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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/96208| 標題: | 開發功能性電化學膜於高效鈷金屬螯合物破壞及鈷自由離子捕捉之研析 Tailoring functional electrochemical membranes for efficient decomplexation of cobalt complexes and subsequent capture of liberated cobalt ion |
| 作者: | 吳偵慈 Jhen-Cih Wu |
| 指導教授: | 侯嘉洪 Chia-Hung Hou |
| 關鍵字: | 電化學膜,電化水處理技術,活性氧物種,二氧化鈦複合碳膜,鈷螯合物破壞,鈷回收,廢塑膠瓶衍生活性碳, Electrochemical membranes,Electrified water treatment technologies,Reactive oxygen species,Co-EDTA decomplexation,TiO2 decorated electrified carbon membranes,Cobalt recovery,Waste PET-derived activated carbon, |
| 出版年 : | 2024 |
| 學位: | 博士 |
| 摘要: | 隨著產業的持續創新和升級,用水需求急劇增加,對水質的要求也日益提高,突顯廢水處理和循環再利用的重要性。工業廢水中常含有重金屬,對人體健康和環境構成嚴重威脅,特別是當這些金屬以穩定的金屬有機螯合物形式存在時。由於螯合物結構複雜,傳統水處理方法難以有效去除,因此,有效的解螯合 (Decomplexation) 技術對於處理這些螯合重金屬並促進金屬資源回收至關重要。
本研究通過開發新穎電化學膜(Electrochemical membrane)和使用廢塑料衍生的活性碳電極,實現對鈷金屬螯合物的有效破壞及釋放鈷自由離子的捕捉。這些功能化電化學膜旨在增強導電性,並提供豐富的反應位點來分解破壞有機污染物。透過產生反應性氧物種,如羥基自由基(•OH)、超氧陰離子(O2•–)和單線氧(1O2),並藉由二氧化鈦(TiO2)的引入顯著增強•OH的生成與貢獻,從而優化了反應動力學並為降解機理提供了新見解。此外,TiO2碳複合電化學膜在光電化學程序中表現出優異的降解及解螯合性能,在20分鐘內去除了超過90%的EDTA-Na2,並在180分鐘內分解了約50%的Co-EDTA,強調了氫氧自由基在提升解螯合效率中的關鍵作用。此外,通過光電化學程序亦成功於陰極回收鈷,並驗證該膜在處理半導體實場含鈷螯合廢水的有效性。 此外,本研究提出了一種高效且可持續的離子捕捉方法,利用廢PET塑料瓶製成活性碳電極,並應用於電容去離子技術(Capacitive deionization)中。經1000°C製備的PET衍生電極展現出1443 m2/g的高比表面積、顯著的中孔率(Vmeso/Vtot為41.3%)和良好的導電性,從而實現了卓越的離子捕捉性能和高效節能的脫鹽效果。此方法不僅通過回收廢PET有效解決塑料廢棄物污染問題,還提供一種可持續的離子捕捉和水質淨化解決方案。 總體而言,本研究引入新穎功能性電化學膜於電化水處理技術中,提升鈷金屬螯合物的破壞與回收過程,並展示廢料衍生材料在提供可持續水淨化解決方案中的巨大潛力。 Industrial wastewater frequently contains heavy metals, posing serious risks to both human health and the environment, particularly when these metals exist in the form of stable metal-organic chelates. These chelates are difficult to remove using traditional water treatment methods due to their complex structures, emphasizing the need for advanced technologies that can break down these compounds and recover valuable metals. This study advances electrochemical water treatment by developing innovative electrochemical membranes and utilizing waste-derived activated carbon electrodes. The functionalized electrochemical membranes are designed to enhance conductivity and provide abundant reactive sites for decomposing organic pollutants. These membranes generate reactive oxygen species (ROS) such as •OH, O2•–, and 1O2, with TiO2 integration significantly boosting •OH generation. This observation deepens our understanding of degradation mechanisms and optimizes reaction kinetics. In a photo-assisted electrochemical reactor, the TiO2 decorated electrified membrane demonstrated over 90% EDTA-Na2 removal in 20 minutes and approximately 50% Co-EDTA decomposition within 180 minutes. These results demonstrated its ability to decomplex EDTA-chelated cobalt and successful cobalt recovery through a photo-electrochemical process. The membrane's performance was further validated in the treatment of real semiconductor wastewater containing cobalt complexes. Furthermore, the study proposes a promising and efficient method for capturing liberated ions released from heavy metal complexes. Activated carbons derived from waste PET bottles were developed for ion capture using capacitive deionization (CDI) technology. The PET-derived electrode prepared at 1000°C exhibited a high surface area of 1443 m2/g, significant mesoporosity (Vmeso/Vtot of 41.3%), and good conductivity. These properties of PET-based electrodes enabled outstanding ion capture performance and energy-efficient desalination using CDI. This approach not only addresses the issue of plastic pollution by recycling waste PET but also offers an eco-friendly solution for ion capture. Overall, the research presents key innovations in electrochemical membrane technology, demonstrates the effective degradation and recovery of cobalt from metal-organic complexes, and showcases the potential of waste-derived electrodes in CDI as a sustainable solution for advanced water treatment. |
| URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/96208 |
| DOI: | 10.6342/NTU202404450 |
| 全文授權: | 同意授權(限校園內公開) |
| 電子全文公開日期: | 2029-10-06 |
| 顯示於系所單位: | 環境工程學研究所 |
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