含水深共熔溶劑系統電化學製備之奈米氫氧化鎳/鎳/碳纖維氈複合電極應用於水分解製氫

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郭虹妏(Hong-Wen Guo) 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

含水深共熔溶劑系統電化學製備之奈米氫氧化鎳/鎳/碳纖維氈複合電極應用於水分解製氫
(Electrochemical Fabrication of Nanostructured Ni(OH)2/Ni/Carbon Felt Electrodes in Water-Containing Deep Eutectic Solvent System for Hydrogen Production via Water Splitting)

相關論文

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至系統瀏覽論文 (2027-6-30以後開放)

摘要(中)

為因應全球能源轉型，再生能源的需求與日俱增，氫能源因其高能量密度和零污染而受到關注。其中水電解是生產氫氣最「綠色」的方法之一，其由陰極的析氫和陽極的析氧組成，過程中不涉及碳的產出。然而這兩種電化學過程都面臨著反應動力學緩慢的狀況，商用及過去所研究的水電解系統額外的高過電位以及催化材料昂貴的價格使得水電解產氫的成本居高不下。已有許多研究試圖開發低成本的過渡金屬催化劑來取代商用的貴金屬催化劑，其中以鎳基材料的性能最為理想，尤其是異質的鎳基催化結構。在本研究中，我們提供了一種於含水氯化膽鹼/尿素深共熔溶劑 (Deep Eutectic Solvent, DES)中進行的一步驟電沉積程序，利用該系統來製備奈米結構的氫氧化鎳/鎳/碳纖維氈複合電極，以催化整體水分解析氫。
實驗使用含有不同水量(1.86 wt.%、11.69 wt.%以及21.67 wt.%)的氯化膽鹼/尿素DES作為電沉積溶液，並改變施加的電壓做為電沉積的參數。我們發現在含水DES的體系中可以合成鎳/氫氧化鎳異質催化結構，-1.5CU10W複合電極表面超薄的氫氧化鎳奈米片為析氫及析氧反應提供豐富的活性位點，並且氫氧化鎳和鎳之間的協同作用以及活性Ni3+物質的存在為析氫及析氧提供了有利的條件。該電極在鹼性溶液中表現出超低的析氫過電位(30 mV@10 mA/cm2)，優於大多數報導的值。較小的塔佛斜率和電荷轉移阻抗表明-1.5CU10W複合電極具有良好的催化動力學和快速的電子傳輸能力。此外，由穩定性測試所得的電解槽析氫電壓為1.69 V，表明-1.5CU10W複合電極具有實際用作雙功能催化劑的潛力。根據複合電極所表現的優異催化性能，我們認為含水DES系統的電沉積是一種製備高活性催化劑的有效方法。

摘要(英)

In response to the global energy transition, the demand for renewable energy has increased recently, and hydrogen energy has attracted attention owing the high energy density and zero greenhouse gas emission. Water electrolysis is one of the most ′′green′′ tactics to produce highly pure hydrogen. In general, water splitting is consisted of anodic oxygen evolution (OER) and cathodic hydrogen evolution reaction (HER). However, these two electrochemical processes are faced with sluggish reaction kinetics, leading to a higher electrolysis voltage, increased energy consumption and hydrogen price. Many studies have attempted to develop low-cost transition metal catalysts to replace commercial noble metal catalysts, among which the performance of nickel-based materials is the most ideal, especially the heterostructure nickel-based catalyst. In this work, we provide a one-step electrodeposition process in water-containing choline chloride/urea deep eutectic solvent (ChCl/urea DES) to prepare nanostructured nickel hydroxide/nickel/carbon fiber felt composite electrodes for water splitting.
According to the materials characterizations, we found that the Ni(OH)2/Ni heterostructure can be successfully synthesized by the water-containing DES system. The -1.5CU10W electrode with ultrathin nickel hydroxide nanosheets on the surface possesses an enriched active site. Also, the possible synergistic effects between Ni(OH)2 and Ni as well as the presence of active Ni3+ species lead to the enhanced HER and OER performance. It is worth noting that -1.5CU10W electrode exhibits an ultra-low HER overpotential (30 mV@10 mA/cm2) in alkaline solution, which is better than most reported values. The smaller Tafel slope and charge transfer impedance indicate that -1.5CU10W electrode has good catalytic kinetic and fast electron transportability. Furthermore, The overall cell voltage obtained by the stability test was 1.69 V, indicating that -1.5CU10W electrode has the potential to replace commercial catalysts. The excellent catalytic performance of the composite electrode suggests that the electrodeposition in a water-containing DES system is an efficient strategy to prepare highly active catalysts.

