電容式去離子（CDI）技術以其高效、低能耗、環保等優點，成為海水淡化和水處理領域的一粒新星。 為了達到去離子的目的，低電壓之直流電使電場產生，誘使溶液中的離子定向遷移並吸附到電極中。CDI的去離子性能高度依賴於電極材料。 在CDI電極主要材料的發展方面，碳材因其多項優異特性而受到廣泛關注，其中包括了高比表面面積（SSA）為離子吸附和積累提供更多活性位點，高導電性，高親水性，極佳的電化學穩定性。然而，在使用單一碳材的應用、會因其疏水性、結構過於不規則、電阻力高等方面仍存在一些挑戰。 此外，碳材料的低電吸附能力也阻礙該材料在CDI技術中的實際應用。爲此，這項研究的主要目的是透過各種改便表面特性的方法以提高碳基材的料電吸附能力。其一，雜原子摻雜至碳架構的方式有助於提高該材料的親水性和導電性，同時降低和離子排出的現象發生。因此，本研究中對碳材料的改性（ N摻雜碳波、N摻雜碳納米纖維、功能化生物炭來源於生物質）顯著實現了較高的去離子性能。
其二，透過組合不同類型的碳材料或把碳材料與其他法拉第材料（包括金屬氧化物、過渡金屬硫族化物）結合之複合材料也可以進一步提高CDI性能。 該實驗理論是依據法拉第電容遠大於碳材料嘅雙電層（EDL）容量的原理。法拉第電容是指電活性材料在碳材料中的欠電位沉積，從而導致高度可逆嘅化學吸附、解吸或氧化還原反應，與電極電容的電荷電位有關。 因此，利用法拉第材料構建碳的複合結構對於CDI電極研究領域的延伸至關重要。例如，利用水熱工藝所製成的二硫化鉬納米片和N摻雜碳球（MoS2@NCS）核殼結構在2000 mg L−1 NaCl和1.4 V的外加電壓下可達成59.9 mg g−1的優越比電吸附容量（SAC）。該項結果發現別於傳統碳材料的一般表現，更展現金屬二硫族化物可應用於未來CDI材料的潛力。在其他研究中，錳鐵素體也可採用沉澱法修飾到維基活性炭纖維（MnFe2O4/N-ACF）上，用於CDI應用。該複合材料可在500 mg L−1的NaCl系統中，透過流速和施加電壓分別為10 mL min−1和1.4 V下，達到41.2 mg g−1的 SAC。 此外，所製備的電極材料可以回收至少50個循環，並且在50次循環後SEC可以保持原始活性的93%以上，證實了MnFe2O4/N-ACF電極優異的循環穩定性。
插層插入材料（金屬碳化物和/或MXene）在CDI應用中的應用因其在高鹽度溶液中出色的除鹽能力而得到廣泛應用。摒除以往利用離子與碳質電極相關的靜電力作用為吸附基礎，該研究成果也展示了透過插層或氧化還原過程從海水中提取鹹離子的可行性。所製備的MXene Ti3C2Tx在結構改變、成分多樣性和性能韌性方面的靈活性表現出優異的脫鹽性能，在3000 mg L-1 NaCl中具有35.4 mg g−1的最高SAC，證明了MXene Ti3C2Tx在實際CDI中的應用潛力無限。
再者，CDI的選擇性吸附能力也是使用CDI作為水修復處理的關鍵考量因素之一。 特異性吸附對於去除和收集廢水中的各種離子具有重要意義，特別是對於重金屬。本研究構建了一種不對稱CDI裝置，其中部分具備活化生物炭（來源於生物AB 作為陽極，功能化金屬碳化物（V2AlC-OHx）作為陰極，用于有效和選擇性地去離子水溶液中嘅Cr(VI）離子。值得一提的是，AB//V2AlC-OHx不對稱CDI裝置除了具有優異的去離子性能，也備有最高的比電吸附容量（43 mg g−1）等同於99%的去除效率，為CDI技術在工業廢水中有毒金屬離子去離子化的實際應用開闢出新的前景。

Capacitive deionization (CDI) technology has become a new star in the field of desalination and water treatment owing to its merits of high efficiency, low energy usage, and environmentally-friendly. To achieve the purpose of deionization, a low voltage of direct-current is used to create an electric field that make ions in solution directionally migrate and adsorbed into electrode. The deionized performance of CDI is highly based on the electrode material. In terms of the development of key materials for CDI electrodes, carbon has attracted wide attention due to a number of excellent advantages that have witnessed all the requirements for CDI electrode materials, such as high SSA to serve more active sites for ions adsorption and accumulation, high electrical conductivity, high hydrophilicity, excellent electrochemical stability. However, there are still some challenges in single composition, hydrophobicity, too irregular structure, and high resistance of carbon materials that hinder the CDI technology development. However, several issues in the low electrosorption capacity prohibits the practical application of carbon materials for CDI technology. This is the primary rationale for diverse modification methods proposed to increase the electrosorption capability. The functionalization and heteroatom doping into carbon network would be critical for the future advancement of utilizing carbon as a CDI electrode materials by increasing their hydrophilicity and conductivity while decreasing the co-ion expulsion impact. As a result, the modification of carbon materials in this research (N-doped carbon sphere, N-doped carbon nanofiber, functionalized activated biochar derived from biomass) significantly achieved high deionization performance.
