利用碳氣凝膠紙電吸附於二氯化銅水溶液現象之探討

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廖仲洲(Jhong-Jhou Liao) 查詢紙本館藏

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論文名稱

利用碳氣凝膠紙電吸附於二氯化銅水溶液現象之探討
(Electrosorption of CuCl2 by Carbon Aerogel Composite)

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摘要(中)

近年來奈米科技的進步，帶動材料科學的發展，種種優異性質材料被相繼被開發出來，其中也發展出嶄新的電吸附材料－碳氣凝膠紙。碳氣凝膠因具備有奈米尺度的細微孔洞、良好的極化能力、高的導電度性和高表面積等，其種種優異的性質適合作為電吸附材，因此有鑑於此，本研究利用碳氣膠電極電吸附水中二氯化銅，控制電壓和濃度，監測溫度、導電度、電流、總銅離子濃度、一價銅離子濃度、氯離子濃度和pH的變化，以瞭解其電吸附重金屬的行為。
研究結果發現，電吸附初期，陽極含氧官能基的氧化反應會釋出氫根離子，而到電吸附後期，陰極上的銅離子和氫根離子可能作為電子失去者，以上所述氧化還原反應的發生均會造成水體中氫根離子持續不斷的累積而導致水體pH值下降和導電度上升。電吸附結果顯示，銅離子初始濃度，對銅之去除效率影響有限，在外加電壓分別為1.2 V與1.0 V時，銅離子的去除效率分別可達99 %和95 %以上，唯達平衡之時間，隨銅離子濃度升高而所縮短。
再生實驗中以pH為3的鹽酸來清洗碳氣凝膠紙的效果最佳，且經酸洗流程後再進行pH調整為10的氫氧化鈉來進行鹼洗，以去除不利於電吸附的氫根離子，碳氣凝膠紙經以上所述再生流程後，即可獲得與新的碳氣凝膠紙相似的電吸附特性。

摘要(英)

Carbon aerogel composite has good properties such as nanopores, high electrical conductivity, and high surface area; therefore, carbon aerogel composite is suitable for electrosorption. In this study, carbon aerogel composite was used to electro-adsorb CuCl2 in pure water. The influences of applied voltage and copper concentration on the electrosoprtion of CuCl2 were investigated. Temperature, conductivity, current, pH, and concentrations of total copper, cuprous and chloride ions were monitored. The result showed that, in the initial stage of electrosorption, hydrogen ions were released from the anode due to the oxidation of oxygen-containing functional groups on the carbon aerogel composite. Later, hydrogen ion may be released from cathode due to the reduction reactions from the functional groups on the carbon aerogel composite. Both reactions resulted in accumulation of hydrogen ions; as the consequence, the solution pH decreased and the conductivity increased. The removal efficiencies were similar (>95%) when the applied voltages were 1.0 V and 1.2 V. However, as the concentration of copper increased, the electrosorption equilibrium time decreased. It was also found that washing the carbon aerogel composite by the HCl solution of pH 3 has the best regenerate efficiency. Further washing by NaOH of pH 10 can wash out the free hydrogen ions in the pores and the washed carbon aerogel composite showed similar electrosoprtion behaviors to a new one.

關鍵字(中)

★ 電吸附
★ 碳氣凝膠紙

關鍵字(英)

★ Electrosorption
★ Carbon aerogel composite

論文目次

圖目錄..................................................................Ⅳ
表目錄...................................................................Ⅶ
第一章前言………………………………………………………………………1
1.1. 研究緣起……………………………………………………………………1
1.2. 研究目的……………………………………………………………………2
1.3. 研究流程……………………………………………………………………3
第二章文獻回顧…………………………………………………………………4
2.1. 碳氣凝膠紙…………………………………………………………………4
2.1.1. Carbon nanofoam 的基本簡介…………………………………………4
2.1.2. 碳氣凝膠的生成…………………………………………………………6
2.1.3. 碳氣凝膠紙的基本性質…………………………………………………8
2.1.4. 碳凝膠紙於環境工程的應用………………………………..…………12
2.2. 電離理論………………………………………………………..…………12
2.3. 電雙層與電吸附……………………………………………………………19
2.3.1. Helmholtz電雙層模型……………….…………………………………19
2.3.2. Stern 電雙層模型………………………………………………………20
2.3.3. 特定吸附…………………………………………………………………22
2.3.4. 電雙層電容器……………………………………………………………24
2.3.5. 電雙層與電吸附…………………………………………………………25
2.3.6. 多孔洞電極………………………………………………………………26
2.3.7. 特定吸附對電位的影響…………………………………………………27
2.4. 物種物化特性對總電容量的影響…………………………………………30
2.5. 碳氣凝膠紙之再生…………………………………………………………34
第三章實驗藥品、設備與方法…………………………………………………35
3.1. 實驗藥品與設備……………………………………………………………35
3.2. 監控流程……………………………………………………………………41
3.3. 實驗方法……………………………………………………………………43
3.3.1. 電吸附實驗………………………………………………………………43
3.3.2. 再生實驗…………………………………………………………………45
3.3.3. 碳氣凝膠紙定性分析……………………………………………………47
3.3.4. 水質分析…………………………………………………………………48
第四章結果與討論………………………………………………………………51
4.1. 碳氣凝膠紙特性分析………………………………………………………51
4.1.1. 表面微觀結構……………………………………………………………51
4.1.2. 表面孔隙分析……………………………………………………………53
4.1.3. 官能基的鑑定……………………………………………………………55
4.1.4. 氧化還原反應的判定……………………………………………………56
4.2. 槽體的測試…………………………………………………………………57
4.2.1. 空氣溶入所增加的導電度………………………………………………57
4.2.2. NaCl 的測試………………………….…………………………………58
4.3. CuCl2 電吸附………………………………………………………………59
4.3.1. 總銅濃度的變化…………………………………………………………59
4.3.2. 電流的變化………………………………………………………………62
4.3.3. pH…………………………………………………………………………63
4.3.4. 導電度……………………………………………………………………65
4.3.5. 銅離子的氧化還原反應…………………………………………………69
4.3.6. 氯離子……………………………………………………………………71
4.4. 銅濃度對吸附容量的影響…………………………………………………74
4.5. 電壓對吸附容量的影響……………………………………………………76
4.6. 銅離子濃度與電壓對物種分佈之影響……………………………………78
4.6.1. 氫根離子…………………………………………………………………78
4.6.2. 氯離子……………………………………………………………………81
4.7. 碳氣凝膠紙的再生…………………………………………………………83
4.8. 再生後的電吸附……………………………………………………………86
4.8.1. 再生方法一：酸洗->去離子水…………………………………………86
4.8.2. 再生方法二：酸洗->鹼洗->去離子水…………………………………88
第五章結論與建議………………………………………………………………91
5.1. 結論…………………………………………………………………………91
5.2. 建議…………………………………………………………………………92
參考文獻……… …………………………………………………………………94

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指導教授

秦靜如(Ching-Ju Chin)

審核日期

2006-7-24

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