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| 研究生： |
王建閎 Jian-Hong Wang |
|---|---|
| 論文名稱： |
生物啟發共價有機框架薄膜之製備及其應用於酸鹼中和以及鹽差能源高效產電 Bioinspired Covalent Organic Framework Membranes for High-Performance Energy Generation from Acid-Base Neutralization and Salinity Gradients |
| 指導教授： |
葉禮賢
Li-Hsien Yeh |
| 口試委員: |
郭紹偉
Shiao-Wei Kuo 吳嘉文 Chia-Wen Wu 王丞浩 Chen-Hao Wang 葉禮賢 Li-Hsien Yeh |
| 學位類別： |
碩士 Master |
| 系所名稱： |
工程學院 - 化學工程系 Department of Chemical Engineering |
| 論文出版年： | 2021 |
| 畢業學年度： | 109 |
| 語文別： | 中文 |
| 論文頁數： | 122 |
| 中文關鍵詞： | 奈米流體學 、離子傳輸 、共價有機框架 、滲透能源 、能源轉換 、離子電流整流 、光響應性 |
| 外文關鍵詞： | Nanofluidics, Ion transport, Covalent organic framework, Osmotic power, Energy conversion, Ion current rectification, Photo responsive |
| 相關次數： | 點閱：214 下載：1 |
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滲透能轉換是一種永續的清淨能源，因其可以利用離子選擇膜藉由逆向電透析法將存在於離子濃度梯度中的化學勢轉化為電能，近年來已引起了國際社會對此技術的廣泛興趣。為了提高滲透能源轉換的效能，至今為各種方法已經被許多研究團隊嘗試，但大部分方法都是使用「無序結構」的多孔膜材料或是孔徑大於 5 nm 的薄膜材料，因此限制了薄膜的離子選擇性，尤其是在高離子濃度下的離子選擇性。在本論文中，我們利用界面合成方法開發了兩種共價有機框架(COF)膜，包括： (i) 1,3,5-三醯基間苯三酚-三 (4-氨基苯基) 胺 (TFP-TPA) 和 (ii) 1,3,5-三醯基間苯三酚-對二氨基偶氮苯 (TFP-Azo) 兩種COF 膜。X射線繞射分析顯示 TFP-TPA 和 TFP-Azo COF 薄膜均具有高結晶性的有序孔洞結構；Brunauer-Emmett-Teller (BET) 等溫吸附實驗結果顯示 TFP-TPA 和 TFP-Azo COF膜具有分別約為 1.1 和 2.7 nm的主要孔徑和分別為520和1650 m2/g的高比表面積。因為TFP-TPA COF膜在強酸或強鹼溶液中都具有非常高的穩定性，所以我們首先將其應用於鹽差與酸鹼中和之滲透能源發電中。實驗結果顯示，TFP-TPA COF 膜在透過混合人工鹽湖水和河水的鹽差條件（500 倍的氯化鈉濃度梯度）下，可以達到創歷史新高的 26.9 W/m2功率密度，此外，在透過酸鹼中和 濃度1 M 的酸鹼對(ABP)的條件下，其功率輸出還可進一步放大到一個難以置信高的 144 W/m2 。
在第二個部分，我們則是將對365 nm 波長紫外線刺激具光響應性的 TFP-Azo COF 膜應用於滲透能轉換的應用上。 我們將已製備出的 TFP-Azo COF 膜與PET單孔膜（其尖端直徑為 450 nm）結合，發現在 10 mM KCl 溶液中，此複合膜具有接近 40倍的類二極體離子電流整流（ICR）效應，而最令人驚訝的是，在紫外線的照射後，ICR 效應可進一步提高至93倍的超高比率。類似的現象也能在滲透能轉換實驗中發現，在紫外線的照射後，於中性 pH 值環境下其每孔滲透產電功率可顯著地從 425提高到 805 pW，優於目前所有最先進的單孔滲透產電系統。
Osmotic energy conversion, one kind of sustainable clean energies, has recently attracted significant interest from international community because it is shown converting chemical potential energy existing in ionic gradients into electricity with ion-selective membranes by reverse electrodialysis. To boost the performance of osmotic energy conversion, many attempts have been made but most of the previous works were realized with “disordered” pore membranes or focused on the nanopore membranes with pore size larger than 5 nm which limits the ion selectivity especially in high ionic concentration. In this study, we develop two types of covalent organic framework (COF) membranes using the interfacial synthesis method, including (i) 1,3,5-triformylphloroglucinol-tris(4-aminophenyl)amine (TFP-TPA) and (ii) 1,3,5-triformylphloroglucinol-4,4′-azodianiline (TFP-Azo) COF membranes. The X-ray diffraction profiles indicated that both the TFP-TPA and TFP-Azo COF membranes have high crystalline and ordered pore structures, and the Brunauer-Emmett-Teller (BET) sorption isotherms show that the TFP-TPA and TFP-Azo COFs have major pore sizes of nearly 1.1 nm and 2.7 nm, respectively, and both have high BET surface areas (520 m2g‒1 for TFP-TPA and 1650 m2g‒1 for TFP-Azo). Therefore, we apply the first TFP-TPA COF membranes in the osmotic energy harvesting from salinity gradients and acid-base neutralization because this membrane has very high stability in either strong acid or base solutions. Results obtained show that the TFP-TPA COF membrane can achieve a record-high power density of 26.9 W/m2 by mixing synthetic salt lake water and river water (500-fold NaCl gradient) and the power can be further amplified to an unbelievable value of up to 144 W/m2 by mixing 1 M acid-base pair (ABP) through acid-base neutralization.
In the second project, we apply the TFP-Azo COF membrane, which has light responsive property under the stimulus of 365 nm UV light, in the osmotic energy conversion application. By integrating the fabricated TFP-Azo COF membrane with a PET single-pore (with tip diameter of 450 nm) membrane, we find that the composite membrane show diode-like ion current rectification (ICR) effect with a ratio of nearly 40 and the most surprising is the UV light can significantly improve the ICR effect to the degree of a ultrahigh ratio of 93 in 10 mM KCl solution. Similar finding can be found in the osmotic energy conversion where the osmotic power can be appreciably boosted from 425 to 805 pW per pore at mild neutral pH after UV irradiation, outperforming all of the state-of-the-art single-pore osmotic harvesters.
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