利用碳氣凝膠紙電容吸附處理水中銨離子之研究

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許琇茹(HSIU-JU,HSU) 查詢紙本館藏

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論文名稱

利用碳氣凝膠紙電容吸附處理水中銨離子之研究
(The removal of ammonium ion via the capacitive deionization using the carbon aerogel electrodes)

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摘要(中)

廢污水之氨氮主要來自工業生產與生活污水，其對生態具有多方面的危害，包括耗用水中溶氧、產生臭味、與造成水體優氧化等，因此考量其對環境與生物健康有一定程度之危害，許多國家皆設立法令控制其排放許可濃度，且越來越嚴苛。本研究使用碳氣凝膠紙為電極，利用電容去離子機制去除銨離子。於研究中，使用循環伏安法來分析碳氣凝膠電極之電化學特性，結果顯示電容量最高約為38 F/g，當提升掃速時比電容量會下降，但電容圖形維持相似的形狀。在電容吸附批次系統中，當初始銨離子濃度為40 ppm且外加電壓從1.0 V上升至1.6 V時，銨離子的去除量從0.15 mg/g上升到1.85 mg/g；而銨離子濃度由10 ppm提高至40 ppm且外加電壓1.1 V或1.6 V時，提升濃度可使去除量增加，但1.1 V時會因吸附飽和量有限而使去除量無法持續提升。並在電容吸附研究中，發現硝酸根離子與亞硝酸根離子的產生，推測具有氧化還原反應發生。電極穩定性與再生性結果，以循環伏安法連續掃描電極三百次，其圖形不隨掃描次數改變，而電容吸附實驗反覆充放電三次的情形下，導電度具有相同的下降與上升趨勢，且下降的幅度維持一致。

摘要(英)

Ammonium in wastewater are harmful to the environment for it is odorous, would consume oxygen and cause eutrophication. Therefore, the regulations on the ammonium have become stricter. This study focused on the removal of ammonium via the capacitive deionization using carbon aerogel electrodes. The electrochemical characteristics of carbon aerogel electrode were investigated vie cyclic voltammetry experiment. The results showed that the highest specific capacitance of carbon aerogel electrode is about 38 F/g. Removal of ammonium vie capacitive deionization were studied. The results showed that the removal amount of ammonium ion increases from 0.15 mg/g to 1.85 mg/g when the applied voltage increased from 1.0 V to 1.6 V with the initial ammonium ion concentration of 40 ppm. In the meantime, trace amount of nitrate and nitrite have been found, which may be due to the oxidation of ammonium ion. The stability of the electrode was established by repeating the cyclic voltammetry measurements at scan rate of 100 mV/s for 300 cycles, which showed 100 % retention. The carbon aerogel electrodes were regenerated in charge/discharge cycle, the conductivity profile suggested that the removal of ammonium ions was repeatedly for up to three cycles.

關鍵字(中)

★ 碳氣凝膠紙
★ 電容去離子
★ 電容吸附
★ 銨離子

關鍵字(英)

