電容去離子技術(Capacitive Deionization, CDI)原理為透過成對電極間施加低電壓，使水中離子受電場驅動移動至相反電荷的電極並儲存在電雙層中，達到去除離子與淨化水質的效果。金屬有機框架(Metal Organic Framework, MOF)為一種具良好離子吸附性能的奈米多孔材料，由金屬離子和有機配位基組成，其家族之一的沸石咪唑酯骨架(Zeolitic imidazolate framework, ZIF)中ZIF-8材料，具有MOF的結構，擁有特殊的熱與化學穩定性，易於調控晶格孔隙大小及性能，可廣泛應用於不同領域。
    本研究的第一部分以沸石咪唑酯骨架材料ZIF-8經高溫碳化與活化製備衍生碳材料，作為電極材料應用於CDI系統，探討碳化溫度(800°C、900°C)對其結構與電吸附性能的影響，進一步選用表現較佳之碳化溫度，於碳化前利用天然多酚化合物-單寧酸(tannic acid, TA)蝕刻形成中空HZIF-8結構，經碳化與活化以優化孔隙分布並提升效能。研究的第二部分將ZIF-8、聚醚碸(polyethersulfone, PES)與聚乙烯吡咯烷酮(polyvinylpyrrolidone, PVP)結合，以金屬酚結構(Metal-Phenolic Network, MPN)製備ZIF-8_PES_PVP複合薄膜，分析薄膜表面特性及孔洞結構，結合膜通量實驗探討薄膜截留水中鹽類離子之能力。
    原始ZIF-8_24hr經過800°C碳化與900°C活化後所得之ZIF-8_24hr_800c_900a，具備高比表面積2419.73 m²/g與良好比電容量(93.06 F/g)，並在CDI系統中擁有穩定的平均去除效率8.44%與平均電吸附量68.65 μmol/g， ZIF-8_24hr經蝕刻後的中空HZIF-8_24hr，經碳化與活化後所製得之HZIF-8_24hr_800c_900a展現更優異之性能，具備比表面積1802.62 m²/g，比電容量於掃描速率為1 mV/s時可高達118 F/g，並於CDI系統中擁有最佳平均去除率11.54%，最佳電吸附量99.13 μmol/g，且在多循環操作下仍具良好穩定性，顯示HZIF-8_24hr_800c_900a作為電極材料可有效提升整體CDI性能與循環穩定性，為研究中最具潛力之衍生多孔碳材料。
    藉由金屬酚結構(Metal-Phenolic Network, MPN)製備ZIF-8_PES_PVP複合薄膜，處理3.4 mM與34 mM NaCl溶液，擁有最高的平均鹽截留率15.41%、7.98%與最高平均鹽去除質量11592 mg、48163 mg，顯示結合ZIF-8於PES薄膜之改質能有效提升PES薄膜對鹽離子的截留能力，具備應用於水處理脫鹽之潛力。


    電容去離子技術(Capacitive Deionization, CDI)原理為透過成對電極間施加低電壓，使水中離子受電場驅動移動至相反電荷的電極並儲存在電雙層中，達到去除離子與淨化水質的效果。金屬有機框架(Metal Organic Framework, MOF)為一種具良好離子吸附性能的奈米多孔材料，由金屬離子和有機配位基組成，其家族之一的沸石咪唑酯骨架(Zeolitic imidazolate framework, ZIF)中ZIF-8材料，具有MOF的結構，擁有特殊的熱與化學穩定性，易於調控晶格孔隙大小及性能，可廣泛應用於不同領域。
    本研究的第一部分以沸石咪唑酯骨架材料ZIF-8經高溫碳化與活化製備衍生碳材料，作為電極材料應用於CDI系統，探討碳化溫度(800°C、900°C)對其結構與電吸附性能的影響，進一步選用表現較佳之碳化溫度，於碳化前利用天然多酚化合物-單寧酸(tannic acid, TA)蝕刻形成中空HZIF-8結構，經碳化與活化以優化孔隙分布並提升效能。研究的第二部分將ZIF-8、聚醚碸(polyethersulfone, PES)與聚乙烯吡咯烷酮(polyvinylpyrrolidone, PVP)結合，以金屬酚結構(Metal-Phenolic Network, MPN)製備ZIF-8_PES_PVP複合薄膜，分析薄膜表面特性及孔洞結構，結合膜通量實驗探討薄膜截留水中鹽類離子之能力。
    原始ZIF-8_24hr經過800°C碳化與900°C活化後所得之ZIF-8_24hr_800c_900a，具備高比表面積2419.73 m²/g與良好比電容量(93.06 F/g)，並在CDI系統中擁有穩定的平均去除效率8.44%與平均電吸附量68.65 μmol/g， ZIF-8_24hr經蝕刻後的中空HZIF-8_24hr，經碳化與活化後所製得之HZIF-8_24hr_800c_900a展現更優異之性能，具備比表面積1802.62 m²/g，比電容量於掃描速率為1 mV/s時可高達118 F/g，並於CDI系統中擁有最佳平均去除率11.54%，最佳電吸附量99.13 μmol/g，且在多循環操作下仍具良好穩定性，顯示HZIF-8_24hr_800c_900a作為電極材料可有效提升整體CDI性能與循環穩定性，為研究中最具潛力之衍生多孔碳材料。
    藉由金屬酚結構(Metal-Phenolic Network, MPN)製備ZIF-8_PES_PVP複合薄膜，處理3.4 mM與34 mM NaCl溶液，擁有最高的平均鹽截留率15.41%、7.98%與最高平均鹽去除質量11592 mg、48163 mg，顯示結合ZIF-8於PES薄膜之改質能有效提升PES薄膜對鹽離子的截留能力，具備應用於水處理脫鹽之潛力。

