| 研究生: |
林哲辰 Lin, Zhe-Chen |
|---|---|
| 論文名稱: |
以金屬有機骨架為模板合成的高螢光強度碳量子點及其於汞離子感測的應用 Synthesis of Highly Fluorescent Carbon Quantum Dots inside the Matrix of Metal-Organic Frameworks and Their Application in Mercury(II) Ions Detection |
| 指導教授: |
李玉郎
Lee, Yuh-Lang |
| 學位類別: |
碩士 Master |
| 系所名稱: |
工學院 - 化學工程學系 Department of Chemical Engineering |
| 論文出版年: | 2024 |
| 畢業學年度: | 112 |
| 語文別: | 中文 |
| 論文頁數: | 137 |
| 中文關鍵詞: | 金屬有機骨架修飾碳量子點 、高螢光量子產率 、金屬離子感測 |
| 外文關鍵詞: | Metal-organic framework-modified carbon quantum dots, high fluorescence quantum yield, metal ion sensing |
| 相關次數: | 點閱:109 下載:0 |
| 分享至: |
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本篇研究使用Ship in a bottle的概念,以溶劑熱法將鄰苯二胺、檸檬酸做為合成碳量子點(Carbon quantum dots, CQDs)的前驅物,並利用不同孔洞大小之金屬有機骨架(Metal-organic frameworks, MOFs) Zr-MOF-808及Zr-UiO-66,做為控制碳量子點成長的模板,藉此限制碳量子點的成長大小,以獲得均一尺寸的碳量子點,並探討其光學性質的變化,後續應用於螢光感測中。實驗中首先獲得CQD/MOF-808及CQD/UiO-66的複合材料,藉由SEM、XRD、ASAP、FTIR、UV、PL等儀器分析其性質,SEM及XRD結果顯示外觀及結晶結構保持一致,顯示MOFs的結構沒有因為合成CQDs而被破壞。ASAP結果也顯示出兩種MOFs的孔洞皆因為合成CQDs後消失,間接證明CQDs成功成長於MOFs的孔洞中。後續為了更進一步探討CQDs的性質,利用蝕刻法將MOFs破壞掉,取出mf-CQD808及mf-CQD66,與不含MOFs合成情況下的碳量子點CQD,三種碳量子點藉由TEM、UV、PL、FTIR、XPS等儀器做性質差異的分析,由TEM結果顯示出經過MOFs控制尺寸後,CQDs的大小與孔洞大小相同,且更為均一。後續計算螢光量子產率,發現經過MOFs修飾及表面鈍化後的mf-CQD808及mf-CQD66可高達到95.81%及87.98%,由XPS的分析得知螢光量子產率隨氧元素的增加也跟著增加。最後將三種碳量子點應用於螢光感測中,發現皆對於汞離子有明顯的螢光焠滅(quenching)發生,進行感測極限(limit of detection, LOD)的測試,得到CQD的LOD為0.889 µM,而經過MOFs鈍化後的mf-CQD808及mf-CQD66能降低至0.541及0.440 µM。
This study utilizes the "Ship in a Bottle" concept to synthesize carbon quantum dots (CQDs) via a solvothermal method, using o-phenylenediamine and citric acid as precursors. Different pore-sized metal-organic frameworks (MOFs), specifically Zr-MOF-808 and Zr-UiO-66, were employed as templates to control the growth of CQDs, thereby limiting their size and achieving uniformity. The optical properties of these CQDs were then examined for potential applications in fluorescence sensing. Initially, CQD/MOF-808 and CQD/UiO-66 composites were synthesized and characterized using SEM, XRD, ASAP, FTIR, UV, and PL techniques. SEM and XRD results confirmed that the appearance and crystalline structure of the MOFs remained unchanged, indicating that the MOF structures were not disrupted during CQD synthesis. ASAP analysis further revealed that the pores of MOFs were filled post-CQD synthesis, indirectly confirming the successful growth of CQDs within the MOF pores.To further investigate the properties of the CQDs, the MOFs were etched away to isolate mf-CQD808 and mf-CQD66, which were compared to CQDs synthesized without MOFs. Characterization via TEM, UV, PL, FTIR, and XPS showed that the sizes of the MOF-templated CQDs matched the pore sizes and exhibited greater uniformity. The fluorescence quantum yields of mf-CQD808 and mf-CQD66 reached 95.81% and 87.98%, respectively, with XPS analysis revealing that the fluorescence quantum yield increased with the oxygen content. In fluorescence sensing applications, all CQDs exhibited significant quenching in the presence of mercury ions. The limit of detection (LOD) tests demonstrated that the LOD for CQDs was 0.889 µM, while the LODs for mf-CQD808 and mf-CQD66 were reduced to 0.541 µM and 0.440 µM, respectively, after MOF passivation.
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