關鍵字(中)

★ 深共熔溶劑
★ 水分解
★ 析氫
★ 析氧
★ 鎳基催化劑

關鍵字(英)

★ Deep Eutectic Solvents
★ Water Splitting
★ Hydrogen Evolution
★ Oxygen Evolution
★ Nickel-Based Catalysts

論文目次

摘要 i
Abstract ii
致謝 iii
目錄 v
圖目錄 viii
表目錄 xi
第一章、序論 1
1-1氫能源的發展 1
1-2氫能源的製造 2
1-3水電解產氫 4
1-3-1陰極析氫反應(Hydrogen Evolution Reaction, HER) 4
1-3-2陽極析氧反應(Oxygen Evolution Reaction, OER) 6
1-3-3 整體水電解電位 7
1-4複合電極 8
1-4-1電極基材 8
1-4-2催化材料之性能衡量 9
1-4-3 催化劑材料的介紹 11
1-5深共熔溶劑(Deep Eutectic Solvents, DESs) 16
1-5-1深共熔溶劑的類別 17
1-5-2基於氯化膽鹼的深共熔溶劑之形成機制 19
1-5-3深共熔溶劑的應用領域 21
1-6研究動機 23
第二章、文獻回顧 24
2-1奈米結構鎳基觸媒 24
2-2自支撐觸媒電極 26
2-3鎳基異質催化劑 29
2-4 基於氯化膽鹼的深共熔溶劑—催化材料的電沉積 31
2-5含水的深共熔溶劑系統 34
2-5-1 水對於深共熔溶劑奈米結構的影響 36
2-5-2 含水DES的金屬電沉積 38
第三章、實驗方法 40
3-1 實驗架構 40
3-2 實驗步驟 43
3-2-1 深共熔溶劑的製備 43
3-2-2 鎳基複合電極的電沉積 43
3-3 材料分析 46
3-3-1 傅立葉轉換紅外線光譜儀 (Fourier-Transform Infrared Spectroscopy, FTIR) 47
3-3-2 流變儀 (Rheometers) 47
3-3-3 X射線繞射儀(X-ray Diffraction, XRD) 47
3-3-4 X射線光電子能譜儀 (X-ray Photoelectron Spectroscopy, XPS) 48
3-3-5高解析場發射掃描式電子顯微鏡 (Field Emission Scanning Electron Microscope, FE-SEM) 48
3-3-6高解析穿透式電子顯微鏡 (Transmission Electron Microscopy, TEM) 49
3-4 複合電極的電化學分析 49
3-4-1 過電位 (Overpotential, η) 50
3-4-2 塔佛斜率 (Tafel slope, b) 51
3-4-3 電化學阻抗分析 (Electrochemical Impedance Spectroscopy, EIS) 52
3-4-4 電化學活性表面積 (Electrochemical Active Surface Area, ECSA) 52
3-4-5 穩定性測試 (Stability) 53
3-4-6 法拉第效率(Faradaic Efficiency) 53
第四章、結果與討論 55
4-1 無水及含水氯化膽鹼/尿素DES之性質分析 55
4-1-1 氯化膽鹼/尿素DES之FTIR分析 55
4-1-2 含水氯化膽鹼/尿素DES之FTIR分析 55
4-1-3 含水氯化膽鹼/尿素DES之黏度與電導率分析 57
4-2 複合電極的材料分析 60
4-2-1 複合電極的XRD分析 60
4-2-2 複合電極的SEM分析 63
4-2-3 複合電極的XPS分析 68
4-2-4複合電極的HRTEM分析 71
4-3 含水氯化膽鹼/尿素DES中氫氧化鎳/鎳的沉積機制 75
4-4 複合電極的催化性能分析 78
4-4-1 析氫極化曲線：過電位分析 78
4-4-2 析氧極化曲線：過電位分析 83
4-4-3電極動力學分析：塔佛斜率 86
4-4-4電極動力學分析：電化學阻抗分析 88
4-4-5電化學活性表面積的評估 93
4-4-6長期穩定性測試 96
4-4-7 產氫效果的評估：法拉第效率 98
第五章、結論與未來展望 100
5-1結論 100
5-1-1含水氯化膽鹼/尿素DES電沉積系統 100
5-1-2複合電極的析氫/析氧催化活性 102
5-2 未來展望 104
參考文獻 105
附錄一 115
附錄二 119

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指導教授

劉奕宏

審核日期

2022-8-8

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