The principle of Capacitive Deionization (CDI) is based on applying a low voltage between a pair of electrodes, driving ions in water to migrate under the electric field toward oppositely charged electrodes, where they are stored in the electrical double layer (EDL), thereby removing ions and purifying the water. Metal-Organic Frameworks (MOFs) are a class of nanostructured porous materials with excellent ion adsorption properties, composed of metal ions and organic linkers. One subclass of MOFs, Zeolitic Imidazolate Frameworks (ZIFs), includes the ZIF-8 material, which possesses the typical MOF structure with unique thermal and chemical stability. Its tunable lattice pore size and functionality make it widely applicable in various fields.
In the first part of this study, the ZIF-8 material was subjected to high-temperature carbonization and activation to prepare derived carbon materials as electrode materials for CDI systems. The effects of carbonization temperatures (800°C and 900°C) on the structure and electro-adsorption performance were investigated. Based on the optimal carbonization temperature, tannic acid (TA), a natural polyphenolic compound, was used to etch the ZIF-8 to form a hollow HZIF-8 structure before carbonization. This aimed to optimize pore distribution and enhance performance through subsequent carbonization and activation.
In the second part of the study, a ZIF-8_PES_PVP composite membrane was fabricated by combining ZIF-8 with polyethersulfone (PES) and polyvinylpyrrolidone (PVP) via a Metal-Phenolic Network (MPN). The surface characteristics and pore structure of the membrane were analyzed. Membrane flux experiments were conducted to evaluate the salt ion rejection capability of the membrane.
The original ZIF-8_24hr, after carbonization at 800°C and activation at 900°C (denoted as ZIF-8_24hr_800c_900a), exhibited a high specific surface area of 2419.73 m²/g and a good specific capacitance of 93.06 F/g. In the CDI system, it achieved a stable average ion removal efficiency of 8.44% and an average electrosorption capacity of 68.65 μmol/g. After etching, the hollow HZIF-8_24hr, when carbonized and activated to form HZIF-8_24hr_800c_900a, showed even better performance. It had a specific surface area of 1802.62 m²/g, and a specific capacitance reaching 118 F/g at a scan rate of 1 mV/s. In the CDI system, it achieved the highest average removal efficiency of 11.54% and the best electrosorption capacity of 99.13 μmol/g. Moreover, it demonstrated excellent stability under multiple cycles, indicating that HZIF-8_24hr_800c_900a is an effective electrode material that significantly enhances CDI performance and cycle stability, making it the most promising porous carbon material in this study.
