碳氣凝膠電容系統對水中重金屬離子競爭吸附之研究

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研究生：	李明翰 Ming-han Lee
論文名稱：	碳氣凝膠電容系統對水中重金屬離子競爭吸附之研究 Competitive Electrosorption of Metal Ions by Carbon Aerogel
指導教授：	秦靜如 Ching-ju Chin
口試委員:
學位類別：	碩士 Master
系所名稱：	工學院 - 環境工程研究所 Graduate Institute of Environmental Engineering
畢業學年度：	97
語文別：	英文
論文頁數：	82
中文關鍵詞：	碳氣凝膠紙、重金屬、競爭吸附
外文關鍵詞：	carbon aerogel, heavy metal, competitive electrosorption
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本研究旨在了解碳氣凝膠電極所建立之電容系統，在競爭吸附情況時，電容去離子化的情形。實驗使用重金屬溶液為氯化鉻、氯化銅及氯化鉛，初始濃度皆為0.5 毫莫爾濃度，在多金屬系統的競爭組合為兩金屬的氯化銅及氯化鉛、氯化銅及氯化鉻與三金屬的氯化鉻、氯化銅及氯化鉛。單一金屬系統為比較離子半徑及價數不同在去除重金屬離子的能力，而多金屬系統則為研究不同電壓及競爭情況下去除的情況。
在單一金屬系統去除效率方面，金屬在相同價數情況下，銅的去除效率較鉛為高，是由於銅的離子半徑較小。而在不同價數的比較中，銅的去除效率也較鉻為高，是由於鉻價數較大，使得電容器僅能夠容納較少的鉻。在兩金屬組合的氯化銅及氯化鉛競爭下，鉛的去除效率較佳，氯化銅及氯化鉻組合中，銅的去除效率較佳。而在鉻、銅及鉛三金屬競爭情況下為去除效率為銅大於鉻，再大於鉛。
電壓可以影響兩金屬組合中的氯化銅與氯化鉛的去除能力，然而在有鉻金屬存在的狀況下，電壓並不能影響其對金屬的去除能力，且被吸附的金屬並不能隨著解除電壓而釋放出來。而在比較鉻、銅及鉛三金屬競爭的能力，鉻為三者中最佳，其次為鉛最後為銅。

The objective of this work was to understand the competitive electrosorption of heavy metal by capatative deionization (CDI) equipped with carbon aerogel. Single-metal-ion system was studied to understand the effects of ionic radius and valence on the removal of heavy metal ions by CDI. Electrosorption of multi-metal-ion was conducted to investigate the effects of the applied voltage and competitive electrosorption of Pb2+/Cu2+, Cu2+/Cr3+, and Pb2+/Cu2+/Cr3+.
The initial concentrations of all three heavy metals used in this work (i.e., CrCl3, CuCl2, and PbCl2) were 0.5 mM in either single-metal-ion or multi-metal-ion systems. The adsorption of Cu2+ was better than that of Pb2+ because the electrosorption efficiency increased with decreasing ionic radius when metal ions have the same valence. The adsorption of Cr3+ was less than that of Cu2+ because Cr3+ had higher charge and the capacitor could hold less Cr3+.
For Pb2+ / Cu2+ adsorption, the adsorption of Pb2+ was better than that of Cu2+. For electrosorption of Cu2+ / Cr3+, the adsorption of Cu2+ was better than that of Cr3+. For electrosorption of Pb2+ / Cu2+ / Cr3+, the order of the adsorption amount and rate from the largest and fastest was Cu2+, Cr3+, and Pb2+. The adsorption of Cr3+ was the most competitive, followed by the adsorption of Pb2+ and, then Cu2+. The applied voltage showed effects on the electrosorption Pb2+ / Cu2+, however, showed no effects on the experiments with Cr3+. When Cr3+ was in the system, Cr3+ helped metal ions be fixed on the carbon aerogel after the removal of the applied voltage.

Figure Captions………………………………………………………………………IV
Tables........................................................................................................................VIII
CHAPTER I INTRODUCTION………………………………………………….....1
1 General Background Information………………………………………..…..1
2 Objective……………………………………………………………………..3
CHAPTER II BACKGROUND…………………………………………………......4
1 Heavy Metal………………………………………………………………….4
1.1 Chromium……………………………………………………………..5
2.2 Copper………………………………………………………………...5
2.3 Lead…………………………………………………………………...6
2 Capacitive Deionization……………………………………………………...7
2.1 Removal of Impurities by the CDI Using Carbon Aerogel Electrodes.8
2.2 Advantages of the Capacitive Deionization…………………………..9
3 Factors Affect the Electrosorption of Carbon Aerogel Electrodes…...............9
3.1 Parameters of the Capacitance of Carbon Aerogel Electrodes………..9
3.2 Mechanisms of the Electrosorption of Carbon Aerogel Electrodes…11
4 Adorption of Heavy Metal Ions via Different Adsorbents………………….13
5 Carbon Aerogel……………………………………………………………..14
5.1 Aerogel………………………...…………………………………….15
5.2 The Preparation of Carbon Aerogel…………………………………15
5.3 The Characteristics of the Carbon Aerogel……………..…………...17
5.4 Applications of the carbon aerogel…………………………………..19
CHAPTER III MATERIALS AND METHODS…………………………………20
1 Materials……………………………………………………………………20
1.1 The Electrodes………………………………….…………………...20
1.2 The Reactor and the Monitoring Systems…………………………..22
1.3 Heavy Metal Solutions………………………………………...……22
2 The Method……………………………………………………………...…25
2.1 The Electrosorption of Heavy Metals………………………………25
2.2 Measurements of Ions and Characterization of Electrodes…………26
3 The Framework of This Study……………………………………………...29
CHAPTER Ⅳ RUSULTS AND DISCUSSION….………………………………30
1 Capacitive Deionization of Single Metal by Carbon Aerogel………………30
1.1 Electrosorption of Pb2+ by Carbon Aerogel……………….………...30
1.2 Electrosorption of Cu2+ by Carbon Aerogel…………………………33
1.3 Electrosorption of Cr3+ by Carbon Aerogel………………………....35
1.4 The Effect of Ionic Radius and Valence………………………….....37
2 Capacitive Deionization of Two Metals by Carbon Aerogel……………….38
2.1 Electrosorption of Pb2+ and Cu2+ by Carbon Aerogel…………...…..38
2.2 Electrosorption of Cu2+ and Cr3+ by Carbon Aerogel…………….…50
2.3 The Effect of Applied Voltage………………………………………66
3 Capacitive Deionization of Three Metals by Carbon Aerogel……………...71
3.1 Electrosorption of Pb2+, Cu2+, and Cr3+ by Carbon Aerogel………...71
3.2 Comparison of Single- and Multi-metals Systems…………………..75
CHAPTER Ⅴ CONCLUSION…………………………………………………...77
1 Conclusions…………………………………………………………………77
2 Suggestions…………………………………………………………………78
REFERENCES……………………………………………………………………...79

                                

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