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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 劉雅瑄(Ya-Hsuan Liou) | |
dc.contributor.author | Wei-Li Lu | en |
dc.contributor.author | 呂偉立 | zh_TW |
dc.date.accessioned | 2021-06-17T02:31:14Z | - |
dc.date.available | 2022-08-25 | |
dc.date.copyright | 2017-08-25 | |
dc.date.issued | 2017 | |
dc.date.submitted | 2017-08-17 | |
dc.identifier.citation | Ahn, Y.H., 'Sustainable nitrogen elimination biotechnologies: A review', Process Biochemistry, 2006, 41, 1709–1721.
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/68700 | - |
dc.description.abstract | 電化學氧化法分解水中氨氮的技術已引起了廣泛的研究與應用。本研究之重點在於透過不同之尺寸穩定性陽極的材料製備方法及電化學氧化系統下降解氨氮,以達到最大氨氮轉換率及氮氣選擇性的目的。以陽極氧化法製備出二氧化鈦奈米管柱後,進行脫管再以濺鍍法及煅燒法來改質材料表面,最後製得披覆鉑之尺寸穩定二氧化鈦奈米洞陽極。實驗結果顯示,最佳的陽極氧化前處理條件為,電壓80 V、時間30分鐘、溫度15℃、含水量3%。最佳披覆鉑厚度為1 nm,最佳煅燒條件為400℃空氣中反應3小時;奈米孔洞可增加約4%到7%的表面積,同時提升產氯反應性的效果;披覆鉑之電極煅燒時,在空氣中400℃燒3小時之材料會具有最佳的反應效果,但溫度高於600℃會使表面的鉑金屬熔解而使電極失去反應性。
批次實驗結果顯示,披覆鉑鈦奈米洞電極可透過氯離子轉換成氯氣後再去降解氨氮物質,氨氮降解率為100%,而且轉換至氮氣的選擇性也高達94%。最佳的電化學氧化實驗系統為電壓3 V、電解液溫度30℃、酸鹼值pH=7。材料表面分析結果顯示,電極表面鉑之氧化態中,零價鉑比例越高時會吸附氫於鉑表面而抑制整體電解反應的進行。反應動力學實驗結果顯示,陽極將氯離子轉換成氯氣之反應為二階反應,本研究的最佳電極之產氯的反應速率常數k=3.34×〖10〗^(-4) (1/Ms),電流效率高達20.45%。本研究結果指出,在反應的過程中氯離子會先與電極表面的鉑反應形成吸附態之氯自由基,氯自由基可能再兩兩結合形成氯氣,或是再一個氯離子與吸附態氯自由基反應形成氯氣,氯氣再溶解在水中形成次氯酸。而整個過程中基材的鈦板會扮演一個幫助氯自由基脫附的角色而提升反應性的角色。當反應形成的次氯酸後會再跟氨氮分反應進而降解氨氮汙染物。因此,本研究結果將有助於開發高選擇、高轉換率之氨氮降解之電化學氧化系統。 | zh_TW |
dc.description.abstract | The electrochemical oxidation process applied in the removal of ammonia in water has been demonstrated to be an effective treatment process. The aim of this study is to enhance the chlorine production, ammonia conversion and nitrogen selectivity through electrochemical oxidation process with different prepared TiO2 nano-hole dimensionally stable anodes. Titanium sheets were treated with anodization method of voltage 80 V, reaction time 30 min, temperature 15℃, electrolyte with fluoride ion and 3% water content, which is able to produce numerous nano-hole pore on surface. Next step, surface modification and calcination were applied. We succeeded in using TiO2 nano-hole dimensionally stable anodes as the working electrodes of electrochemical oxidation process to transform chlorine ions to chlorine. Finally, ammonia was degradated.