Through the fabrication of ZIF-8_PES_PVP composite membranes via the Metal-Phenolic Network (MPN), tests using 3.4 mM and 34 mM NaCl solutions showed a maximum average salt rejection rate of 15.41% and 7.98%, respectively, and the highest average salt removal masses of 8572 mg and 48163 mg, respectively. These results demonstrate that incorporating ZIF-8 into PES membranes effectively improves the salt ion rejection capability, showing potential for desalination applications in water treatments.

目錄
中文摘要	I
英文摘要	III
目錄	V
List of Figure	VIII
List of Table	XIII
第一章	緒論	1
1.1	研究源起	1
1.2	研究目的	2
第二章	文獻回顧	4
2.1	海水淡化處理技術	4
2.2	電容去離子技術	5
2.2.1	電容去離子技術原理	5
2.2.2	電雙層 (electrical double layer) 理論	7
2.2.3	電化學反應及過程	8
2.2.4	電容去離子技術之發展與應用	10
2.3	金屬有機框架(Metal-Organic Framework, MOF)	10
2.4	沸石咪唑酯骨架材料(Zeolitic Imidazolate Framework, ZIF)	12
2.5	沸石咪唑酯骨架材料-8 (Zeolitic Imidazolate Framework-8, ZIF-8)	13
2.5.1  沸石咪唑酯骨架-8材料介紹與生長原理	13
2.5.2  沸石咪唑酯骨架-8衍生碳材料	16
2.5.3  中空孔洞沸石咪唑酯骨架材料-8 (Hollow ZIF-8)	17
2.6	ZIF-8_PES_PVP薄膜	19
第三章	實驗方法與材料	21
3.1	研究架構	21
3.2	實驗設備	25
3.2.1	實驗藥品	25
3.2.2	實驗設備	26
3.3	電極材料製備	27
3.3.1	ZIF-8_24hr材料製備	27
3.3.2	ZIF-8_24hr衍生碳材料製備(碳化與活化)	28
3.3.3	Hollow ZIF-8_24hr (HZIF-8_24hr)材料製備	28
3.3.4	HZIF-8_24hr衍生碳材料製備(碳化與活化)	28
3.4	CDI電極製備	28
3.4.1  ZIF-8_24hr衍生碳電極製備-噴槍法	28
3.4.2  HZIF-8_24hr衍生碳電極製備-噴槍法	29
3.4.3  ZIF-8_24hr/ZIF-8_24hr 衍生碳材料循環伏安法電極製備	29
3.4.4  HZIF-8_24hr/HZIF-8_24hr衍生碳材料循環伏安法電極製備	29
3.5	ZIF-8_PES_PVP薄膜製作	31
3.6	實驗分析方法	32
3.6.1	X射線繞射分析(X-Ray Diffractometer, XRD)	32
3.6.2	掃描式電子顯微鏡分析(Scanning Electron Microscope, SEM )	32
3.6.3	能量散射X射線譜(Energy Dispersive X-Ray Microanalysis, EDX )	33
3.6.4	傅立葉變換紅外光譜儀(Fourier-transform infrared spectroscopy, FTIR)	33
3.6.5	接觸角分析 (Contact angle, CA)	34
3.6.6	水通量 (water flux)	34
3.7	計算公式	34
3.7.1	循環伏安法分析 (CV)	34
3.7.2	CDI吸脫附循環	35
3.7.3	薄膜水通量	37
第四章	結果與討論	38
4.1	ZIF-8_24hr或HZIF-8_24hr衍生碳材料應用於電容去離子系統	38
4.1.1	ZIF-8_24hr或HZIF-8_24hr衍生碳材料表面特性與孔洞結構分析	38
4.1.2  ZIF-8_24hr或HZIF-8_24hr衍生碳材料電化學特性分析	56
4.1.3	ZIF-8_24hr或HZIF-8_24hr應用於電容去離子系統	61
4.2	ZIF-8_PES_PVP薄膜應用於脫鹽技術	69
4.2.2	ZIF-8_PES_PVP薄膜水通量	80
4.2.3	ZIF-8_PES_PVP薄膜鹽截留率	90
第五章	結論與建議	96
參考文獻	98

List of Figure
Figure 2.2.1.1 Electrosorption and desorption process of CDI system to removal ions from solution.	6
Figure 2.2.2.1 EDL (Porada et al., 2013)	7
Figure 2.2.3.1 Non-Faradaic and Faraday reactions. (Porada et al., 2013)	9
Figure 2.3.1 Metal organic framework synthesis of 1D, 2D and 3D networks, from metal ions and organic linkers (Kate Milburn., 2014).	11
Figure 2.4.1 The bridging angle in both ZIFs and zeolites is 145°.(Kate Milburn., 2014)	12
Figure 2.5.1.1 Proposed mechanism for the formation of ZIF-8 crystals in water. (Meipeng Jian et al., 2015)	15