In addition, the introduction of the composites obtained by combining different types of carbon materials or by combining carbon materials with other Faradaic materials (including metal oxides, transition metal dichalcogenide) can further enhance the CDI performance. This theory is dependent on the fact that the Faradaic capacitance of Faradaic materials is much larger than the electrical double layer (EDL) capacity of carbon material. Faradaic capacitance refers to the underpotential deposition of electroactive materials in carbon material, thereby leading to highly reversible chemisorption, desorption or redox reactions, which are related to the charge potential of the electrode capacitance. Therefore, to built the composite construction of carbon with Faradaic material is essential for the extension of CDI electrode research fields. For instance, the nanoarchitecture of deposition of molybdenum disulfide nanosheets onto N-doped carbon sphere (MoS2@NCS) has been successfully developed using hydrothermal processes for CDI applications. The superior specific electrosorption capacity (SAC) of 59.9 mg g−1 is obtained at 2000 mg L−1 NaCl and applied voltage of 1.4 V. This result is difficult to achieve with traditional carbon materials, indicating that the deposition of metal dichacogenide into the carbon network may be the key to CDI's future use in actual water desalination. In other work, the manganese ferrite was decorated onto 1-dimensional based activated carbon fiber (MnFe2O4/N-ACF) by precipitation method for CDI application. A SAC of 41.2 mg g−1 in the presence of 500 mg L−1 can be achieved when the flow rate and applied voltage are 10 mL min−1 and 1.4 V, respectively. Moreover, the as-prepared electrode materials can be recycled for at least 50 cycles and the SAC can be maintained over 93% of the original activity after 50 cycles, corroborating the excellent cycling stability of MnFe2O4/N-ACF electrode.
The utilization of intercalation-insertion material (metal carbide and/or Mxene) for CDI application have been widely implemented due to their excellent salt removal capability in high salinity solution. Instead of electrostatic forces associated with the carbonaceous electrode, salty ions can be extracted from sea water through intercalation or redox processes. The flexibility in structural alterations, compositional diversity, and properties tenability of as-prepared MXene Ti3C2Tx exhibits the superior desalination performance with the highest SAC of 35.4 mg g−1 in 3000 mg L-1 NaCl, demonstrating the promising application of MXene Ti3C2Tx for practical CDI.
The selective adsorption capacity of CDI is also one of the critical factors in using CDI as water remediation treatment. Specific adsorption is of great significance to remove and collect various ions from wastewater, especially for heavy metals. In this study, an asymmetric CDI device where functionalized activated biochar (derived from biomass, AB) plays as the anode and funtionalized metal carbide (V2AlC-OHx) serves as the cathode was constructed for the effective and selective deionization of Cr(VI) ions from aqueous solution. Interestingly, the AB//V2AlC-OHx asymmetric CDI device possesses superior deionization performance for Cr(VI) removal with the highest specific electrosorption capacity of 43 mg g−1 and removal efficiency of 99%, indicating the prospect to open a wide window for practical applications of CDI technology in the deionization of toxic metal ions from industrial wastewater.

