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| DC 欄位 | 值 | 語言 |
|---|---|---|
| dc.contributor.advisor | 陳浩銘 | zh_TW |
| dc.contributor.advisor | Hao Ming Chen | en |
| dc.contributor.author | 劉芷云 | zh_TW |
| dc.contributor.author | Chih-Yun Liu | en |
| dc.date.accessioned | 2023-10-24T16:30:43Z | - |
| dc.date.available | 2025-08-07 | - |
| dc.date.copyright | 2023-10-24 | - |
| dc.date.issued | 2023 | - |
| dc.date.submitted | 2023-08-08 | - |
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Development of a Liquid Chromatography Ion Trap Mass Spectrometer Method for Clinical Drugs of Abuse Testing with Automated On-Line Extraction Using Turbulent Flow Chromatography. 2014. 42. Wang, M.; Árnadóttir, L.; Xu, Z. J.; Feng, Z., In Situ X-ray Absorption Spectroscopy Studies of Nanoscale Electrocatalysts. Nano Micro Lett. 2019, 11 (1), 47. 43. Zhang, L., X-Ray Absorption Spectroscopy of Metalloproteins. In Metalloproteins: Methods and Protocols, Hu, Y., Ed. Springer New York: New York, NY, 2019; pp 179-195. | - |
| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/90962 | - |
| dc.description.abstract | 相對於工業所選擇的電解水反應（OER）來說，尿素氧化反應（UOR）被視為能應用在二氧化碳還原反應（CO2RR）電解器的替代陽極反應。然而，目前尚未明確建立尿素分子吸附取向、催化劑結構與產物選擇性之間的關係。本研究設計了兩種配位環境，分別為具有孤立活性位點的單原子鐵催化劑FeNC與相鄰活性位點的奈米氧化鐵FeO進行系統性的比較，以釐清尿素吸附取向與催化劑配位形式對產物選擇性的影響。結果顯示，FeNC不僅擁有最好的 UOR 催化活性，在1.33 V的陽極工作電位下即可達到10 mA cm-2。此外，FeNC對氮氣選擇性高達95%。透過臨場X光吸收光譜與拉曼光譜技術揭示了催化劑的動態結構以及反應中間體，說明 FeNC 能促進尿素分子內的氮原子進行分子內的 N-N 鍵的耦合，使氮氣產量上升，而FeO則主導了氮氧化物中間體 *NO 與 *NO3- 的生成。藉由分析尿素吸附在活性位點時尿素分子中化學鍵可移動的程度，建立了催化劑結構與產物選擇性之間的關係，並成功優化UOR催化劑的設計。 | zh_TW |
| dc.description.abstract | Urea oxidation reaction (UOR) has been considered as a promising alternative to anodic oxygen evolution reaction (OER) for carbon dioxide reduction (CO2RR) electrolyzer. However, the high selectivity of non-nitrogen species hinders its sustainable application. The relationship between catalyst structure and product selectivity has not been well-defined. Herein, this study systematically designed a single-atom iron catalyst and a nano iron oxide catalyst for urea mono-coordination and bi-coordination environments to clarify the impact of urea-catalyst coordination on product selectivity. The results showed that the single-atom iron catalyst exhibited the highest UOR catalytic activity with working potential of 1.33 V to deliver 10 mA cm–2, and 95% N2 selectivity. In situ X-ray absorption spectroscopy and Raman spectroscopy revealed the dynamic structure of the catalyst and reaction intermediates. FeNC could trigger a different route of the N-N coupling of urea molecules. In contract of FeO dominated the formation of the intermediates *NO and *NO3-. Based on the flexibility of the urea molecule in coordination with active sites, the structure-product selectivity relationship was established. These findings provided guidance for the design and optimization of catalyst for UOR performance. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2023-10-24T16:30:43Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2023-10-24T16:30:43Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 摘要 I
