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  • 學位論文

碳奈米複合材料與Eucalyptus globulus生物合成奈米銀粒子之應用

The Application of Using Carbon Nanocomposite and Biosynthesis of Silver Nanoparticles with Eucalyptus globulus

指導教授 : 陳生明

摘要


第一部分 利用石墨烯氧化物(GO)結合多層奈米碳管(MWCNT)固定發光胺(PLM)和中性紅(PNR)混合修飾薄膜,成功提升導電度和達到立體奈米層結構。可由SEM 和AFM得知PLM-PNR-MWCNT-GO修飾薄膜為菌絲狀的立體奈米組成,並由電化學系統得知其電化學活性、與pH值之相關性和穩定度。實驗得知此修飾薄膜對菸鹼醯胺腺嘌呤二核苷酸(NADH)之電化學催化反應呈現高電流與低電位,其靈敏度達288.9 μA mM-1 cm-2 (Eapp. = +0.1 V)、線性濃度測量範圍1.33×10-8 – 1.95×10-4 M,及偵測極限為1.33×10-8 M (S/N = 3);此外,另一線性濃度測量範圍為2.08×10-4 – 5.81×10-4 M,靈敏度達151.3 μA mM-1 cm-2。實驗證明石墨烯氧化物結合多層奈米碳管固定發光胺和中性紅混合修飾薄膜的奈米結構,可有效地提升對NADH的測量。 第二部分 本實驗提出簡單的電化學方法,利用均勻分散的氧化石墨烯氧化物(GO)和多層奈米碳管(MWCNT),製備靈敏的GO和MWCNT複合修飾電極,利用電化學檢測pyrazinamide(PZM)。透過穿透式電子顯微鏡(TEM)觀測表面形態,證實MWCNT被GO包覆。相較於單一的MWCNT或GO,MWCNT/GO複合修飾電極對PZM的還原反應電催化活性明顯優異,主要原因是由於MWCNT和GO存在協同效應,利用電化學循環伏安法(CV)和差分脈衝伏安法(DPV)研究PZM的還原反應,PZM的反應線性濃度範圍為37.5 – 1800 μM,具偵測極限5.54 μM(S/N = 3),靈敏度為38 μA mM-1 cm-2,此感測器具有良好的靈敏度和選擇性,對真實樣品中的PZM偵測結果可證實其精準度,除此之外,此電化學感測器對市售製藥中的PZM亦呈現很好的偵測結果。 第三部分 相較於化學和物理方法合成,利用葉子萃取物生物合成奈米銀粒子(AgNPs)對環境相對友善,此實驗利用單一步驟低溫合成過程製備AgNPs,葉子萃取物作為還原劑,還原出穩定的AgNPs。奈米粒子用多種儀器做分析,顯示他們的形態學、化學組成和生物活性,奈米結構、結晶特性、純度和形態學,利用掃描式電子顯微鏡(SEM)、原子力顯微鏡(AFM)、氣相色譜法–質譜法(GC/MS)、X光繞射(XRD)和循環福安法(CVs)觀測,粒子大小在100 – 500 nm,葉子汁濃度和金屬離子對AgNPs的生物合成有很大的影響,可以更詳細的研究說明生物奈米粒子合成的機制。此簡單、價格低和環保的AgNPs合成方法,對環境、生物技術和生物醫藥的應用十分有價值。

並列摘要


Part 1 Hybridization of poly(luminol) (PLM) and poly(neutral red) (PNR) has been successfully performed and further enhanced by a conductive and steric hybrid nanotemplate using graphene oxide (GO) and multi-walled carbon nanotubes (MWCNT). Morphology of PLM-PNR-MWCNT-GO mycelium-like nanocomposite is studied by SEM and AFM and it is electroactive, pH-dependent, and stable in the electrochemical system. It shows eletrocatalytic activity to NADH with high current response and low overpotential. By amperometry, it shows a high sensitivity of 288.9 μA mM-1 cm-2 to NADH (Eapp. = +0.1 V). Linearity is estimated in a concentration range of 1.33×10-8 – 1.95×10-4 M with a detection limit of 1.33×10-8 M (S/N = 3). Particularly, it also shows another linear range of 2.08×10-4 – 5.81×10-4 M with a sensitivity of 151.3 μA mM-1 cm-2. Hybridization and activity of PLM and PNR can be effectively enhanced by MWCNT and GO, performing an active hybrid nanocomposite for determination of NADH. Part 2 This study presents a simple electrochemical approach for preparing the graphene oxide (GO)/multiwalled carbon nanotubes (MWCNTs) composite by homogenous dispersion of MWCNTs and GO, which responds sensitively for the electrochemical determination of pyrazinamide (PZM). The surface morphological results by transmission electron microscope (TEM) confirmed that MWCNTs were wrapped with GO sheets. The MWCNTs/GO composite showed superior electrocatalytic activity towards the reduction of PZM when compared with either pristine MWCNTs or GO. The major reason for the efficient simultaneous detection at nanocomposite was the synergistic effect between MWCNTs and GO. The electrochemical reduction of PZM was investigated by cyclic voltammetry and differential pulse voltammetry. The response of PZM is linear over the concentration range from 37.5 – 1800 μM, with the detection limit (S/N = 3) of 5.54 μM and the sensitivity was found to be 38 μA mM -1 cm -2. The proposed sensor exhibits good sensitivity, selectivity and has shown potential for the detection of PZM in real samples with appreciable consistency and precision. In addition, the proposed electrochemical sensor showed good results towards the commercial pharmaceutical formulated PZM samples. Part 3 The preparation of nanostructured metal particles provides an environmentally friendly option, as compared to currently available chemical and/or physical methods. Here we have biosynthesized silver nanoparticles (AgNPs) from plant extracts. In this work, a single-step low-temperature biosynthetic route for producing AgNPs using Eucalyptus (Eucalyptus globulus) extract. Stable AgNPs were formed by treating solution using the plant extracts as reducing agents. These nanoparticles were analyzed by various characterization techniques to reveal their morphology, chemical composition, and bioactivity. Nanostructure size, crystal nature, purity and morphologies were characterized by scanning electron microscopy (SEM) and atomic force microscopy (AFM), Gas chromatography–mass spectrometry (GC/MS), X-ray diffraction (XRD) and Cyclic voltammetry (CVs). The particle size ranging from 100 to 500 nm and the shape of the plate and spherical structures could be controlled by changing the reaction temperature and leaf broth concentration. The concentrations of leaves extract and metal ion are playing an important role in the biosynthesis of AgNPs. More elaborate studies are required to elucidate the mechanism of biological nanoparticles synthesis. This simple, low cost and greener method for development of AgNPs may be valuable in environmental, biotechnological and biomedical applications.

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