全球發展造成水資源匱乏與工業用水激增，因此增加純淨水與硬水處理受到各地之關注。
電容去離子技術(Capacitive deionization, CDI)為一新穎的海水淡化技術，其原理為利用電吸附機制去除水中離子，具有低耗能、低成本、操作簡易與無二次汙染等優勢，應用層面廣泛，除可應用於脫鹽外，亦可應用於硬水軟化處理。
影響CDI技術的重要因素之一為電極材料之選擇，本研究其中一個目的為探討對環境友善之三種還原劑製備石墨烯為基本電極，進行鹽水與硬度離子之去除，其中以HMTA製備之石墨烯擁有最高之比電容量(82.71 F/g)，對NaCl去除率達4.4 %，並對硬度離子Ca2+、Mg2+可分別達到2.74與0.56 mg/g之電吸附量。石墨烯對Ca2+、Mg2+、Na+電吸附之離子選擇性為Ca2+ > Mg2+ > Na+。
本研究另一目的為製備奈米Mn/rGO複合材料，藉由添加奈米錳提升原始石墨烯之親水性與比電容(111.42 F/g)，並組成非對稱電容去離子系統去除硬度離子處理，對Ca2+、Mg2+、Na+ 分別達2.83、1.05與0.61 mg/g之吸附量，與對稱CDI系統相比，更有效提升其電吸附量。

Global development has led to water scarcity and increasing industrial water usage, so increasing pure water and treatment of hard water has received lots of attention worldwide.
Capacitive deionization (CDI) technology is a novel desalination technology. The principle of CDI is to remove ions in water by electrosorption mechanism, it has the advantages of low energy consumption, low cost, easy operation and no secondary pollution generated. CDI has a wide range of applications, in addition to desalination, it can also be applied to hard water softening treatment. One of the important factors affecting CDI technology is the selection of electrode materials. 
One of the objectives of this study was to investigate the differences of three environmentally friendly reducing agents used to prepare the graphene for removing NaCl and hardness ions. Among them, graphene prepared by HMTA has the highest specific capacitance (82.71 F/g), the NaCl removal efficiency is 4.4%, and the electrosorption capacity of hardness ions Ca2+ and Mg2+ can be achieved to 2.74 and 0.56 mg/g, respectively. The ion selectivity of graphene electrosorption is Ca2+ > Mg2+ > Na+.
Another purpose of this study is to prepare nano-Mn/rGO composites, which can improve the hydrophilic and specific capacitance (111.42 F/g) of the original graphene by adding nano-manganese. An asymmetric capacitive deionization system to remove the hardness ion was also compared in this study.
The electrosorption capacity of Ca2+, Mg2+, and Na+ was 2.83, 1.05, and 0.61 mg/g, respectively, in the symmetric CDI system. Compared with the symmetric CDI system, asymmetric capacitive deionization is more effective in increasing the electrosorption capacity.

目錄
第一章	研究緣起	1
1.1	研究起源	1
1.2	研究目的	2
第二章	文獻回顧	3
2.1	淡化技術	3
2.2	CDI技術	6
2.2.1	原理	7
2.2.2	常用電極材料	9
2.3	石墨烯	10
2.3.1	石墨烯之化學改質	11
2.3.2	石墨烯之金屬複合物合成	13
2.4	對稱/非對稱之電容去離子技術	15
2.5	電容去離子應用於硬水軟化	19
第三章	材料與方法	23
3.1	實驗架構	23
3.2	實驗藥品與設備	25
3.2.1	實驗藥品	25
3.2.2	實驗儀器與設備	26
3.3	電極材料之製作	27
3.3.1	氧化石墨烯(Graphene Oxide, GO)之製備	27
3.3.2	石墨烯(Reduced Graphene Oxide, rGO)之製備	29
3.3.3	水熱法-錳/石墨烯複合材料(Mn/rGO)之製備	31
3.4	電極之製備	33
3.5	分析方法	35
3.5.1	X射線繞射分析 (XRD)	35
3.5.2	掃描式電子顯微鏡分析 (SEM)	35
3.5.3	孔徑與表面積分析 (BET)	36
3.5.4	接觸角測定實驗 (Contact angle)	36
3.5.5	循環伏安法 (Cyclic Voltammetry, CV)	37
3.5.6	計時電位法 (Chronopotentiometry, CP)	38
3.5.7	計時電流法 (Chronoamperometry, CA)	38
3.5.8	電化學阻抗譜分析 (EIS)	38
3.5.9	差分電容最小測量值 (Differential capacitance minimum measurements)	39
3.5.10	感應耦合電漿原子發射光譜儀 (ICP-OES)	39
3.6	電容去離子技術 (Capacitive deionization, CDI)	40
3.6.1	電容去離子系統 (CDI system)	40
3.6.2	非對稱電容去離子系統 (Asymmetric CDI system)	40
第四章	結果與討論	42
4.1	以不同還原劑製成石墨烯應用於電容去離子技術	42
4.1.1	不同石墨烯之表面特性分析	42
4.1.2	不同石墨烯之電化學特性	52
4.1.3	不同石墨烯應用於電容去離子技術	64
4.2	利用電容去離子技術去除水中硬度	68
4.2.1	單一離子去除	68
4.2.2	多離子之競爭	72
4.3	以錳/石墨烯複合材料應用於非對稱電容去離子技術	77
4.3.1	錳/石墨烯複合材料之表面特性分析	77
4.3.2	錳/石墨烯複合材料之電化學特性	82
4.3.3	錳/石墨烯複合材料應用於不對稱CDI系統去除水中硬度	90
第五章	結論與建議	95