Figure 2.5.3.1 Graphical description of Microporous Carbon ,Hollow Carbon and Hollow Activated Carbon with different nanoarchitectures and porosities .(Minjun Kim., 2021)	18
Figure 2.6.1 Illustration of the synthesis of ZIF-8/(TA-Zn2+)n/PES membrane with TA-Zn2+network as zinc precursor.	20
Figure 3.1.1 Schematic of research structure.	23
Figure 3.1.2 Schematic of research structure.	24
Figure 3.7.2.1 Schematic diagram of CDI.	36
Figure 4.1.1.1 XRD spectra of ZIF-8_24hr, ZIF-8_24hr_800c, ZIF-8_24hr_900c, and ZIF-8_24hr_800c_900a.	40
Figure 4.1.1.2 XRD spectra of HZIF-8_24hr, HZIF-8_24hr_800c and HZIF-8_24hr_800c_900a.	41
Figure 4.1.1.3 SEM spectra of (a) (e) ZIF-8_24hr, (b) (f) ZIF-8_24hr_800c, (c) (g) ZIF-8_24hr_900c and (d) (h) ZIF-8_24hr_800c_900a with magnification at 10 KX or 20 KX.	42
Figure 4.1.1.4 SEM spectra of (i) (l) HZIF-8_24hr, (j) (m) HZIF-8_24hr_800c, (k) (o) HZIF-8_24hr_800 c_900a with magnification at 10 KX or 20 KX.	43
Figure 4.1.1.5 FT-IR spectra of ZIF-8_24hr, ZIF- 8_24hr_800c, ZIF- 8_24hr_900c and ZIF-8_24hr_800c_900a.	50
Figure 4.1.1.6 FTIR functional groups of ZIF-8_24hr, ZIF- 8_24hr_800c, ZIF- 8_24hr_900c and ZIF-8_24hr_800c_900a.	51
Figure 4.1.1.7 FTIR functional groups of HZIF-8_24hr, HZIF- 8_24hr_800c and H ZIF-8_24hr_800c_900a.	52
Figure 4.1.1.8 FTIR functional groups of HZIF-8_24hr, HZIF- 8_24hr_800c and H ZIF-8_24hr_800c_900a.	53
Figure 4.1.1.9 Contact angles of ZIF-8 derived porous activated carbons (a) ZIF- 8_24hr_800c, (b) ZIF- 8_24hr_900c and (c) ZIF- 8_24hr_800c_900a.	54
Figure 4.1.1.10 Contact angles of HZIF-8 derived porous activated carbons (d) HZIF- 8_24hr_800c, and (e) HZIF- 8_24hr_800c_900a.	55
Figure 4.1.2.1 Cyclic voltammograms of (a) ZIF-8_24hr,(b) ZIF-8_24hr_800c,(c) ZIF-8_24hr_900c, and (d) ZIF-8_24hr_800c_900a at scan rates of 100, 50, 10, 5, and 1 mV/s.	57
Figure 4.1.2.2 Cyclic voltammograms of (e) HZIF-8_24hr, (f) HZIF-8_24hr_800c,and (g) HZIF-8_24hr_800c_900a at scan rates of 100, 50, 10, 5, and 1 mV/s.	58
Figure 4.1.2.3 Specific capacitances of ZIF-8_24hr derived porous activated carbons with various .	59
Figure 4.1.2.4 Specific capacitances of HZIF-8_24hr derived porous activated carbons with various scan rates.scan rates.	59
Figure 4.1.2.5 Specific capacitances of ZIF-8_24hr or HZIF-8_24hr derived porous activated carbons with various scan rates.scan rates.	60
Figure 4.1.3.1 Conductivity changes during the electrosorption (50 minutes) and desorption (30 minutes) process with ZIF-8_24hr_800c, ZIF-8_24hr_900c, and ZIF- 8_24hr_800c_900a electrodes applied in CDI systems.	64
