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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101716完整後設資料紀錄
| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 侯嘉洪 | zh_TW |
| dc.contributor.advisor | Chia-Hung Hou | en |
| dc.contributor.author | 張睿耀 | zh_TW |
| dc.contributor.author | Jui-Yao Chang | en |
| dc.date.accessioned | 2026-02-26T16:57:36Z | - |
| dc.date.available | 2026-02-27 | - |
| dc.date.copyright | 2026-02-26 | - |
| dc.date.issued | 2026 | - |
| dc.date.submitted | 2026-01-26 | - |
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Separation and Purification Technology, 328, 125094. https://doi.org/10.1016/j.seppur.2023.125094 Zhu, Y., He, Z., Choi, Y., Chen, H., Li, X., Zhao, B., Yu, Y., Zhang, H., Stoerzinger, K. A., Feng, Z., Chen, Y., & Liu, M. (2020). Tuning proton-coupled electron transfer by crystal orientation for efficient water oxidization on double perovskite oxides. Nature Communications, 11(1), 4299. https://doi.org/10.1038/s41467-020-17657-9 Zou, C. W., Shao, L. X., Guo, L. P., Fu, D. J., & Kang, T. W. (2011). Ferromagnetism and ferroelectric properties of (Mn, Li) co-doped ZnO nanorods arrays deposited by electrodeposition. Journal of Crystal Growth, 331(1), 44–48. https://doi.org/10.1016/j.jcrysgro.2011.06.039 | - |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/101716 | - |
| dc.description.abstract | 隨著全球產業的快速發展，資源永續循環已成為當前技術發展的重要目標。其中，氨氮(包含氨氣與銨離子)被視為各產業關鍵的化學原料與未來能源發展的重要載體(Energy carrier)，其需求量隨著科技進步而持續增加。然而，傳統的哈伯法(Haber-Bosch process)製氨技術需消耗大量能源，限制了其永續性。此外，工業活動的快速擴張亦導致大量含高濃度硝酸鹽的廢水排放，對環境與人體健康造成潛在危害。因此，開發具高效率與高選擇性的硝酸鹽還原(Nitrate reduction)技術，以氨氮為主要生成產物並實現其選擇性回收，具有關鍵的重要性。
本研究開發複合式氧化還原電極(Redox composite electrodes)，結合功能性穿透式電極(Functional flow-through electrode)與嵌入式電極(Intercalation electrode)之設計，透過電化學氧化還原機制成功實現選擇性電化學硝酸鹽還原為氨氮，並達到氨氮的選擇性濃縮與回收。本研究的重點首先在於驗證功能性穿透式電極(Flow-through electrode)相較於傳統流經式電極(Flow-by electrode)在電化學硝酸鹽還原反應中的效能提升與反應機制。接著進一步設計改良功能性穿透式電極以實現高效硝酸鹽去除與高選擇性氨氮生成。透過在靜電紡絲活性碳纖維上電鍍金屬銅/氧化銅，藉由控制電鍍時間以調控金屬銅與氧化銅的晶面生長，從而提升硝酸鹽去除速率、氨氮選擇性與氨氮生成速率。此外，本研究結合具金屬有機骨架結構特性的普魯士藍(Prussian blue analogs, PBAs)材料與高導電性奈米碳管(Carbon nanotubes, CNTs)，構築高電化學活性的氧化還原嵌入式電極，以實現水中銨離子的選擇性捕捉。藉由普魯士藍材料金屬有機骨架結構特性，可有效實現銨離子的選擇性電化學捕捉與濃縮。同時，該奈米碳管複合嵌入式電極展現出高導電性與高比電容等優異電化學特性，並具備高中孔比例以促進離子傳輸。 總體而言，本研究將功能性穿透式電極與高電化學活性嵌入式電極引入水處理技術中，成功提升電化學硝酸鹽去除效率並實現氨氮的選擇性生成。同時，透過對銨離子的選擇性捕捉與濃縮，有望達成氨氮資源回收與再利用的目標，展現此技術於永續水資源管理中的應用潛力。 | zh_TW |
| dc.description.abstract | With the rapid development of global industries, sustainable resource circulation has become a crucial goal in modern technological advancement. Among various resources, ammonia, including ammonia gas and ammonium ions, is recognized as a key chemical feedstock for many industries and an important energy carrier for future energy systems, with its demand continuing to rise alongside technological progress. However, the conventional Haber–Bosch process for ammonia synthesis is highly energy-intensive, limiting its sustainability. In addition, the rapid expansion of industrial activities has led to the discharge of large volumes of nitrate-containing wastewater, posing potential threats to both the environment and human health. Therefore, developing an efficient and highly selective nitrate reduction technology that produces ammonia as the primary product and enables its selective recovery is of critical importance.