Through different calcination treatments, the Platinum on electrode surface forms in different oxidation state. Moreover, increasing the amount of Pt(0) restrains the reaction due to the adsorbed atomic hydrogen on Pt(0). The experiment result compiled with computational kinetic simulation showed that the dynamic behavior of our reaction system is a second order reaction. Furthermore, we derived the empirical formula of the degradation ammonia system and built the mechanism of reaction system. The production of adsorbed •Cl radicals generated from Cl− discharge reactions, and then the adsorbed •Cl· combines with Cl− or another adsorbed• Cl· and releases Cl2. | en |
dc.description.provenance | Made available in DSpace on 2021-06-17T02:31:14Z (GMT). No. of bitstreams: 1 ntu-106-R04224113-1.pdf: 16962935 bytes, checksum: 1eb60b4395ae6794addb960dbe073d57 (MD5) Previous issue date: 2017 | en |
dc.description.tableofcontents | 中文摘要 I
Abstract II 目錄 III 圖目錄 VII 表目錄 XI 第一章 緒論 1 1.1 研究緣起 1 1.2 研究目的與內容 2 第二章 文獻回顧 3 2.1. 氨氮廢水之簡介 3 2.1.1. 氨氮之危害 4 2.1.2. 氨氮污染源 6 2.2. 氨氮去除技術之簡介 8 2.2.1. 生物移除氨氮技術 8 2.2.2. 離子交換法 11 2.2.3. 薄膜蒸餾法 13 2.2.4. 電透析法 14 2.2.5. 氨氮吹脫法 15 2.2.6. 折點加氯法 16 2.2.7. 電化學氧化法 18 2.3. 電化學氧化法之回顧 19 2.3.1. 介質電解法 19 2.3.2. 電化學氧化法降解氨氮之效能指標 23 2.3.3. 電極材料 26 2.4. 二氧化鈦電極之簡介 29 2.4.1. 二氧化鈦基本性質 29 2.4.2. 二氧化鈦電極之製備 31 2.4.3. 二氧化鈦奈米洞電極 33 第三章 研究方法與設備 34 3.1. 實驗設計 34 3.2. 電極材料製備 35 3.2.1. 奈米洞電極製備 35 3.2.2. 電極表面改質 36 3.3. 批次實驗 37 3.3.1. 產氯實驗 37 3.3.2. 氨氮降解實驗 38 3.3.3. 電解液影響實驗 39 3.4. 污染物與產物分析方法 40 3.4.1. 餘氯檢測 40 3.4.2. 氨氮檢測 41 3.4.3. 硝酸鹽氮檢測 41 3.4.4. 亞硝酸鹽氮檢測 41 3.5. 材料物化特性分析 42 3.5.1. 場發射掃描式電子顯微鏡暨能量散佈分析儀 42 3.5.2. X射線光電子能譜分析儀 43 3.5.3. 原子力顯微鏡 44 3.6. 電化學特性分析 45 3.6.1. 線性掃描伏安法 45 3.6.2. 循環伏安法分析 47 第四章 結果與討論 48 4.1. 二氧化鈦奈米洞電極之最佳前處理條件之選定 48 4.1.1. 電極種類之選定 49 4.1.2. 二氧化鈦奈米洞電極之最佳前處理條件之選定-反應電壓 50 4.1.3. 二氧化鈦奈米洞電極之最佳前處理條件之選定-反應時間 52 4.1.4. 二氧化鈦奈米洞電極之最佳前處理條件之選定-反應溫度 54 4.1.5. 二氧化鈦奈米洞電極之最佳前處理條件之選定-含水量 54 4.2. 電化學氧化法產活性氯物種動力學實驗 56 4.2.1. 電化學反應系統建置-反應電壓之決定 56 4.2.2. 電化學反應系統建置-電解液酸鹼值 57 4.2.3. 電化學反應系統建置-電解液溫度 58 4.2.4. 電化學反應系統建置-電解液濃度 61 4.2.5. 電極表面改質-披覆鉑厚度 64 4.2.6. 電極材料後處理-煅燒氣氛 65 4.2.7. 電極材料後處理-煅燒溫度 66 4.2.8. 電極材料後處理-煅燒升溫程序 67 4.2.9. 電極材料後處理-煅燒時間 69 4.2.10. 電極材料後處理-煅燒順序 69 4.3. 電化學氧化法降解氨氮動力學實驗 75 4.3.1. 空白實驗 75 4.3.2. 降解氨氮動力學實驗 77 4.3.3. 氨氮濃度之影響 79 4.3.4. 氯離子濃度之影響 81 4.3.5. 電極耐用性測試 82 4.4. 反應機制探討 83 4.4.1. 電化學特性分析 83 4.4.2. 孔徑與產氯反應性 85 4.4.3. 披覆鉑氧化態對產率反應性之影響 89 4.4.4. 反應機制 96 第五章 結論與建議 103 5.1. 結論 103 5.1. 建議 105 參考資料 106 附錄 118 | |
dc.language.iso | zh-TW | |
dc.title | 製備穩定二氧化鈦奈米洞陽極轉換水中氨氮為氮氣之研究 | zh_TW |
dc.title | Fabrication of stable TiO2 nano-hole anodes for ammonia transformation to nitrogen | en |
dc.type | Thesis | |
dc.date.schoolyear | 105-2 | |
dc.description.degree | 碩士 | |
dc.contributor.oralexamcommittee | 林進榮,官文惠,胡景堯,鄧茂華 | |
dc.subject.keyword | 電化學氧化法,陽極氧化法,尺寸穩定性陽極,氨氮, | zh_TW |
dc.subject.keyword | Electrochemical oxidation,Anodization,Dimensionally stable anodes(DSA),Ammonia, | en |
dc.relation.page | 124 | |
dc.identifier.doi | 10.6342/NTU201703800 | |
dc.rights.note | 有償授權 | |
dc.date.accepted | 2017-08-18 | |
dc.contributor.author-college | 理學院 | zh_TW |
dc.contributor.author-dept | 地質科學研究所 | zh_TW |
顯示於系所單位: | 地質科學系 |
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