 
List of Figure
Figure 2.2.1.1 Schematic illustration of the working principle of ion removal in CDI. (a) In charging phase, ions are temporarily electroadsorbed in porous carbon electrodes. (b) In discharging phase, most of the ions are released back into the solution (Yu et al., 2016).	8
Figure 2.3.1.1 (a) SEM image (cross-sectional view), (b) TEM image (Mohanapriya et al., 2016).	12
Figure 2.3.2.1 Cyclic voltammograms of MORGO with RGO and Mn3O4       (Yao et al., 2018).	14
Figure 2.4.1 Comparison of NaCl conductivity change curves of the four CDI cells: (a) Cell CS and Cell C; (b) Cell CN and Cell C; (c) Cell CSN and Cell C (Yang et al., 2013).	17
Figure 2.4.2 The assembly of the four cells and corresponding quantified desalting performances (Yang et al., 2013).	18
Figure 2.5.1 Normalized concentration of ions : Na (▲), Mg (■), and Ca (□) at a flow rate of 4 mL / min using the AC cloth type electrode. The applied voltage was 1.5 V with the feed solution of 1000 μS / cm conductivity. The apparent surface area of each compartment was 25 cm2 (Seo et al., 2010).	21
Figure 2.5.2 The electrosorption performance for different monovalent anions under an applied voltage of 1.2 V (Yingzhen Li et al., 2016).	22
Figure 3.1.1 Experimental structure for CDI system.	24
Figure 3.3.1.1 Graphene oxide (GO) preparation procedure.	28
Figure 3.3.2.1 Graphene (rGO) preparation procedure.	30
Figure 3.3.3.1 Manganese/Graphene (Mn/rGO) preparation procedure.	32
Figure 3.4.1 Carbon electrodes prepared with a modified evaporation casting method.	34
Figure 3.6.2.1 Schematic diagram of the CDI system.	41
Figure 4.1.1.1 XRD patterns of (a) Graphene oxide (GO), (b) Dithionite-rGO, (c) NaBH4 -rGO and (d) HMTA-rGO.	43
Figure 4.1.1.2 SEM images of (a), (b) Dithionite-rGO, (c), (d) NaBH4-rGO and (e), (f) HMTA-rGO.	45
Figure 4.1.1.3 Pore volume distribution of (a) Dithionite-rGO, (b) NaBH4-rGO and (c) HMTA-rGO.	47
Figure 4.1.1.4 Contact angle images of (a) Dithionite-rGO, (b) NaBH4-rGO and (c) HMTA-rGO.	50
Figure 4.1.2.1 Cyclic voltammograms of (a) Dithionite-rGO, (b) NaBH4 -rGO and (c) HMTA-rGO at various scan rates.	53
Figure 4.1.2.2 Cyclic voltammograms of (a) Dithionite-rGO, (b) NaBH4-rGO and (c) HMTA-rGO at scan rate of 50 mV/s.	54
Figure 4.1.2.3 Mass normalized specific capacitance of different rGO with respect to the scan rates.	56
Figure 4.1.2.4 Charge-discharge curves of (a) Dithionite-rGO, (b) NaBH4-rGO and (c) HMTA-rGO at various current densities.	58
Figure 4.1.2.5 Charge-discharge curves of different rGO at current densities of 1 A/g.	59
Figure 4.1.2.6 The current-time response obtained at applied cyclic potential on different rGO.	61
Figure 4.1.2.7 The electrochemical impedance spectra (EIS) measured at frequency range of 100 kHz to 0.01 Hz for different rGO.	63
Figure 4.1.3.1 Electrosorption/desorption profiles of the (a)Dithionite-rGO, (b) NaBH4-rGO and (c) HMTA-rGO electrode in 50 ppm NaCl solution (at 1.0 V).	66
Figure 4.1.3.2 Electrosorption/desorption profiles of the different rGO electrode.	67
Figure 4.2.1.1 Electrosorption/desorption of the HMTA-rGO electrode in 200 mg/L  (a) NaCl (b) MgCl2 and (c) CaCl2 solution (at 1.0 V).	70
Figure 4.2.2.1 Electrosorption/desorption of the HMTA-rGO electrode in        200 ppm Ca - Mg solution (at 1.0 V).	73
Figure 4.2.2.2 Electrosorption/desorption of the HMTA-rGO electrode in        200 ppm Ca - Na solution (at 1.0 V).	74
Figure 4.2.2.3 Electrosorption/desorption of the HMTA-rGO electrode in        200 ppm Mg - Na solution (at 1.0 V).	74
Figure 4.2.2.4 Electrosorption/desorption of the HMTA-rGO electrode in        200 ppm Ca - Mg - Na mixture solution (at 1.0 V).	75
Figure 4.3.1.1 XRD patterns of (a) HMTA-rGO and (b) Mn/rGO electrode materials.	78
Figure 4.3.1.2 SEM images of (a) HMTA - rGO (b) Mn/rGO and (c) EDS analyses of Mn/rGO.	79
Figure 4.3.1.3 The contact angle measurement of (a) HMTA-rGO, (b) Mn/rGO.	81
Figure 4.3.2.1 Cyclic voltammograms of Mn/rGO at various scan rates.	83
Figure 4.3.2.2 Cyclic voltammograms of HMTA-rGO and Mn/rGO at scan rate of 50 mV/s.	83
Figure 4.3.2.3 Mass normalized specific capacitance of HMTA-rGO and Mn/rGO with respect to the scan rates.	84
Figure 4.3.2.4 Charge-discharge curves of Mn/rGO at various current densities.	86
Figure 4.3.2.5 Charge-discharge curves of HMTA-rGO and Mn/rGO at current densities of 1 A/g.	86
Figure 4.3.2.6 The current-time response obtained at applied cyclic potential on HMTA-rGO and Mn/rGO.	87
Figure 4.3.2.7 The electrochemical impedance spectra (EIS) measured at frequency range of 100 kHz to 0.01 Hz for HMTA-rGO and Mn/rGO.	88
Figure 4.3.2.8 Normalized differential capacitance curves of HMTA-rGO and Mn/rGO.	89
Figure 4.3.3.1 Electrosorption/desorption of the Mn/rGO and HMTA-rGO electrode in 200 ppm (a) NaCl (b) MgCl2 (c) CaCl2 solution (at 1.0 V).	92
Figure 4.3.3.2 Electrosorption/desorption of the Mn/rGO and HMTA-rGO electrode in 200 ppm Ca - Mg - Na mixture solution (at 1.0 V).	93
 