Abstract II 目錄 III 圖目錄 VI 表目錄 X 第一章 緒論 1 1.1 全球暖化與能源危機 1 1.2 尿素氧化反應 (UOR) 2 1.2.1 尿素氧化反應之困境 2 1.2.2 尿素氧化反應之反應機制探討 3 1.2.3 尿素氧化反應之催化劑篩選標準 8 1.2.4 尿素氧化反應之催化劑 9 1.3 單原子催化劑(Single atom catalysts, SACs) 19 1.3.1 單原子催化劑(SACs)之合成 19 1.3.2 單原子催化劑(SACs)中真實活性位點之重要性 21 1.3.3 單原子本質特性對活性之影響 23 1.3.4 單原子催化劑於電催化之應用 26 1.4 研究動機 30 第二章 實驗步驟與儀器分析原理 32 2.1 實驗流程 32 2.2 實驗藥品 32 2.3 實驗藥品資訊 33 2.4 鎳網之前處理 34 2.5 FeNC&NC之製備 34 2.6 樣品鑑定與分析 35 2.6.1 X 光繞射儀 (X-ray diffraction, XRD) 35 2.6.2 電子顯微鏡 (Electron Microscope, EM) 37 2.6.3 穿透式電子顯微鏡 (Transmission Electron Microscope, TEM) 38 2.6.4 掃描透射電子顯微鏡Scanning Transmission Electron Microscopy (STEM) 39 2.6.5 能量散佈光譜儀 (Energy-Dispersive X-ray spectroscopy, EDS) 40 2.6.6 X光光電子能譜儀(X-Ray Photoelectron Spectroscopy, XPS) 40 2.6.7 拉曼光譜儀 (Raman spectroscopy) 42 2.7 電化學量測方法 43 2.7.1 伏安法 (Voltammetry) 43 2.7.2 定電位測定法 (Chronoamperometry) 44 2.7.3 電阻電降補償 (iR-drop compensation) 44 2.7.4 塔弗爾斜率 (Tafel slope) 45 2.7.5 電化學表面積測量：雙電層電容法 45 2.7.6 尿素氧化反應之H型電化學反應系統 46 2.7.7 感應耦合電漿質譜儀 (Inductive Coupling Plasma Mas Spectrometer, ICP-MS) 47 2.8 電化學中產物之定性與定量分析 48 2.8.1 氣相層析質譜儀 (Gas Chromatography, GC) 48 2.8.2 二氧化碳還原電解器介紹 49 2.9 X光吸收光譜 (X-ray absorption spectroscopy, XAS) 50 2.9.1 吸收邊緣 (The absorption edge) 52 2.9.2 X光吸收過程 (X-ray absorption process) 52 2.9.3 X光吸收光譜的種類 (Classification of X-ray absorption spectroscopy) 53 2.9.4 X光吸收近邊緣結構(X-ray absorption near-edge spectroscopy, XANES) 53 2.9.5 延伸 X光吸收細微結構（Extended X-ray absorption fine structure, EXAFS) 54 第三章 結果與討論 58 3.1 鐵單原子材料之材料鑑定 58 3.1.1 鐵單原子材料之合成方法 58 3.1.2 X光繞射分析 58 3.1.3 電子顯微鏡分析 59 3.1.4 拉曼光譜分析 63 3.1.5 X光光電子能譜分析 63 3.1.6 FeNC之電子結構分析 64 3.2 電催化尿素氧化反應分析 69 3.2.1 線性掃描伏安法分析 69 3.2.2 尿素氧化反應之產物分析 72 3.3 臨場技術之分析 74 3.3.1 臨場X光吸收譜分析 74 3.3.2 臨場拉曼光譜分析 78 3.4 鐵金屬催化劑之尿素氧化反應機制探討 80 3.4.1 尿素氧化反應之機制驗證 81 3.5 UOR//CO2RR系統之效能探討 84 第四章 結論 86 第五章 文獻 87 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 臨場分析 | zh_TW |
| dc.subject | 氮氣選擇性 | zh_TW |
| dc.subject | 單原子催化劑 | zh_TW |
| dc.subject | 尿素氧化反應 | zh_TW |
| dc.subject | in situ measurement | en |
| dc.subject | urea oxidation reaction | en |
| dc.subject | single-atom catalyst | en |
| dc.subject | N2 selectivity | en |
| dc.title | 臨場分析鐵單原子催化劑於尿素氧化反應之動態結構變化 | zh_TW |
| dc.title | Operando analyzing the dynamic structure of Fe single atomic catalyst in urea oxidation reaction | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 111-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 廖尉斯;林律吟;陳効謙;童敬維 | zh_TW |
| dc.contributor.oralexamcommittee | Wei-Ssu Liao;Lu Yin Lin ;Hsiao-Chien Chen;Chine-Wei Tung | en |
| dc.subject.keyword | 尿素氧化反應,單原子催化劑,氮氣選擇性,臨場分析, | zh_TW |
| dc.subject.keyword | urea oxidation reaction,single-atom catalyst,N2 selectivity,in situ measurement, | en |
| dc.relation.page | 92 | - |
| dc.identifier.doi | 10.6342/NTU202303395 | - |
| dc.rights.note | 未授權 | - |
| dc.date.accepted | 2023-08-10 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| 顯示於系所單位： | 化學系 | |
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