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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 | 陳彥妤 | zh_TW |
| dc.contributor.author | Yen-Yu Chen | en |
| dc.date.accessioned | 2023-10-03T17:16:02Z | - |
| dc.date.available | 2023-11-09 | - |
| dc.date.copyright | 2023-10-03 | - |
| dc.date.issued | 2023 | - |
| dc.date.submitted | 2023-08-11 | - |
| dc.identifier.citation | 1. Pareek, A.; Dom, R.; Gupta, J.; Chandran, J.; Adepu, V.; Borse, P. H., Insights into renewable hydrogen energy: Recent advances and prospects. Materials Science for Energy Technologies 2020, 3, 319-327.
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/90706 | - |
| dc.description.abstract | 隨著化石燃料使用率的提升導致二氧化碳排放逐年上升，全球暖化的問題越來越嚴重，因此通過開發綠氫來取代化石燃料能源有助於減少二氧化碳的排放。其中，電解水產氫反應（HER）可以說是現今開發綠氫的一大主流，有許多研究已經開發多種不同電催化劑以提高產氫效率，並通過薩巴捷原理之火山圖呈現並解釋。在薩巴捷原理中，鍵結能是探討這個原理中最關鍵的因素，但是鍵結能的概念從理論預測或從實驗的角度來說都非常具有挑戰性，因此本研究將透過HER來深入探討其中。
本研究主要是通過簡單的HER機制了解關於反應中間體之鍵結能及電荷儲存在電催化劑表面之現象。對於反應中間體的探討，大多數的研究都是透過薩巴捷原理來解釋，然而實際上，真實反應過程中之環境複雜性及結構變動性造成與薩巴捷原理之火山圖形有所偏差。因此在本研究中，我們將通過探討5d單金屬原子模型在HER中的電荷儲存來了解中間體的鍵結性質，其中電荷儲存的情況會反應到氫電荷的覆蓋率，並透過固液界面中中間體之分子內相互作用決定，而這又與d電子的數量有直接的相關性。從臨場實驗結果中發現當動態d電子數為5時，可以達到一個最佳的分子內相互作用從而提供最佳的反應活性、最低的電荷轉移電阻及最少的電荷累積，也因此推敲出固液界面的結構及其對應之等效電路。通過這些發現我們可以將實驗和理論之間的關聯性連結起來，也能夠更準確的去設計出活性優異的催化劑材料，此外本研究提出之模型也可以被應用至其他電催化反應。 | zh_TW |
| dc.description.abstract | With the increasing use of fossil fuels leading to a rise in carbon dioxide emissions year by year, the issue of global warming is becoming increasingly severe. Therefore, developing green hydrogen as a substitute for fossil fuel energy helps reduce carbon dioxide emissions. Among various methods, the hydrogen evolution reaction (HER) through water electrolysis has become a major mainstream approach for green hydrogen production. Many studies have been conducted to develop different electrocatalysts to enhance hydrogen production efficiency and are explained using the Sabatier volcano plot. In the Sabatier principle, bond energy is a crucial factor, but the concept of bond energy is challenging from both theoretical predictions and experimental perspectives. Thus, this study aims to delve into the HER process to gain a deeper understanding.
The primary focus of this research is to comprehend the bond energy of reaction intermediates and the charge storage phenomenon on the electrocatalyst surface during the HER mechanism. Previous studies have mostly explained the reaction intermediates through the Sabatier principle. However, due to the complexity of the actual reaction environment and structural variations, there are deviations from the volcano plot of the Sabatier principle. Therefore, in this study, we investigate the charge storage on 5d single-atom catalysts (SACs) models during HER to understand the bonding properties of intermediates. The charge storage affects the coverage of hydrogen charges, determined by the intramolecular interactions at the solid-liquid interface and directly related to the number of d-electrons. From in-situ experimental results, we find that when the dynamic d-electron count is 5, the optimal intramolecular interactions can be achieved, leading to the best reaction activity, lowest charge transfer resistance, and minimal charge accumulation. This insight helps deduce the structure of the solid-liquid interface and its corresponding equivalent circuit. By connecting these findings, we can establish a link between experiments and theories and design more accurate catalyst materials with excellent activity. Additionally, the proposed model in this study can be applied to other electrocatalytic reactions as well. | en |
