以含水深共熔溶劑電化學系統製備奈米鎳銅合金/碳纖維氈複合電極應用於水分解製氫

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曾棻彥(Fen-Yan Zeng) 查詢紙本館藏

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化學工程與材料工程學系

論文名稱

以含水深共熔溶劑電化學系統製備奈米鎳銅合金/碳纖維氈複合電極應用於水分解製氫
(Development of Nickel-Copper Carbon Felt Electrodes in Water-Containing Deep Eutectic Solvent-based Electrochemical System for Water Splitting)

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至系統瀏覽論文 (2028-6-30以後開放)

摘要(中)

為因應全球淨零碳排放趨勢，尋求可再生能源來解決能源危機和環境問題是首要辦法。其中，氫能因具有高能量密度與低碳排等特色，被視為傳統高汙染產業的重要替代能源。然而，水電解製氫因為在過程中沒有二氧化碳的排放，是近幾年主要用來生產氫氣的方式之一，但受昂貴的催化劑價格與高過電位影響，限制了氫氣的製備效率和可行性。為了解決這些問題，本研究致力於開發低成本的過渡金屬催化劑來取代貴金屬催化劑，材料的選擇上，以具有高催化活性與適當氫吸附能的鎳及銅金屬，透過金屬合金化的方式，在三維結構的碳纖維氈基材上，通過一步驟電沉積來合成鎳銅合金複合材料，並進一步將催化材料應用於水電解產氫。
本研究在無外加水(0 wt.%)及不同比例外加水(1 wt.%、3 wt.%以及5 wt.%)之氯化膽鹼/乙二醇深共熔系統中，進行恆電位電沉積。實驗中，分別在-1.5 V(V vs Ag/AgCl sat, KCl)及-2V(V vs Ag/AgCl sat, KCl)的電壓下進行材料的製備。從結果發現，在深共熔系統中添加額外水，除有助於使得沉積結構更均勻外，對於鎳銅合金比例也具調控性。其中，以-2NiCu(3)/CF複合材料在1.0 M KOH溶液中表現出最優異的析氫(27 mV@10 mA/cm2)與析氧(390 mV@50 mA/cm2)過電位表現，透過金屬間的協同作用以及添加水導致的更細緻結構，有助於活性位點數量的提升，對於催化性能產生直接影響。另外，該複合材料在長時間的水電解產氫也展現優異的穩定性，水電解電壓達1.52 V，優於商業上常見之水電解槽，代表在含微量水的深共熔系統中製備雙功用電催化劑，是相當有潛力的做法，這將對於綠氫的生產提供更多的選擇性。

摘要(英)

Energy is a crucial element in modern daily life and has a significant impact on our future. Hydrogen, a clean-burning fuel, can be produced from various sources and applied in multiple industries, such as transportation and power generation. Water electrolysis, using electricity to split water molecules into hydrogen and oxygen, is an environmentally friendly method to produce pure hydrogen. However, there are still obstacles to overcome, such as the high drive voltage and high cost of production. Transition metal-based materials are regarded as a potential solution to this issue due to their cost-effectiveness and high catalytic activity for water electrolysis, as suggested by many studies. Our research proposes a one-step electrodeposition method in a choline chloride/ethylene glycol deep eutectic solvent (ChCl/EG DES) with varying water content to fabricate nickel-copper alloy/carbon fiber felt composite electrodes for water splitting.
Based on the materials analysis, it can be confirmed through XRD, SEM, and XPS analyses that the Nickel-Copper alloy can be effectively synthesized using the water-containing DES system. The catalyst electrode synthesized at -2 V in ChCl/EG with 3 wt.% water exhibits an excellcent hydrogen evolution (HER) overpotential (27 mV@10 mA/cm2) in 1.0 M KOH solution, outperforming previously reported values. The smaller charge transfer impedance and Tafel slope indicate that the Nickel-Copper alloy/CF electrode has high electron transport efficiency, which facilitates chemical reactions. In addition, the stability of the electrode is confirmed by a 12 hour chronopotentiometry test, and the overall water splitting voltage obtained by the stability test is lower than that of commercial devices, indicating that the composite electrode has the potential to replace commercial catalysts. Its outstanding catalytic performance proves that the one-step electrodeposition in the water-containing DES system is a feasible method for synthesizing composite electrodes.