★ carbon aerogel
★ CDI
★ capacitance adsorption

論文目次

目錄
摘要 I
Abstract II
致謝 III
目錄 V
圖目錄 IX
表目錄 XI
第一章前言 1
1-1研究緣起 1
1-2 研究內容與目的 2
1-3 研究流程 3
第二章文獻回顧 4
2-1 電容去離子技術 4
2-1-1 電容器 5
2-1-2 電雙層理論（electric double layer, EDL） 6
2-1-3 特定吸附 7
2-1-4電雙層重疊 9
2-2 電容去離子技術之發展與應用 10
2-2-1 多孔洞碳電極 11
2-2-2 電容去離子之影響因素 14
2-2-3 電容去離子技術現況 17
2-3 水中之氨氮 20
2-3-1 基本特性 20
2-3-2 氨氮之危害 20
2-3-3 氨氮處理技術 21
2-3-4 管制現況 24
第三章實驗方法 25
3-1實驗藥品與設備 25
3-1-1實驗藥品 25
3-1-2 實驗設備 26
3-2實驗方法 29
3-2-1 碳氣凝膠特性分析 29
3-2-2 電極電容特性分析 30
3-2-3 電容吸附實驗 32
3-2-4 水質分析 34
3-2-5 去除量、脫附量計算 34
第四章結果與討論 36
4-1 電極表面特性分析 36
4-1-1表面結構分析 37
4-1-2比表面積與孔徑分佈 38
4-2 電容特性分析 40
4-2-1 掃描速率之影響 40
4-2-2 電解質濃度之影響 43
4-3 電容吸附現象 47
4-3-1 非電容吸附與電容吸附 47
4-3-2 電壓對去除氨氮之影響 52
4-3-3 初始濃度對去除氨氮之影響 62
4-3-4 綜合評估 66
4-4 含氮物質之宿命 67
4-4-1 硝酸根離子與亞硝酸根離子之量測 67
4-4-2 含氮物質反應推估 72
4-5 電極之穩定性與再生 76
4-5-1 電極之穩定性 76
4-5-2 電極之再生性 78
第五章結論與建議 79
5-1 結論 79
5-2 建議 81
附錄 82
參考文獻 83

圖目錄
Fig. 1-1 研究流程圖 3
Fig. 2-1 電容去離子示意圖 4
Fig. 2-2 Stern電雙層模型示意圖 8
Fig. 2-3 電雙層重疊示意圖 9
Fig. 2-4 多孔性碳材結構示意圖 13
Fig. 3-1 循環伏安法之電位控制圖 30
Fig. 3-2 理想電容之循環伏安圖 31
Fig. 3-3 三極式電解槽 32
Fig. 3-4 實驗系統架構 33
Fig. 3-5 採樣時間點示意圖 34
Fig. 4-1 碳氣凝膠氮氣吸脫附等溫線 38
Fig. 4-2 碳氣凝膠平均孔徑分布圖 39
Fig. 4-3 各掃描速率之碳氣凝膠電極循環伏安比電容圖。 42
Fig. 4-4各電解質濃度對碳氣凝膠電極之循環伏安比電容圖之影響 46
Fig. 4-5 DI水空白實驗之導電度變化 47
Fig. 4-6 非電容吸附之導電度變化情形 49
Fig. 4-7 初始濃度對非電容吸附量之影響 49
Fig. 4- 8 銨離子濃度與導電度隨時間之變化 51
Fig. 4-9 各電壓對溶液導電度之變化情形 53
Fig. 4- 10 電容吸附實驗之再現性 56
Fig. 4- 11 電容吸附實驗之導電度變化。 57
Fig. 4-12 電壓對銨離子去除量之影響 58
Fig. 4-13 施加電壓為1.1 V時銨離子之濃度變化 60
Fig. 4-14 電壓對銨離子脫附之影響 61
Fig. 4-15 初始濃度對去除量之影響 64
Fig. 4-16 初始濃度對去除效率之影響 65
Fig. 4-17 各施加電壓對溶液中硝酸根離子濃度之影響 69
Fig. 4-18 碳氣凝膠紙之FT-IR圖譜 70
Fig. 4-19 不同電壓之pH值變化 74
Fig. 4-20 碳氣凝膠紙之SEM圖 75
Fig. 4-21 重複掃描碳氣凝膠電極之CV圖變化 77
Fig. 4-22 連續充放電之導電度變化 78

表目錄
Table. 3-1 實驗藥品 25
Table. 4-1 碳氣凝膠表面積與孔徑特性 39
Table. 4-2 各掃描速率之碳氣凝膠電極循環伏安比電容值 42
Table. 4-3電容吸附前後碳氣凝膠紙元素分析結果 71
Table. 4-4 水中銨離子可能發生之反應 74

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指導教授

秦靜如

審核日期

2016-1-26

推文