研究生: |
張鈞堯 Chang, Chun-Yao |
---|---|
論文名稱: |
碳量子點/金屬有機骨架複合材料之製備及其於光催化產氫的應用 Preparing of Carbon Quantum Dots/Metal–Organic Frameworks Composites and Their Applications in Photocatalytic Hydrogen Evolution |
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: | 2023 |
畢業學年度: | 111 |
語文別: | 中文 |
論文頁數: | 140 |
中文關鍵詞: | 碳量子點 、後修飾金屬有機骨架 、螢光材料 、光催化產氫 |
外文關鍵詞: | Carbon quantum dots, Postsynthetic modification Metal Organic frameworks, photoluminescence, photocatalysis of hydrogen evolution reaction |
相關次數: | 點閱:42 下載:0 |
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本研究利用金屬有機骨架(Metal organic frameworks, MOFs) Ti-MlL-125作為載體,將其置於鄰苯二胺、檸檬酸等碳量子點(Carbon quantum dots, CQD)的前驅物中,以溶熱法來合成CQDs,嘗試將量子點包覆於MOF的孔洞中,製作CQD/MOF複合物。所製得的材料藉由SEM、XRD、BET、HRTEM、UV、PL、XPS、ICP、GC等儀器來分析其特性,並將其應用於光催化產氫。實驗結果顯示MOF在CQD合成前後的XRD及FTIR圖譜並無改變,顯示MOFs的結構沒有因CQD的合成程序而破壞。而UV及PL光譜分析發現,在波長500 nm 附近,CQD/MOF與一般溶熱法所合成的CQDs有相同的吸收訊號,但在500 nm光源的激發下,COD/MOF的放射波長(570 ~590 nm)相較於之後取出CQDs的放射波長有紅移現象。研究中亦藉由鹼的蝕刻來破壞MOF結構,將MOF中的CQDs取出,分析此CQDs的特性。由PL光譜分析發現這些CQDs的放射波長(439 ~530 nm)與CQD/MOF及一般合成所得的CQDs不同,並且會隨溫度的改變而有明顯的不同,這結果表示CQDs 確實包覆於MOF結構中,且包覆於MOF結構中的CQDs與未被包覆的有不同的特性。此外,CQDs的成長會受到MOF的存在及反應溫度的改變而變化。最後我們將此一材料應用做為光催化產氫的觸媒。實驗中證實此CQD/MOF具有實際的產氫效能,若再將白金添加至CQD/MOF上作為共觸媒(Pt/CQD/MOF),其在甲醇與水的混和液中,於模擬太陽光照射下,最佳條件能達到2213 µmole g-1 h-1的產氫速率。
In this study metal-organic frameworks (MOFs) Ti-MIL-125 is served as the templet and utilized o-phenylenediamine and citric acid as wprecursors of carbon quantum dots (CQDs) to prepare CQD/MOF composites by solvothermal method. After synthesized, the materials were analyzed by SEM, XRD, BET, HRTEM, UV, PL, XPS, ICP, GC to study their characteristics. Then, these composites were applied in photocatalytic hydrogen production.
Form the experiment data, the spectra of FTIR and XRD suggest the structure of MOF is intact after synthesized CQD. In the result of UV and PL spectra, showed that the absorption signal of CQD/MOF around a wavelength of 500 nm was similar to the surface group signal of CQDs synthesized by using conventional methods. However, upon excitation with a 500 nm wavelength light, CQD/MOF exhibited a redshift in the emission wavelength (570 ~ 590 nm) compared to the later extracted CQDs. In order to, confirm the encapsulation of CQDs within the MOF structure, an alkali etching process was employed to destroy the MOF structure and extract the CQDs. The PL spectral analysis of these extracted CQDs (emission wavelength: 439 ~ 530 nm) demonstrated distinct differences from CQD/MOF and conventionally synthesized CQDs, and its stand for their characteristics were significantly affected by temperature changes.
Finally, the CQD/MOF composites were applied as catalysts for photocatalytic hydrogen production. The experimental results confirmed their practical hydrogen production efficiency. When platinum was added as a co-catalyst (Pt/CQD/MOF), under simulated solar light irradiation, the optimal condition achieved a hydrogen production rate of 2213 µmole g-1 h-1 in a mixture of methanol and water.
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