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系統識別號 U0002-1507202009553400
中文論文名稱 以改質活性碳為顆粒電極之三維電極程序處理含硝基苯的廢水
英文論文名稱 Granular activated carbon loaded with copper as particle electrodes in three-dimensional electrochemical process for treating nitrobenzene-containing wastewater
校院名稱 淡江大學
系所名稱(中) 水資源及環境工程學系碩士班
系所名稱(英) Department of Water Resources and Environmental Engineering
學年度 108
學期 2
出版年 109
研究生中文姓名 陳子懿
研究生英文姓名 Tzu-Yi Chen
學號 608480157
學位類別 碩士
語文別 英文
第二語文別 中文
口試日期 2020-07-03
論文頁數 47頁
口試委員 指導教授-李奇旺
委員-彭晴玉
委員-陳孝行
中文關鍵字 三維電化學  吸附  活性碳  顆粒電極  硝基苯  化學需氧量  銅負載 
英文關鍵字 three-dimensional electrochemical  Adsorption  Granular activated carbon (GAC)  Particle electrode  Nitrobenzene (NB)  COD removal  Copper loaded GAC 
學科別分類 學科別應用科學環境工程
中文摘要 利用三維電極系統去除含NB廢水。該系統由銥銠合金包覆的鈦板作為陽極,碳板作為陰極以及負載銅的活性碳作為顆粒電極所組成。首先探討pH以及銅溶液濃度對活性碳上銅負載比例的影響。對於三維電極系統,探討了攪拌方式,系統的電氧化能力(包括二維系統,新鮮活性碳的三維系統以及銅負載活性碳的三維系統),電壓梯度(0.9375, 1.875, 3.125, 6.25, 9.375 V/cm),以及反應時間對硝基苯去除效率的影響。
  結果顯示,在濃度為3g/L的銅溶液濃度以及pH 3的條件下能達到17.1 mg/g的負載比例。以機械攪拌方式並以新鮮活性碳作為顆粒電極的三維電極系統能達到96%的去除效率。以機械攪拌方式並以銅負載活性碳作為顆粒電極的三維電極系統能達到76%的去除效率。雖然新鮮活性碳的去除效率較高但單就電氧化能力而言,銅負載活性碳的去除效率高出新鮮活性碳8%。改變電壓梯度以及提高反應時間並不會提高去除效率,並在電壓梯度為1.875 V/cm反應時間為60分鐘時候能達到最好的去除效率。
英文摘要 NB-containing wastewater was treated using a three-dimensional electrode system (3DE) consisting of a titanium plate coated with ruthenium and iridium as an anode, a carbon plate as a cathode and granular activated carbon loaded with copper as particle electrodes (Cu-GAC). For the Cu-GAC, the effects of pH and concentration of copper solution on copper-loading ratio were investigated. For the 3DE, the stirring effect, the electro-oxidation capacity (including the 2DE and 3DE with virgin GAC and Cu-GAC as particle electrodes), voltage gradient (0.9375, 1.875, 3.125, 6.25, 9.375 V/cm) and reaction time on NB removal efficiency were investigated.
The results show that the maximum loading ratio of 17.1 mg Cu/g GAC was achieved at copper concentration of 3 g/L and pH 3. A removal efficiency of 96% and 76% can be achieved by the 3DE with virgin GAC and Cu-GAC, respectively. Although the removal efficiency of virgin GAC was higher, the removal efficiency of Cu-GAC as particle electrodes was 8% higher in terms of the electro-oxidation capacity alone. The change of voltage gradient and the increase of reaction time do not improve the removal efficiency. The best removal efficiency was achieved when the voltage gradient is 1.875 V/cm and the reaction time is 60 min.