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| dc.description.provenance | Made available in DSpace on 2023-10-03T17:16:02Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 摘要 i
Abstract iii 目錄 v 圖目錄 viii 表目錄 xv 第一章 文獻探討 1 1.1 能源危機與替代能源 1 1.2 氫能 1 1.3 電解水產氫反應（Electrocatalytic Hydrogen Evolution Reaction, HER） 3 1.3.1 HER機制 4 1.3.2 HER分析方法12 5 1.3.2.1 過電位（Overpotential）12 5 1.3.2.2 塔菲爾分析（Tafel analysis） 6 1.3.3 單原子催化劑（Single Atom Catalysts, SACs） 7 1.3.3.1 SACs的簡介及優勢 8 1.3.3.2 SACs的種類及在電解水產氫反應的應用 8 1.3.3.2.1異原子的摻雜（heteroatom doping） 9 1.3.3.2.2原子缺陷（atom defects） 19 1.3.3.2.3空間和/或配位上的限制（spatial and/or coordination confinement） 20 1.4 薩巴捷原理（Sabatier principle） 22 1.4.1 簡介 22 1.4.2 d電子調控 23 1.4.2.1 藉由改變中心金屬調控d電子 24 1.4.2.2 藉由改變基材調控d電子 24 1.5研究動機與目的 25 第貳章 藥品與儀器原理分析 28 2.1 藥品、溶劑、氣體資訊 28 2.2 儀器原理及分析 29 2.2.1 高角度環形暗場像-掃描透射電子顯微鏡（High-Angle Annular Dark-Field Scanning Transmission Electron Microscopy, HAADF-STEM） 29 2.2.2 穿透式電子顯微鏡（Transmission Electron Microscope, TEM） 30 2.2.3 能量色散X光光譜儀（Energy-Dispersive X-ray Spectroscopy, EDS） 31 2.2.4 感應耦合電漿質譜儀（Inductively Coupled Plasma Mass Spectroscopy, ICP-MS） 31 2.2.5 X光繞射儀（X-ray Diffraction, XRD） 33 2.2.6 X光吸收光譜（X-ray Absorption Spectroscopy, XAS） 34 2.2.6.1 概述 34 2.2.6.2 XAS 組成與特徵 35 2.2.6.3 XAS數據分析方法 36 2.2.7 電化學分析 38 2.2.7.1概述 38 2.2.7.2 線性掃描伏安法（Linear Sweeping Voltammetry, LSV） 39 2.2.7.3 循環伏安法（Cyclic Voltammetry, CV） 40 2.2.7.4 計時電流法（Chronoamperometry, CA） 41 第三章 水分解的電荷存儲化學研究 43 3.1 實驗部分 43 3.1.1 材料製備方式 43 3.1.2 電化學量測 43 3.1.3 In-house鑑定 44 3.2.4 臨場XAS量測 44 3.2.5 EXAFS擬合 45 3.2.6 電化學參數細節 45 3.2.6.1 脈衝伏安圖（PV）和總表面電荷 45 3.2 結果與討論 46 3.2.1 M-NC在HER的電催化反應 46 脈衝伏安圖與總表面電荷討論 56 3.2.2 M-NC電催化劑的電荷存儲化學 60 氧化價態之線性關係討論 62 EXAFS擬合結果討論 66 3.2.3 總電荷與動態d電子之間的關聯性 70 金屬位點的電子轉移數量 73 雙層電荷和偽電荷 76 3.3 結論 77 第四章 參考文獻 78 | - |
| dc.language.iso | zh_TW | - |
| dc.subject | 單原子催化劑 | zh_TW |
| dc.subject | 臨場光譜分析 | zh_TW |
| dc.subject | 電解水產氫反應 | zh_TW |
| dc.subject | X光吸收譜 | zh_TW |
| dc.subject | 中間體 | zh_TW |
| dc.subject | HER | en |
| dc.subject | in-situ spectroscopy | en |
| dc.subject | XAS | en |
| dc.subject | single-atom catalysts | en |
| dc.subject | intermediates | en |
| dc.title | 電催化產氫之表面電荷效應 | zh_TW |
| dc.title | Surface-charging effect on electrocatalytic hydrogen evolution | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 111-2 | - |
| dc.description.degree | 碩士 | - |
| dc.contributor.oralexamcommittee | 林律吟;廖尉斯;陳効謙;童敬維 | zh_TW |
| dc.contributor.oralexamcommittee | Lu-Yin Lin;Wei-Ssu Liao;Hsiao-Chien Chen;Ching-Wei Tung | en |
| dc.subject.keyword | 單原子催化劑,電解水產氫反應,臨場光譜分析,X光吸收譜,中間體, | zh_TW |
| dc.subject.keyword | single-atom catalysts,HER,in-situ spectroscopy,XAS,intermediates, | en |
| dc.relation.page | 88 | - |
| dc.identifier.doi | 10.6342/NTU202303675 | - |
| dc.rights.note | 同意授權(全球公開) | - |
| dc.date.accepted | 2023-08-12 | - |
| dc.contributor.author-college | 理學院 | - |
| dc.contributor.author-dept | 化學系 | - |
| dc.date.embargo-lift | 2028-08-08 | - |
| 顯示於系所單位： | 化學系 | |
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