In this study, redox composite electrodes were developed by integrating a functional flow-through electrode and an intercalation electrode, enabling the coupling of electrochemical reduction and oxidation processes to achieve selective electrochemical nitrate reduction to ammonia, as well as selective ammonium enrichment and recovery. The first focus of this research was to elucidate the performance enhancement and reaction mechanisms of a functional flow-through electrode compared with a conventional flow-by electrode in electrochemical nitrate reduction. Furthermore, a functional flow-through electrode was designed to achieve efficient nitrate removal and high ammonia selectivity. By electrodepositing Cu/Cu2O onto electrospun activated carbon fibers and controlling the electrodeposition time to tune the crystal facet growth of Cu and Cu2O, the nitrate removal rate, ammonia selectivity, and ammonia production rate were significantly improved. Furthermore, this study combined Prussian blue analogs (PBAs), which possess metal–organic-framework-like structures, with highly conductive carbon nanotubes (CNTs) to construct a high-electrochemical-activity intercalation electrode for the selective capture of ammonium. The CNT-composited intercalation electrode exhibited excellent electrochemical properties, including high electrical conductivity, high specific capacitance, and a large mesoporous ratio that facilitated ion transport. Additionally, its metal–organic-framework-like (MOF-like) structure enabled selective electrochemical capture and enrichment of ammonium ions. Overall, this study successfully introduced novel functional flow-through electrodes and high-electrochemical-activity intercalation electrodes into water treatment technology, enhancing electrochemical nitrate removal efficiency and achieving selective ammonia generation, as well as selective capture and enrichment of ammonium ions. This work demonstrates great potential for realizing ammonia nitrogen resource recovery and reuse, contributing to sustainable water resource management. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2026-02-26T16:57:36Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2026-02-26T16:57:36Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 誌謝 i
中文摘要 iii ABSTRACT iv CONTENTS vi LIST OF TABLES x LIST OF FIGURES xi DECLARATION OF PUBLICATIONS xxi SYMBOLS AND ABBREVIATIONS xxii CHAPTER 1 INTRODUCTION 1 1.1 Background/Problem Statement 1 1.2 Research Hypotheses 4 1.3 Research Objectives 5 1.4 Organization of Thesis 8 CHAPTER 2 LITERATURE REVIEW 11 2.1 Novel and Sustainable Pathways for Restoring the Nitrogen Cycle through Nitrate-to-Ammonia Conversion 11 2.2 Current Technologies for Nitrate Removal 12 2.3 Electrochemical Nitrate Reduction Technology 14 2.3.1 Mechanism Insight of Electrochemical Nitrate Reduction 14 2.3.2 The Design and Exploitation of Redox Composite Electrodes for Electrochemical Nitrate Reduction 18 2.3.3 Functional Flow-Through Electrodes 21 2.4 Current Technologies for Ammonia Recovery 23 2.4.1 Physicochemical Technologies 23 2.4.2 Electrochemical Ion Separation Technologies 24 2.5 Capacitive Deionization (CDI) 26 2.5.1 Mechanism Insight of CDI 26 2.5.2 Electrode Materials of CDI 27 2.6 Knowledge Gap 30 CHAPTER 3 EXPERIMENTAL METHODS 32 3.1 Materials and Chemicals 32 3.2 Characterization and Analytical Instruments 33 3.2.1 Material Characterization 34 3.2.2 Electrochemical Characterization 35 3.2.3 Water Quality Analysis 36 3.3 Fabrication of Redox Composite Electrodes 36 3.3.1 Preparation of the 3D Cu-Pd Bimetallic Flow-Through Electrode 36 3.3.2 Preparation of the Electrospun-derived Activated Carbon Fibers 37 3.3.3 Preparation of the Cu/Cu2O Heterostructured Functional Flow-Through