List of Table
Table 2.1.1 Year 2011 global annual desalted water production and estimated associated saline feed water flow rates and gaseous emissions (Lior, 2017).	5
Table 2.5.1 The ion radius, hydrated radius, and hydration ratio of different anions (Yingzhen Li et al., 2016).	22
Table 3.2.1.1 Manufactures and purity of experimental medicines.	25
Table 3.2.2.1 Manufacturers and model of equipment.	26
Table 4.1.1.1 Surface areas and porosity ratio of different rGO.	48
Table 4.1.1.2 Contact angle analyses of different rGO.	51
Table 4.1.2.1 Mass normalized specific capacitance (F/g) of different rGO with respect to the scan rates.	56
Table 4.1.3.1 Removal efficiency and electrosorption capacity of different rGO.	67
Table 4.2.1.1 Removal efficiency and electrosorption capacity of different cations.	71
Table 4.2.1.2 The ion radius, hydration radius, and hydration ratio of three cations (Yingzhen Li et al., 2016).	71
Table 4.2.2.1 Removal efficiency and electrosorption capacity of the HMTA-rGO electrode in different cations mixture solutions.	76
Table 4.3.1.1 EDS elemental compositions of the Mn/rGO composite materials.	79
Table 4.3.1.2 Surface areas and porosity ratio of HMTA-rGO and Mn/rGO.	80
Table 4.3.2.1 Mass normalized specific capacitance (F/g) of HMTA-rGO and Mn/rGO with respect to the scan rates.	84
Table 4.3.3.1 Removal efficiency and electrosorption capacity of the Mn/rGO and HMTA - rGO asymmetric CDI system in different mixture solution.	94

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