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  • 學位論文

穀胱甘肽輔助聚合物金奈米團簇之合成並應用於硫化氫檢測

Glutathione assisted preparation of polymer-capped gold nanoclusters and their applications as hydrogen sulfide sensor

指導教授 : 張煥宗

摘要


螢光金奈米團簇由於具備良好的生物相容性、生命週期長及光穩定性高,已被廣泛應用於生物感測器、細胞顯影等不同領域。目前小分子硫醇化合物、DNA、蛋白質及聚合物都已成功被當作合成金奈米團簇時之模板。其中聚合物包覆之金奈米團簇其性質可藉由利用不同特性的聚合物作為模板來控制,但其合成仍十分繁瑣費時。本研究藉由使用穀胱甘肽來輔助聚合物包覆之金奈米團簇(polymer/GSH-Au NCs)的合成,使用聚二烯丙基二甲基氯化銨(polydiallyldimethylammonium chloride, PDDA)及聚苯乙烯磺酸鈉(poly(sodium 4-styrenesulfonate), PSS)兩種帶電特性不同的聚合物,探討聚合物種類與濃度對於polymer/GSH-Au NCs性質的影響。同時也探討合成時pH值、聚合物分子量、穀胱甘肽及金離子濃度等條件對於聚合物包覆之金奈米團簇合成的影響。在最佳條件下可以在2小時合成出具有穩定螢光性質的PDDA/GSH-Au NCs。穀胱甘肽在此系統中扮演還原劑角色以簡化聚合物包覆之金奈米團簇合成,而聚合物在此系統中則為包覆劑。PDDA/GSH-Au NCs在PDDA的包覆下可以穩定存在於不同pH值及高鹽類環境,我們同時也將此材料應用於硫化氫之偵測,硫化氫會與PDDA/GSH-Au NCs反應形成聚集體而導致其螢光下降。在最佳化條件下,此系統之偵測極限為0.25 M,並具有良好的選擇性、高靈敏度及檢測快速(反應可於10 分鐘完成)等優點。此系統也被成功應用至湖水樣品中硫化氫含量及氣態硫化氫的偵測,證明此系統於真實環境樣品中硫化氫濃度偵測之可行性。

並列摘要


Fluorescence gold nanoclusters (Au NCs) have been widely used in sensing and imaging due to its good biocompatibility, long lifetime, and outstanding photostability. Various kinds of compounds have been used as templates in the preparation of Au NCs, such as small thiol molecules, DNA, proteins and polymers. Among them, the properties of polymer-capped Au NCs can be controlled by using polymers with different physical and chemical properties. However, the preparation of polymer-capped NCs is still tedious and complicated. In this study, glutathione (GSH) assisted preparation of polymer/GSH-Au NCs has been demonstrated. Polydiallyldimethylammonium chloride (PDDA) and poly(sodium 4-styrenesulfonate) (PSS) were employed to study the effects of polymer and their concentrations on the properties of as-prepared polymer/GSH-Au NCs. The effects of pH conditions, molecular weight of polymer and concentrations of GSH and Au3+ were also investigated. PDDA/GSH-Au NCs with good stability can be prepared in 2 hours under optimal conditions. The major role of GSH is acting as reducing agent to simplify the preparation of polymer-capped Au NCs, while polymer serving as capping agent that protects as-prepared Au NCs against salt and changes in pH conditions. PDDA/GSH-Au NCs was further applied to develop H2S sensors owning to its good stability. H2S can react with PDDA/GSH-Au NCs and lead to aggregation and further quench the fluorescence of Au NCs. PDDA/GSH-Au NCs allowed detection of H2S down to 0.25 M in 10 minutes with the advantages of great stability against salt, sensitivity and selectivity. The practicality of this assay has also been validated by the detection of H2S in pond water samples and gaseous H2S.

參考文獻


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