Electrodes 38 3.3.4 Preparation of the Carbon Nanotube Bridged Nickel Hexacyanoferrate (NiHCF/CNT) Electrode 39 3.4 Experimental Setup 42 3.4.1 Batch-Mode Electroreduction of NO3− Using the NF/CuxPdy Electrode 42 3.4.2 NO3− Electroreduction to NH3 by Using the Cu/Cu2O/ACF-x Flow-Through Electrodes 43 3.4.3 Single-pass Mode CDI Experiments for Ammonium Enrichment 44 3.5 Performance Indicators 46 3.5.1 Performance Indicators for Nitrate Electroreduction to NH3 46 3.5.2 Performance Indicators for Ammonium Enrichment 49 CHAPTER 4 BOOSTING NITRATE ELECTROREDUCTION REACTIVITY WITH A FLOW-THROUGH ELECTRODE 52 4.1 Characterization of NF/CuxPdy Electrodes 53 4.2 Electrochemical Reduction of NO3− 58 4.2.1 Influence of the Cu/Pd Ratio 58 4.2.2 Comparison of Flow-By and Flow-Through Configurations 65 4.2.3 Effect of the Initial NO3− Concentration 70 4.2.4 Effect of Initial pH Values 75 4.3 Summary 81 CHAPTER 5 SELECTIVE ELECTROCHEMICAL REDUCTION OF NITRATE TO AMMONIA USING FUNCTIONAL FLOW-THROUGH ELECTRODES 82 5.1 Characterization of Cu/Cu2O/ACF-x Functional Flow-Through Electrodes 83 5.2 Electrochemical Reduction of Nitrate to Ammonia 96 5.2.1 Effect of the Electrodeposition Time 96 5.2.2 Effect of the Applied Potential 103 5.2.3 Effect of the Electrolyte Concentration 107 5.2.4 Comparison of Electrocatalytic Performance between Cu/Cu2O Functional Flow-Through Electrodes and Previously Reported Materials 110 5.3 Summary 113 CHAPTER 6 SELECTIVE ENRICHMENT OF AMMONIUM BY CARBON NANOTUBE BRIDGED INTERCALATION ELECTRODE 114 6.1 Morphological and Structural Characterizations of the electrodes 115 6.2 Electrochemical Properties of the electrodes 118 6.3 Ammonium Enrichment Experiments Using the NiHCF/CNT Electrode at Different Stopped-flow Time 125 6.4 Ammonium Enrichment Experiments Using the NiHCF/CNT Electrode in Mixed-salt Solutions 130 6.5 Summary 136 CHAPTER 7 CONCLUSIONS AND RECOMMENDATIONS 137 7.1 Conclusions 137 7.2 Recommendations 139 REFERENCE 141 LIST OF PUBLICATION 169 | - |
| dc.language.iso | en | - |
| dc.subject | 複合式氧化還原電極 | - |
| dc.subject | 功能性穿透式電極 | - |
| dc.subject | 電化學硝酸鹽還原 | - |
| dc.subject | 金屬銅/氧化銅晶面調控 | - |
| dc.subject | 嵌入式電極 | - |
| dc.subject | 氨氮選擇性回收 | - |
| dc.subject | 氨氮濃縮 | - |
| dc.subject | 電容去離子技術 | - |
| dc.subject | Redox composite electrode | - |
| dc.subject | functional flow-through electrode | - |
| dc.subject | electrochemical nitrate reduction | - |
| dc.subject | Cu/Cu2O crystal facet engineering | - |
| dc.subject | intercalation electrode | - |
| dc.subject | selective ammonia recovery | - |
| dc.subject | ammonium enrichment | - |
| dc.subject | capacitive deionization | - |
| dc.title | 開發複合式氧化還原電極於電化學選擇性硝酸鹽還原至氨氮回收之研析 | zh_TW |
| dc.title | Tailoring redox composite electrodes for selective electrochemical nitrate reduction toward ammonia recovery | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 114-1 | - |
| dc.description.degree | 博士 | - |
| dc.contributor.oralexamcommittee | 盧明俊;蘇鎮芳;潘述元;李公哲;林逸彬 | zh_TW |
| dc.contributor.oralexamcommittee | Ming-Chun Lu;Jenn-Fang Su;Shu-Yuan Pan;Kung-Cheh Li;Yi-Pin Lin | en |
| dc.subject.keyword | 複合式氧化還原電極,功能性穿透式電極電化學硝酸鹽還原金屬銅/氧化銅晶面調控嵌入式電極氨氮選擇性回收氨氮濃縮電容去離子技術 | zh_TW |
| dc.subject.keyword | Redox composite electrode,functional flow-through electrodeelectrochemical nitrate reductionCu/Cu2O crystal facet engineeringintercalation electrodeselective ammonia recoveryammonium enrichmentcapacitive deionization | en |
| dc.relation.page | 169 | - |
| dc.identifier.doi | 10.6342/NTU202600260 | - |
| dc.rights.note | 未授權 | - |
| dc.date.accepted | 2026-01-27 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 環境工程學研究所 | - |
| dc.date.embargo-lift | N/A | - |
| 顯示於系所單位： | 環境工程學研究所 | |
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