博碩士論文 109329007 詳細資訊




以作者查詢圖書館館藏 以作者查詢臺灣博碩士 以作者查詢全國書目 勘誤回報 、線上人數:130 、訪客IP:18.227.114.218
姓名 黃定為(Ting-Wei Huang)  查詢紙本館藏   畢業系所 材料科學與工程研究所
論文名稱 釕-銅雙金屬電催化觸媒於廣酸鹼值電解液的高效析氫反應
(Ruthenium-Copper Bimetallic Electrocatalyst for Efficient Hydrogen Evolution Reaction in Wide pH Values)
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摘要(中) 電化學水分解製氫是追求潔淨和持續能源的一種有效途徑。實際應用中,具高效能、經濟、簡便的析氫反應(hydrogen evolution reaction, HER)被高度關注。儘管鉑(Pt)在酸性介質中具有快速的動力學和最佳的氫鍵能(hydrogen bonding energy, HBE),但其在鹼性介質中的穩定性和活性不佳,阻礙了其在廣泛pH值範圍內之實際應用。
在此,本研究提出非鉑基之釕銅觸媒(RuCu),透過增加結晶性和添加過渡金屬(銅)用以調整觸媒之HBE,使其可應用於酸鹼介質中並具有高活性。RuCu在0.5 M H2SO4和1.0 M KOH電解液中,在電流密度10 mA cm-2時過電位(η10)分別僅32和8 mV 且Tafel 斜率分別為36和37 mV dec-1。此外,RuCu在鹼性介質中進行5000圈加速老化測試後幾乎零損失。值得注意的是,RuCu在鹼性介質中甚至比Pt具有更快的反應動力學、更低的Tafel斜率和更高的轉換頻率(turnover frequency, TOF)。另一方面,釕-銅之間的交互作用對HER的效能影響也由一系列的物理分析及電化學量測證實,如於CO剝離測試、毒化測試和原位X光吸收光譜(in-situ X-ray absorption spectroscopy, in-situ XAS)分析RuCu的活性位點及其HER機制。本研究為製備高效能HER觸媒於酸鹼性介質的應用提供新的思維。
摘要(英) 電化學水分解製氫是追求潔淨和持續能源的一種有效途徑。實際應用中,具高效能、經濟、簡便的析氫反應(hydrogen evolution reaction, HER)被高度關注。儘管鉑(Pt)在酸性介質中具有快速的動力學和最佳的氫鍵能(hydrogen bonding energy, HBE),但其在鹼性介質中的穩定性和活性不佳,阻礙了其在廣泛pH值範圍內之實際應用。
在此,本研究提出非鉑基之釕銅觸媒(RuCu),透過增加結晶性和添加過渡金屬(銅)用以調整觸媒之HBE,使其可應用於酸鹼介質中並具有高活性。RuCu在0.5 M H2SO4和1.0 M KOH電解液中,在電流密度10 mA cm-2時過電位(η10)分別僅32和8 mV 且Tafel 斜率分別為36和37 mV dec-1。此外,RuCu在鹼性介質中進行5000圈加速老化測試後幾乎零損失。值得注意的是,RuCu在鹼性介質中甚至比Pt具有更快的反應動力學、更低的Tafel斜率和更高的轉換頻率(turnover frequency, TOF)。另一方面,釕-銅之間的交互作用對HER的效能影響也由一系列的物理分析及電化學量測證實,如於CO剝離測試、毒化測試和原位X光吸收光譜(in-situ X-ray absorption spectroscopy, in-situ XAS)分析RuCu的活性位點及其HER機制。本研究為製備高效能HER觸媒於酸鹼性介質的應用提供新的思維。
關鍵字(中) ★ 釕
★ 銅
★ 析氫反應
★ X光吸收光譜
★ 氫鍵能
關鍵字(英) ★ Ruthenium
★ Cooper
★ Hydrogen evolution reaction
★ Crystallinity
★ Hydrogen bonding energy
★ X-ray absorption spectrum
論文目次 摘要 I
Abstract II
致謝 III
Table of Contents V
List of Figures VII
List of Tables X
Chapter 1 Introduction 1
1.1 Mechanism of HER 2
1.2 Ru-based electrocatalysts 4
1.3 Crystallinity dependence of Ru electrocatalysts 7
1.4 Motivation and approach 9
Chapter 2 Experimental Section 10
2.1 Preparation of catalysts 10
2.1.1 Reagents 10
2.1.2 Synthesis of RuCux/C catalysts 10
2.1.3 Synthesis of Ru/C catalysts 11
2.2 Characterization of catalysts 12
2.3 Electrochemical characterization 14
Chapter 3 Results and Discussion 17
3.1 The characterizations of catalysts 17
3.2 The electrochemical characterizations of catalysts 28
3.2.1 HER performance of catalysts 28
3.2.2 The active sites and HER mechanism of catalysts 44
Chapter 4 Conclusions 55
Reference 56
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指導教授 王冠文(Kuan-Wen Wang) 審核日期 2022-6-9
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