關鍵字(中)

★ 含水深共熔溶劑
★ 鎳基合金催化劑
★ 水電解
★ 析氫
★ 析氧

關鍵字(英)

★ Deep eutectic solvent
★ Nickel-based alloy catalyst
★ Water electrolysis
★ Hydrogen Evolution
★ Oxygen Evolution

論文目次

摘要 i
致謝 iii
目錄 v
圖目錄 viii
表目錄 xii
第一章、序論 1
1-1能源的發展 1
1-2氫能源種類 2
1-3全球氫能源發展 3
1-4目前電解產氫技術概況 4
1-5水電解原理 7
1-5-1 陰極析氫反應(Hydrogen Evolution Reaction,HER) 7
1-5-2 陽極析氧反應(Oxygen Evolution Reaction,OER) 10
1-6 深共熔溶劑(Deep Eutectic Solvents,DES) 12
1-6-1 深共熔溶劑種類 13
1-6-2深共熔溶劑形成機制 15
1-6-3目前深共熔溶劑實際應用範圍 16
1-7 研究動機 18
第二章、文獻回顧 19
2-1 常見之析氫催化劑 19
2-2 常見之析氧催化劑 23
2-3 提升催化活性之方式 27
2-4合金材料常見之合成方式 29
2-5合金材料優勢 31
2-6 氯化膽鹼-乙二醇深共熔系統電沉積相關應用 32
2-7 含水的深共熔系統電沉積相關應用 33
第三章、實驗方法 37
3-1 實驗架構 37
3-2 實驗步驟 40
3-2-1碳氈基材前處理 40
3-2-2 深共熔溶劑的製備 40
3-2-3 鎳銅合金複合電極的製備 41
3-2-4電極材料之電化學分析 42
3-3 複合電極材料之材料分析 43
3-3-1 傅立葉轉換紅外線光譜儀 (Fourier-Transform Infrared Spectroscopy, FTIR) 44
3-3-2 流變儀 (Rheometers) 44
3-3-3 導電度計 (Conductivity Meter) 45
3-3-4 X射線繞射儀 (X-ray Diffraction, XRD) 45
3-3-5 場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscope, FE-SEM) 46
3-3-6 X射線光電子能譜儀 (X-ray photoelectron spectroscopy , XPS) 46
3-4 複合電極材料之電化學分析 47
3-4-1 線性掃描伏安法 (Linear Sweep Voltammetry,LSV) 48
3-4-2 塔佛動力學 (Tafel Kinetics) 49
3-4-3 電化學阻抗圖譜 (Electrochemical Impedance Spectroscopy,EIS) 49
3-4-4 電雙層電容 (Double-Layer Capacitance,Cdl) 50
3-4-5 恆電流測試(Chronopotentiometry test,CP) 50
3-4-6 腐蝕電位(Corrosion Potential) 51
3-4-7 產氫效率 52
3-4-8 氣相層析質譜儀 53
第四章、結果與討論 54
4-1 碳氈基材前處理分析 54
4-2 無水及含少量水之氯化膽鹼/乙二醇深共熔溶劑性質分析 56
4-2-1 無水氯化膽鹼/乙二醇深共熔溶劑之FTIR分析 56
4-2-2 含水氯化膽鹼/乙二醇深共熔溶劑之FTIR分析 56
4-2-3 含水氯化膽鹼/乙二醇深共熔溶劑之導電度及粘度分析 59
4-3 電觸媒複合材料之材料分析 62
4-3-1 電觸媒複合材料之XRD分析 62
4-3-2 電觸媒複合材料之SEM分析 63
4-3-3 電觸媒複合材料之EDS分析 67
4-3-4 電觸媒複合材料之XPS分析 69
4-4 含水氯化膽鹼/乙二醇深共熔溶劑中鎳銅合金複合材料形成機制 72
4-5 電觸媒複合材料之電性分析 73
4-5-1線性掃描伏安: 析氫過電位分析 73
4-5-2線性掃描伏安法: 析氧過電位分析 79
4-5-3 塔佛動力學:複合材料之動力學分析 85
4-5-4 電化學阻抗:複合材料之動力學分析 87
4-5-5 電雙層電容:複合材料之電化學活性面積分析 92
4-5-6 腐蝕電位:複合材料之耐腐蝕性測試 96
4-5-7 恆電流測試:複合材料之長期穩定性分析 99
4-5-8 法拉第效率:複合材料之析氫及析氧效能分析 102
4-5-9 氣相層析質譜儀:析氫端產氫純度分析 104
第五章、結論與未來展望 105
5-1 結論 105
5-1-1 含水深共熔系統製備鎳銅合金複合材料 105
5-1-2 鎳銅合金複合材料之電化學表現 107
5-2 未來展望 109
參考文獻 110

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指導教授

劉奕宏(Yi-Hung Liu)

審核日期

2023-8-11

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