得2.6 V (±1.3 V)。另一方面，透過光熱效應使薄膜在1倍太陽光下的產水率為1.2 kg m-2 h-1，符合世界衛生組織(WHO)的飲用水標準。
另一方面，太陽蒸餾薄膜在長期的操作下，常因汙染物堆積，造成薄膜的結垢現象(Fouling)，大幅度影響了薄膜的效率與壽命，儘管目前已有部分方法能有效去除一定程度的結垢，然而無法準確判定材料實際結垢程度與清洗時機。為了克服上述議題，本研究於第二部份進一步引入無機的鈦酸鋇(Barium titanate, BaTiO3)，與石墨烯的協同效應強化了PVDF的壓電性能。另一方面，壓電效應同時抑制光生載流子(Photogenerated carrier)重組。薄膜同時具備四種功能包含太陽蒸餾、海浪發電、壓電光降解及結垢移除/監控(Fouling removing/monitoring)。相較於先前研究，在模擬海浪1 Hz下薄膜電壓輸出為8 V (±4 V)，最大發電功率為5.73 W m-2。對於剛果紅(Congo red, CR)染料的壓電光降解率為93%，透過逆壓電振動，對應自監控的電阻回復率為60%。
除了水與能源的短缺，科技的進步總是伴隨著工業汙染，這導致了環境修復在近年來成為備受矚目的議題之一，因此我們針對薄膜以環境友善的壓電降解為目標進行進一步的探討。透過薄膜產生的強壓電場與水或氧氣反應產生活性氧物質(Reactive oxygen species, ROS)如超氧自由基(Superoxide radical, ∙O2-)與氫氧自由基(Hydroxyl radical, ∙OH)，進一步降解汙染物。其中最適化PVDF/Graphene薄膜不僅對於有毒染料羅丹明B(Rhodamine B, RhB) 展現96.1%的降解效率並且在8個循環測試中擁有良好的穩定性與重複性。
本研究深入探討並完成可實現資源生成(潔淨水、能源)和環境修復(汙染物降解)的多功能石墨烯壓電薄膜的技術開發，結合壓電效應與不同機制探討在各領域應用的可行性與潛能，為未來以綠色能源和永續發展為核心的薄膜領域研究人員提出一種新的方向與可能。

In recent years, with global population growth and extreme climate conditions, the issues of water and energy scarcity have become increasingly severe. Although there already have many traditional methods to produce clean water and energy, but most of them need additional resources. For example, the efficient utilization and treatment of water resources require a large amount of energy, while the production of energy also demands substantial water resources. The high degree of interdependence between these two issues makes it impossible to consider them separately. Consequently, extensive research is dedicated to developing low-energy water treatment methods, novel power generation approaches, and innovative technologies that simultaneously acquire both water and energy resources.
Membrane technology is one of the most effective and feasible solutions to address these complex issues. This study proposed a graphene-polyvinylidene fluoride (PVDF) piezoelectric membrane to obtain clean water and energy simultaneously through solar evaporation and the piezoelectric effect, aiming to overcome the aforementioned challenges. PVDF was induced to transfer from the non-polar α phase to the piezoelectric β phase by using the electrostatic interaction with the addition of graphene. The membrane driven by ocean waves converted the mechanical energy into electrical energy, generating 2.6 V (±1.3 V) under a simulated 1 Hz sea wave. Meanwhile, a membrane with photothermal effect achieved a water production rate of 1.2 kg m-2 h-1 under 1 sun illumination, in compliance with the WHO’s standards.
On the other hand, under long-term operation, membrane fouling commonly occurs in membrane applications, and significantly affects the membrane’s efficiency and lifespan due to the accumulation of contaminants. Although some methods effectively remove a certain degree of fouling, accurately determining the actual extent of fouling and the appropriate cleaning time remains challenging. Therefore, in the second part of this thesis, further introducing inorganic barium titanate (BaTiO3), which had a synergistic effect with graphene, enhanced the PVDF’s piezoelectric properties, while also suppressing the recombination of photogenerated carrier. The membrane shows four functions, including solar evaporation, sea wave power generation, piezo-photodegradation and fouling removing/monitoring. Compared to the results in the first part, the membrane exhibited a voltage output of 8 V (±4 V) and a maximum power generation of 5.73 W m-2 at 1 Hz simulated sea wave. The piezo-photodegradation rate for dyes reached 93%. By using reverse piezoelectric vibrations, the corresponding recovery rate of the resistance for self-monitoring was 60%.
In addition to water and energy scarcity, technological advancements have often been accompanied by industrial pollution, making environmental remediation a highly pressing issue in recent years. Therefore, this study aimed to further explore the membrane's environment-friendly piezoelectric degradation capabilities. By utilizing the strong piezoelectric field generated to react with H2O and O2 by the membrane, reactive oxygen species (ROS) such as superoxide radical (∙O2-) and hydroxyl radical (∙OH) are produced to further degrade pollutants. The optimized PVDF/Graphene membrane not only exhibited degradation rates of 96.1% for the toxic dye rhodamine B (RhB) but also showed the good repeatability in 8 cycles.
This thesis delved deeply and accomplished the development of multifunctional graphene-based piezoelectric membranes capable of resource generation and environmental remediation. By integrating piezoelectric effect and exploring different mechanisms, we evaluated the feasibility and potential of their applications across various domains. This presents a new direction and potential for researchers in the field of membrane technology who focus on green energy and sustainable development in the future.

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