液相沉積NixFe1-xOy在氧化鐵光陽極應用在太陽能產氫

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李彥瑾(Yan-Jin Li) 查詢紙本館藏

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機械工程學系

論文名稱

液相沉積NixFe1-xOy在氧化鐵光陽極應用在太陽能產氫
(Solution-phase deposition of NixFe1-xOy on hematite photoanode as electocatalyst for application to solar-hydrogen production)

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摘要(中)

太陽能產氫是有效產氫方式之一。太陽能水分解的理想材料應具有以下性質：適當的能帶邊緣位置，帶隙小，良好的電子和空穴傳輸特性，以及高的化學穩定性。對於赤礦鐵材料載子擴散距離短、導帶位置低於氫還原電位限制了該材料在光電化學催化技術中的發展應用。因此，本研究利用脈衝雷射濺鍍沉積(Pulsed-laser deposition method, PLD)製備氧化鐵奈米薄膜於FTO導電玻璃上成長氧化鐵奈米陣列薄膜，解決氧化鐵載子擴散距離短問題，提升光電流密度；液相沉積(Solution-phase deposition, SPD)，在氧化鐵上沉積一層催化劑，改善表面能階位置不合適問題，降低起始電位。
本研究中，我們成功以脈衝雷射濺鍍沉積製備氧化鐵奈米薄膜，並在薄膜表面以液相沉積的方式沉積NixFe1-xOy作為Fe2O3/SnO2光陽極上的電催化劑。這方法允許我們可控制NixFe1-xOy催化劑覆蓋層的組成和厚度。其中以前驅物鎳鐵含量比為8:2製成之電極在光電流密度電性測試中性質最佳，起始電位為0.85 V (vs. RHE)，在1.4 V (vs. RHE)測得的光電流密度值為0.55 mA/cm2。

摘要(英)

Solar hydrogen production is one of the promising methods for hydrogen generation. In photoelectrochemical method, hydrogen is generated by using a water-splitting device composed of a photoanode and a photocathode immersed in electrolyte (KOH, H2SO4, etc). To achieve this goal efficiently, the material of photoelectrodes should have properties of appropriate band edges, small bandgap, great electron (hole) conductivity, high chemical stability and high natural abundance. Hematite has great properties of appropriate bandgap and high chemical stability, but short carrier diffusion distances and conduction band below water reduction level limit its performance. Therefore, we proposed a strategy including optimization of carrier density in hematite photoanode and modification of surface state position using pulsed laser deposition (PLD) and solution-phase deposition (SPD). The optimal samples showed the onset potential of 0.85 V (vs. RHE) and current density of 0.55 mA/cm2 at 1.4 V (vs. RHE).

關鍵字(中)

★ 光電化學產氫
★ 雷射脈衝沉積法
★ 氧化鐵
★ 催化劑

關鍵字(英)

★ Solar hydrogen production
★ Pulsed laser deposition
★ Hematite
★ Electrocatalyst

論文目次

中文摘要 I
ABSTRACT II
目錄 III
表目錄 VI
圖目錄 VII
第一章、緒論 1
1-1研究背景 1
1-2研究動機 2
第二章、研究背景與動機 4
2-1光電化學水分解 4
2-2半導體能帶觀念 5
2-2-1能帶與能隙 5
2-2-2費米分佈函數 7
2-2-3半導體水溶液界面性質 9
2-3目前常見水分解光陽極材料 15
2-3-1氧化鐵光陽極 17
2-4催化劑 18
2-5脈衝雷射濺鍍沉積法 22
2-6研究目的 23
第三章、實驗方法 24
3-1實驗流程 24
3-2氧化錫與氧化鐵靶材製備 24
3-3基材準備 27
3-4電極製備 28
3-4-1脈衝雷射沉積奈米結構薄膜 28
3-4-2吸附Co(II)離子 30
3-4-3表面蝕刻+催化劑(FeOOH) 30
3-4-4液相沉積NiFeOx薄膜 31
3-5電極封裝 31
3-6奈米結構薄膜特性分析 32
3-6-1場發式電子顯微鏡 32
3-6-2穿透式電子顯微鏡 33
3-7電極效能分析 33
3-7-1開路電位 35
3-7-2光電流密度 35
3-7-3交流阻抗分析 36
3-7-4 Mott-Schottky 37
第四章、結果與討論 39
4-1脈衝雷射濺鍍沉積法製備氧化鐵薄膜研究 39
4-1-1熱處理溫度影響 40
4-1-2 沉積時氣壓對薄膜影響 44
4-1-3 氧化鐵氧化程度的影響 48
4-2吸附CO離子 51
4-3表面蝕刻+催化劑(FeOOH) 52
4-4液相沉積NiXFe1-XOY 53
4-4-1不同Ni:Fe比例溶液沉積薄膜影響 55
4-4-2不同沉積時間對薄膜影響 60
第五章、結果與建議 64
5-1 結論 64
5.2 未來工作建議 66
參考文獻 67

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指導教授

曾重仁(Chung-jen Tseng)

審核日期

2017-7-28

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