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標題: | 功能性奈米材料的開發於感測器及催化反應上的應用 Development of Functional Nanomaterials for Sensors and Catalytic Applications |
作者: | 央御 Anuj Anuj |
指導教授: | 廖尉斯 Wei-Ssu Liao |
關鍵字: | EW-CRDS,腔衰盪光譜,金屬納米粒子,傳感,光觸媒,農藥,抗生素, EW-CRDS,Cavity Ring-down Spectroscopy,Metal Nanoparticle,Sensing,Photocatalysis,Pesticides,Antibiotics, |
出版年 : | 2023 |
學位: | 博士 |
摘要: | 吸收光譜法可能是液相分析中最常用的光譜技術,因為它的簡單性和通用性。 然而,吸收光譜有一些明顯的局限性,即較低的靈敏度和檢測限。 倏逝波腔衰盪光譜 (EW-CRDS) 技術是 CRDS 的應用之一,CRDS 是一種在氣相中行之有效的技術。 EW-CRDS 被認為是研究具有較低檢測限和良好靈敏度的界面/表面現象的有前途的候選者。 EW-CRDS 是一種直接吸收光譜技術,通過監測兩個高反射鏡內光學腔中捕獲的光的衰減率來測量物質的吸光度。 該技術基於在光學腔內的二氧化矽界面上形成的倏逝波。 相比之下,EW-CRDS 技術利用漸逝波來表徵固體表面上的吸附物特性。 通過利用這項技術的多功能性、簡單性和直接解釋,我們的目標是將這項技術作為檢測前列腺特異性抗原 (PSA) 的靈敏探針來實施。
合成了大小均勻的金納米粒子 (AuNP) 作為敏感的報告基因,與硫醇修飾的靶 DNA 緊密結合。 當 AuNPs/目標 DNA 在細胞中流動時,緩衝的目標 DNA 可能與固定在二氧化矽表面上的適體 DNA 雜交。 EW-CRDS 已被引入用於不同分析物的界面研究。 倏逝波對材料吸收的微小變化高度敏感,這會導致衰盪時間常數發生顯著變化. 2.光催化是光引發的降解過程,其中光催化劑用於在紫外或可見光照射下通過氧化和/或還原反應分解污染物。 結合二氧化鋯(\ce{ZrO2}@Ru 和 \ce{ZrO2}@Au)納米結構的釕和金金屬納米粒子被開發為用於廢水修復的有前途的光催化劑。 這些納米結構是使用水熱法合成的,並通過多種技術進行了很好的表徵。 \ce{ZrO2} 表現出類似納米花的形態,而球形 Ru/Au NPs 單獨結合在 \ce{ZrO2}@Ru 和 \ce{ZrO2}@Au 納米複合材料的 \ce{ZrO2} 表面上。 研究了 \ce{ZrO2}@Ru 和 \ce{ZrO2}@Au 對敵草隆 (DI) 和甲基對硫磷 (MP) 農藥降解的光催化性能。 兩種納米結構在可見光照射下均表現出顯著的光催化活性。 此外,還進行了活性物質清除劑研究和質譜分析,以說明光催化降解機制。 農藥降解主要由羥基自由基通過氧化途徑控制。 此外,\ce{ZrO2}@Ru 的可重複使用性得到驗證,這揭示了它們降解有毒物質以實現環境賠償的巨大能力. 3. 由於抗生素廢水對環境的有害影響,禁止排放抗生素廢水已受到重視。 迄今為止,已經開發了多種技術來降解廢水中的抗生素。 在這項研究中,光解、光催化 (PC) 和光電催化 (PEC) 這三個系統已應用於磺胺甲噁唑 (SMZ) 和甲硝唑 (MNZ) 抗生素的降解。 已經開發了一種新型 PEC 反應器用於降解 SMZ 和 MNZ。 \ce{ZnBi2S4}、\ce{ZnBi2Se4} 和 \ce{ZnBi2Te4} 納米材料已使用水熱技術合成,以減少 SMZ 和 MNZ 抗生素。 這些催化劑的合成是通過使用簡單易行的水熱法完成的,並使用多種技術進行了很好的表徵。 合成後的納米材料顯示出從 FE-TEM 觀察到的納米棒狀形態。 該反應器是通過使用塗有合成納米材料的 ITO 電極製備的,以通過施加一定電壓來提高催化劑的效率。 與抗生素的常規光催化降解相比,在外部偏壓和可見光照射下,SMZ 和 MNZ 的降解效率要高得多 The implementation of evanescent wave cavity ring-down spectroscopy (EW-CRDS) has enabled the detection of prostate-specific antigen (PSA) with high sensitivity, achieving a sub-femtomolar limit of detection (LOD). PSA, an important biomarker for detecting prostate cancer, was targeted using gold nanoparticles (Au NPs) as a sensitive reporter. The Au NPs were strongly bound to the thiol-modified target DNA and flowed through a microfluidic channel where they hybridized with aptamer DNA immobilized on the silica surface. The adsorption kinetics of hybridization between the Au NPs/target and aptamer was measured using the Langmuir fit of adsorption equilibrium, and the LOD of the Au NPs/PSA sensor was found to be 0.54 fM, demonstrating the remarkable detecting proficiency of EW-CRDS. The evanescent wave is highly sensitive to small changes in absorption, making it an ideal technique for interfacial sensing. Furthermore, the excellent surface plasmonic properties of Au NPs make them a promising probe material for this process. In comparison, the substitution of 5-carboxy tetramethylrhodamine as a reporter led to a significantly lower LOD of 99.1 fM. Therefore, the EW-CRDS approach holds great potential as an efficient sensing technique for detecting malignant diseases and various biological reactions. 