論文目次 CONTENTS
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . i
中文摘要 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . ii
Abstract . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . iii
Contents . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . v
List of Tables . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . vii
List of Figures . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . viii
1 Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.1 Motivation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1
1.2 Objectives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 2
2 Literature reviews . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 4
2.1 Three-dimensional electrochemical process (3DE) . . . . . . . . . . . . 4
2.1.1 Comparison of 3D and 2D systems . . . . . . . . . . . . . . . . 4
2.1.2 3D system configuration . . . . . . . . . . . . . . . . . . . . . . 7
2.2 GAC and GAC loaded with metal . . . . . . . . . . . . . . . . . . . . . 10
2.3 Effects of voltage gradient . . . . . . . . . . . . . . . . . . . . . . . . . 13
3 Materials and Methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.1 Materials and Chemicals . . . . . . . . . . . . . . . . . . . . . . . . . . 14
3.2 Experimental setup . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 15
3.2.1 Reactor of Cu-loading GAC production . . . . . . . . . . . . . . 15
3.2.2 3DE reactor system . . . . . . . . . . . . . . . . . . . . . . . . . 16
3.3 Experiment methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
3.3.1 Pre-treatment of GAC . . . . . . . . . . . . . . . . . . . . . . . 19
3.3.2 Effects of copper concentration and reaction pH on the loading
of copper onto GAC . . . . . . . . . . . . . . . . . . . . . . . . 19
3.3.3 Effects of adsorption and electro-oxidation . . . . . . . . . . . . 20
3.3.4 Effect of mixing . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
3.3.5 Effect of electro-oxidation . . . . . . . . . . . . . . . . . . . . . 21
3.3.6 Effect of Voltage gradient . . . . . . . . . . . . . . . . . . . . . 21
3.3.7 Effect of reaction time . . . . . . . . . . . . . . . . . . . . . . . 21
3.4 Analytical methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
4 Results and Discussion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.1 Copper loaded on GAC . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.2 COD removal by vaporization . . . . . . . . . . . . . . . . . . . . . . . 26
4.3 COD removal by adsorption and electro-oxidation . . . . . . . . . . . . 28
4.4 COD removal by electro-oxidation . . . . . . . . . . . . . . . . . . . . . 31
4.5 COD removal by voltage gradient . . . . . . . . . . . . . . . . . . . . . 33
4.6 COD removal by reaction time . . . . . . . . . . . . . . . . . . . . . . . 36
5 Conclusions and suggestions . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
5.1 Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38
5.2 Suggestions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 39
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 40

LIST OF TABLES
2.1 Comparison of pollutant removal efficiency of 3DE & 2DE . . . . . . . 6
2.2 Loaded GAC with different metals . . . . . . . . . . . . . . . . . . . . 11
3.1 Chemicals and brands used in this study . . . . . . . . . . . . . . . . . 15
4.1 The copper loading ratio as a function of initial copper ions concentrations. 23
4.2 The t-test for removal efficiency of COD with different voltage gradient. 34

LIST OF FIGURES
3.1 Schematic diagram of the experimental set-up used for copper loading
reactor . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 16
3.2 Schematic diagram of the experimental set-up used for 3DE reactor . . 18
3.3 The electrode plates of the 3DE reactor. (a) Anode side without cov
ered, (b) Cathode side with covered. . . . . . . . . . . . . . . . . . . . 18
4.1 The copper loaded ratio as a function of pH. Initial copper ions con
centration = 3 g/L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
4.2 The copper speciation as a function of pH. Modeled using Mineql+. . . 25
4.3 SEM images 3000 X of Cu-GAC. (a) Cu-GAC SEM image, (b) Element
mapping images for copper. . . . . . . . . . . . . . . . . . . . . . . . . 26
4.4 The evaporation of NB under aeration. Experimental conditions: Aer
ation rate = 1.5 L/min, initial COD concentration = 2900 ∼ 3200 mg/L. 27
4.5 The evaporation of NB using magnet stirring. Experimental conditions:
Mechanic mixing (600 rpm), initial COD concentration = 2900 ∼ 3200
mg/L. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28
4.6 COD removal efficiency in single batch experiment for various processes,
including 2DE, 3DE process as well as adsorption. Voltage gradient =
1.875 V/cm (2DE and 3DE), Virgin GAC as particle electrodes (3DE
and adsorption) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 29
4.7 COD removal efficiency by 3DE and adsorption processes with virgin
GAC being repeatedly used three times, Voltage gradient = 1.875 V/cm. 30
4.8 COD removal efficiency for 2DE and 3DE with virgin GAC and Cu-GAC
as particle electrodes. Both virgin GAC and Cu-GAC were impregnated
at saturation NB for more than 24 hours before the experiments. Voltage
gradient = 1.875 V/cm. . . . . . . . . . . . . . . . . . . . . . . . . . . 32
4.9 COD removal efficiency by 3DE with virgin GAC and Cu-GAC as par
ticle electrodes. The virgin GAC and Cu-GAC being repeatedly used
three times. Both virgin GAC and Cu-GAC were impregnated at sat
uration NB for more than 24 hours before the experiments. Voltage
gradient = 1.875 V/cm. . . . . . . . . . . . . . . . . . . . . . . . . . . 33
4.10 COD removal efficiency under various voltage gradient with Cu-GAC
in 3DE system. These values are 1.5, 3, 5, 10 and 15 V. . . . . . . . . . 34
4.11 Energy consumption under various voltage gradient. These values are
represented 1.5, 3, 5, 10 and 15 V. . . . . . . . . . . . . . . . . . . . . . 35
4.12 COD removal efficiency by 3DE with Cu-GAC. Reaction time 120 min,
Voltage gradient = 1.875 V/cm. . . . . . . . . . . . . . . . . . . . . . . 37
4.13 COD removal efficiency by 3DE with Cu-GAC being repeatedly used
three times. Reaction time 120 min/times, Voltage gradient = 1.875
V/cm. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 37
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