Figure 4.1.3.2 Conductivity changes during the electrosorption (50 minutes) and desorption (30 minutes) process with HZIF-8_24hr_800c and HZIF-8_24hr_800c_900a electrodes applied in CDI systems.	64
Figure 4.1.3.3 Conductivity changes during the electrosorption (50 minutes) and desorption (30 minutes) process with ZIF-8_24hr or HZIF-8_24hr derived porous activated carbons electrodes applied in CDI systems.	65
Figure 4.1.3.4 The average removal efficiency (%) and average electrosorption capacity (μmole/g) with ZIF-8_24hr or HZIF-8_24hr derived porous activated carbon electrodes in four cycles of CDI system.	67
Figure 4.2.1.1 XRD spectra of PES_PVP, (TA-Zn2+)2_PES_PVP and ZIF-8_ PES_PVP.	71
Figure 4.2.1.2 SEM spectra of the top view of (a)(d) PES_PVP, (b)(e) (TA-Zn2+)2_PES_PVP, and (c)(f) ZIF-8_ PES_PVP.	72
Figure 4.2.1.3 SEM spectra of cross-sectional view of (a)(d) PES_PVP, (b)(e) (TA-Zn2+)2_PES_PVP and (c)(f) ZIF-8_ PES_PVP. 	73
Figure 4.2.1.4 SEM/EDX image of (a) PES_PVP, (b) (TA-Zn2+)2_PES_PVP, and (c) ZIF-8_ PES_PVP.	74
 Figure 4.2.1.5 ATR-FTIR spectra of PES_PVP, (TA-Zn2+)2_PES_PVP, and ZIF-8_ PES_PVP.	77
Figure 4.2.1.6 The comparison of FT-IR spectra of PES_PVP, (TA-Zn2+)2_PES_PVP, and ZIF-8_ PES_PVP.	78
Figure 4.2.1.7 Contact angles of ZIF-8_ PES_PVP membranes (a) PES_PVP, (b) (TA-Zn2+ )2_PES_PVP and (c) ZIF-8_ PES_PVP.	79 
Figure 4.2.2.1 Water Flux in DI water for PES_PVP、(TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP.	81
Figure 4.2.2.2 Water Flux in DI water for PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP.	82
Figure 4.2.2.3 Average Water Flux in DI water for PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP.	83
Figure 4.2.2.4 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	84
Figure 4.2.2.5 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	85
Figure 4.2.2.6 Average Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	86
Figure 4.2.2.7 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 34 mM NaCl Solution.	87
Figure 4.2.2.8 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 34 mM NaCl Solution.	88
Figure 4.2.2.9 Average Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP, and ZIF-8_ PES_PVP in 34 mM NaCl Solution.	89
Figure 4.2.3.1 Average salt removal (mg) and average salt rejection rate (%) of PES_PVP, (TA-Zn2+ )2_PES_PVP and ZIF-8_ PES_PVP in 3.4 mM NaCl solution with two measurements.	93
Figure 4.2.3.2 Average salt removal (mg) and average salt rejection rate (%) of PES_PVP, (TA-Zn2+ )2_PES_PVP and ZIF-8_ PES_PVP in 34 mM NaCl solution with two measurements.	95

List of Table
Table 3.2.1.1 Manufactures and purity of experimental chemicals.	25