2. Photocatalysis is the light-initiated degradation process in which a photocatalyst is used to decompose pollutants through oxidation and/or reduction reactions under the illumination of ultraviolet or visible light. Ruthenium and gold metal nanoparticles incorporated zirconium dioxide (\ce{ZrO2}@Ru and \ce{ZrO2}@Au) nanostructures were developed as promising photocatalysts for wastewater remediation. These nanostructures were synthesized using a hydrothermal method and were well characterized with several techniques. \ce{ZrO2} exhibited a nanoflower-like morphology while spherically-formed Ru/Au NPs were individually incorporated on the \ce{ZrO2} surface in \ce{ZrO2}@Ru and \ce{ZrO2}@Au nanocomposites. The photocatalytic performance of ZrO2@Ru and ZrO2@Au was investigated for the degradation of diuron (DI) and methyl parathion (MP) pesticides. Both nanostructures exhibited remarkable photocatalytic activity under visible light exposure. Furthermore, the reactive species scavenger study and mass spectroscopy analyses were conducted to illustrate the photocatalytic degradation mechanism. Pesticide degradation was primarily governed by hydroxyl radicals via an oxidative pathway. In addition, the reusability of \ce{ZrO2}@Ru was validated, which reveals their immense capability for the degradation of toxic substances for environmental indemnity. 3. The harmful impact of antibiotic wastewater discharge on the environment has led to significant attention towards its reduction. Numerous techniques have been developed to degrade antibiotics present in wastewater. This study aims to investigate the efficacy of three approaches, namely photolysis, photocatalysis (PC), and photoelectrocatalytic (PEC), in degrading Sulfamethoxazole (SMZ) and Metronidazole (MNZ) antibiotics in wastewater. The degradation of antibiotics has been achieved using \ce{ZnBi2S4}, \ce{ZnBi2Se4}, and \ce{ZnBi2Te4} nanomaterials as catalysts. To synthesize these nanomaterials, an autoclave-based hydrothermal technique was employed, resulting in their nanorod-like morphology as observed through FE-TEM and SEM. The PC activity of these nanomaterials was evaluated under visible light irradiation. In order to improve catalyst efficiency, a novel PEC reactor was developed to investigate the degradation of SMZ and MNZ. This reactor utilized ITO glass electrodes coated with the as-synthesized nanomaterials and applied a certain voltage to enhance catalyst performance. The degradation efficiency of SMZ and MNZ was found to be higher when subjected to external bias and visible light illumination, in comparison to conventional photolysis and PC degradation methods for antibiotics. |
URI: | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/87351 |
DOI: | 10.6342/NTU202300679 |
全文授權: | 同意授權(限校園內公開) |
電子全文公開日期: | 2028-03-21 |
顯示於系所單位: | 化學系 |
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