Contents
Acknowledgements I
Abstract III
摘要 VI
Contents VII
List of figures XI
List of tables XVIII
ABBREVIATIONS, UNITS, AND SYMBOLS XIX
Chapter 1 1
Introduction 1
1.1. Motivation 2
1.2. Water shortage and the need in water treatment technology 4
1.3. Capacitive deionization technology for desalination and water remediation 5
1.3.1. Conventional technology in desalination 5
1.3.2. Capacitive deionization technology 11
1.3.3. The development of CDI technology 14
1.4. Overview of electrochemical reaction and process in CDI 16
1.4.1. Theory of Electrical double layer 16
1.4.2. Theory of Pseudo-capacitance 18
1.5. Carbon-based electrode materials for CDI device 20
1.5.1. Carbon materials 20
1.5.2. Carbon-based nanocomposites 22
1.5.3. Metal carbide and MXene 24
1.6. Aim and objective 30
1.7. Thesis design and summary 31
Chapter 2 34
Fabrication of carbon electrodes for CDI applications 34
2.1. Introduction 35
2.2. Reagents and methods 38
2.2.1. Reagents 38
2.2.2. Synthesis of nitrogen-doped carbon spheres (NCS) 38
2.2.3. Synthesis of carbon nanofiber 39
2.2.4. Synthesis of functionalized activated biochar (AB) derived from the badam tree leaves 39
2.3. Characterization 40
2.4. Electrochemical measurements 40
2.5. Electrosorption of NaCl by carbon electrode 41
2.6. Physicochemical characterization of as-fabricated carbon electrodes 42
2.6.1. Surface characterization of as-fabricated carbon electrodes 42
2.6.2. Electrochemical properties of as-fabricated carbon electrodes 48
2.7. CDI application using different carbon-electrodes 51
2.8. Conclusions 54
Chapter 3 56
Architectures of flower-like MoS2 nanosheet coated N-doped carbon sphere electrode materials for enhanced capacitive deionization 56
Summary 57
3.1. Introduction 58
3.2. Experimental 61
3.2.1. Reagents 61
3.2.2. Synthesis of dopamine-derived N-doped carbon spheres (NCS) 62
3.2.3. Preparation of MoS2@NCS 62
3.2.4. Characterization 63
3.2.5. Electrochemical measurements 63
3.2.6. Electrosorption of NaCl by MoS2@NCS 64
3.2.7. Modeling 65
3.3. Results and discussion 66
3.3.1. Surface characterization of MoS2@NCS 66
3.3.2. Electrochemical property of MoS2@NCS 74
3.3.3. Desalination performance of MoS2@NCS-800 77
3.3.4. Cycling stability 87
3.4. Conclusions 91
Chapter 4 93
Manganese ferrite decorated N-doped polyacrylonitrile-based carbon nanofiber for the enhanced capacitive deionization 93
Summary 94
4.1. Introduction 95
4.2. Experimental 98
4.2.1. Chemicals 98
4.2.2. Fabrication of MnFe2O4/N-ACF 99
4.2.3. Characterization of N-ACF and MnFe2O4/N-ACF nanocomposites 99
4.2.4. Electrochemical measurement 100
4.2.5. Electrosorption of salt by N-ACF and MnFe2O4/N-ACF 101
4.3. Results and discussion 101
4.3.1. Surface characteristic of N-ACF and MnFe2O4/N-ACF nanocomposites 101
4.3.2. Electrochemical property of MnFe2O4/N-ACF 110
4.3.3. Electrosorption performance of MnFe2O4/N-ACF 115
4.3.4. Regeneration properties of MnFe2O4/N-ACF electrodes 121
4.4. Conclusions 122
Chapter 5 124
Ti3C2Tx MXene as an intercalation-type pseudocapacitive electrode for boosting capacitive deionization performance 124
Summary 125
5.1. Introduction 126
5.2. Experimental and methods 129
5.2.1. Reagents 129
5.2.2. Synthesis of Ti3C2Tx MXene by in-situ generated HF method 130
5.2.3. Surface characterization 130
5.2.4. Electrochemical characterizations 131
5.2.5. CDI application 131
5.3. Results and discussion 132
5.3.1. Surface characteristics of different MXenes 132
5.3.2. Electrochemical characterizations 138
5.3.3. Desalination performance using Ti3C2Tx-1 as CDI electrode martial 141
5.3.4. Electrosorption selectivity in CDI application 145
5.4. Conclusions 151
Chapter 6 152
Effective removal of Cr(VI) using the badam tree leaf-derived carbon and functionalized metal carbide 2D framework for asymmetric CDI electrode 152
Summary 153
6.1. Introduction 154
6.2. Materials and methods 156
6.2.1. Reagents 156
6.2.2. Synthesize of materials 157
6.2.3. Sample characterization 157
6.2.4. Electrochemical measurement 158
6.2.5. CDI application for Cr(VI) removal 159
6.3. Results and discussion 159
6.3.1. Surface characteristics of AB and functionalized V2AlC-OHx 159
6.3.2. Electrochemical performance of AB and V2AlC-OHx 165
6.3.3. Electrosorption performance 167
6.4. Conclusions 179
Chapter 7 181
Conclusions and Perspectives for future research 181
7.1. Conclusions 182
7.2. Perspectives for future research 184
Curriculum vitae 186
List of publications 187
References 189

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