| 研究生: |
王藝森 Wang, Yi-Sen |
|---|---|
| 論文名稱: |
具氧化還原活性之金屬有機骨架與其奈米複合材料於水相超電容中的應用 The applications of redox-active metal─organic frameworks and their nanocomposites in aqueous supercapacitors |
| 指導教授: |
龔仲偉
Kung, Chung-Wei |
| 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: | 2020 |
| 畢業學年度: | 108 |
| 語文別: | 中文 |
| 論文頁數: | 122 |
| 中文關鍵詞: | 石墨烯奈米緞帶 、氧化石墨烯 、氧化錳 、氧化還原躍遷 、超電容 、以鋯為基底的金屬有機骨架 |
| 外文關鍵詞: | graphene nanoribons, graphene oxide, manganese oxide, redox hopping, supercapacitor, zirconium-based MOF |
| 相關次數: | 點閱:133 下載:3 |
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本研究分為兩個部分,第一部分將以鋯為基底的金屬有機骨架 (Zirconium-based metal–organic frameworks, Zr-MOFs)在室溫下直接生長在奈米碳材,包括石墨烯奈米緞帶 (Graphene nanoribbons, GNRs)以及氧化石墨烯 (Graphene oxide, GO),形成具導電性的奈米複合材料。其導電性以及孔洞性可藉由調整合成時MOF與碳材之間的比例而具高度可調性,而具氧化還原活性的錳活性中心,藉由後修飾的方式安裝至奈米複合材料的MOF結構上,使得電荷在MOF骨架內有氧化還原躍遷(redox hopping)的途徑可以傳遞,之後在水溶液態的電解質中探討MOF-GNR以及MOF-GO複合材料的擬電容表現。利用碳材的高度導電性以及MOF骨架中高密度具氧化還原活性的錳位置,使得經錳修飾的奈米複合材料相較於原始的錳修飾MOF以及錳修飾的碳材具有更好的擬電容表現。第二部分則是利用不同孔洞結構的Zr-MOFs,藉由後修飾安裝上具氧化還原活性的錳位置,使電荷同樣都能藉由redox hopping在不同骨架結構內傳遞。而後探討不同MOFs在水溶液態的電解質中的擬電容表現,找出具最佳超電容表現的Zr-MOF種類,為未來的研究提供Zr-MOFs在超電容應用方面較佳的結構選項。
In my thesis, nanocrystals of a zirconium-based metal–organic framework (Zr-MOF), UiO-66, were grown on two dimensionally distinct carboxylate-functionalized graphene-based materials, graphene oxide (GO) and graphene nanoribbons (GNRs), at room temperature to synthesize various electrically conducting UiO-66-carbon nanocomposites. The redox-active manganese sites were then installed in the UiO-66 and nanocomposites at room temperature by the solvothermal deposition in MOFs (SIM) technique to endue charge transport within the UiO-66 phase via redox hopping under electrochemical conditions. The electrochemical performances of these nanocomposites were investigated and compared with those of the Mn-decorated UiO-66 and Mn-decorated GO and GNRs. With the electrical conductivity provided by nanocarbons and the high-density redox-active manganese sites supported by the porous framework, the Mn-decorated nanocomposites exhibit better performances as the materials for pseudocapacitors than the pristine Mn-decorated MOF and nanocarbons.
To probe the effect of the pore structures of Zr-MOFs on the resulting electrochemical performances, four structurally distinct Zr-MOFs were used for the installation of manganese for gauging their pseudocapacitive behaviors. After decorated with Mn, the electrochemical performance of these Zr-MOFs were measured. The findings suggest that the manganese-decorated MOF-808 has a better electrochemical performance than other Mn-decorated Zr-MOFs, indicating that MOF-808 should be a better candidate for making nanocomposites for electrochemical purposes in future studies.
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