Table 3.2.1.2 Manufacturers and models of equipments.	26
Table 4.1.1.1 Elemental composition of ZIF-8_24hr, ZIF-8_24hr_800c, ZIF-8_24hr_900c, ZIF-8_24hr_800c_900a, HZIF-8_24hr, HZIF-8_24hr_800c and HZIF-8_24hr_800c_900a based on EDX analyses.	44
Table 4.1.1.2 Specific surface area and porosity analyses of ZIF-8_24hr or HZIF-8_24hr derived porous activated carbon.	47
Table 4.1.1.3 FTIR functional groups of ZIF-8, ZIF-8_800c, ZIF-8_800c_800a and ZIF-8_800c_900a.	51
Table 4.1.1.4 FTIR functional groups of HZIF-8_24hr, HZIF- 8_24hr_800c and H ZIF-8_24hr_800c_900a.	53
Table 4.1.2.1 Specific capacitance of ZIF-8_24hr or HZIF-8_24hr derived porous activated carbon with various scan rates.	60
Table 4.1.3.1 Removal efficiency (%) and electrosorption capacity (μmole/g) of with ZIF-8_24hr or HZIF-8_24hr derived porous activated carbons electrodes in the CDI system during the electrosorption (50 minutes) and desorption (30 minutes) process.	66
Table 4.1.3.2 Comparison of capacitive deionization performance of HZIF-8_24hr_800c_900a with other reported carbon electrodes.	68
Table 4.2.1.1 Elemental composition of PES_PVP, (TA-Zn2+)2_PES_PVP, and ZIF-8_ PES_PVP.	75
Table 4.2.1.2 FTIR functional groups of PES_PVP, (TA-Zn2+)2_PES_PVP, and ZIF-8_ PES_PVP.	78
Table 4.2.2.1 Water flux (LMH) in DI water for PES_PVP、(TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP.	81
Table 4.2.2.2 Water flux (LMH) in DI water for PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP.	82
Table 4.2.2.3 Average Water flux (LMH) in DI water for PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP.	83
Table 4.2.2.4 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	84
Table 4.2.2.5 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	85
Table 4.2.2.6 Average Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 3.4 mM NaCl Solution.	86
Table 4.2.2.7 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 34 mM NaCl Solution.	87
Table 4.2.2.8 Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 34 mM NaCl Solution.	88
Table 4.2.2.9 Average Water flux of PES_PVP, (TA-Zn²⁺)2_PES_PVP,and ZIF-8_ PES_PVP in 34 mM NaCl Solution	89
Table 4.2.3.1 Water flux (LMH) and permeate conductivity (mS/cm) and salt rejection rate (%) and salt removal (mg) of  PES_PVP, (TA-Zn2+ )2_PES_PVP membrane and ZIF-8_ PES_PVP in 3.4 mM NaCl solution with two measurements.	92
Table 4.2.3.2 Water flux (LMH) and permeate conductivity (mS/cm) and salt rejection rate (%) and salt removal (mg) of PES_PVP membrane, (TA-Zn2+)2_PES_PVP membrane and ZIF-8_ PES_PVP membrane in 34 mM NaCl solution with two measurements.	94

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