利用有機酸添加物以電沉積法誘發碳覆蓋層對赤鐵礦電極結構與光催化特性研究

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研究生：	蔣嘉哲 Chiang, Chia Che
論文名稱：	利用有機酸添加物以電沉積法誘發碳覆蓋層對赤鐵礦電極結構與光催化特性研究 The Structural and Photocatalytic Characteristics of Induced Elemental Carbon Overlayers Hematite Electrodes Prepared by Electrodeposition with Organic Acid Additives
指導教授：	王竹方 Wang Chu Fang
口試委員:	談駿嵩 Tan, Chung Sung 蔣本基 Chiang, Pen Chi
學位類別：	碩士 Master
系所名稱：	原子科學院 - 生醫工程與環境科學系 Department of Biomedical Engineering and Environmental Sciences
論文出版年：	2016
畢業學年度：	104
語文別：	英文
論文頁數：	90
中文關鍵詞：	電沉積、赤鐵礦、水分解、碳包覆、有機酸
外文關鍵詞：	electrodeposition, hematite, water splitting, carbon-coated, organic acid
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本研究發現利用電鍍法來製備赤鐵礦電極時，在電鍍液中添加不同親和力有機酸都會誘發碳覆蓋層的產生，且所製備的光電極其光電流密度和製備電鍍液的pH值具有顯著相關性，可以透過有機酸與氧化鐵之間吸附吸附平衡關係解釋，此外，厚度2~5奈米的碳包覆赤鐵礦電極可提升10倍的光電流，達到2 mA/cm2 (0.4 V vs SCE) 的表現。雖然厚度2~5奈米碳包覆層可以鈍化赤鐵礦表面態階(surface state)，但經過90分鐘的照光後，赤鐵礦與碳包覆層之間的界面會形成一個電容，導致光電流下降。根據本研究結果，一個有效的碳包覆層的特性包含: (i) 可透過鈍化表面態階讓降低光電流起始電壓， (ii) 提升赤鐵礦電極載子濃度，(iii) 增強電極的穩定性，以維持長時間的陽光照射。

In this study, we found that it could be an universal case that an elemental carbon overlayer would be induced when hematite electrodes are prepared using electrodeposition with additional organic acid additives in the electrolyte. Their photocurrent densities are strongly dependent on the electrolyte pH where they were prepared as the thickness of elemental carbon ovrelayers is regulated by the amount of adsorbed organic acids on electroreduced iron oxyhydroxides during electrodeposition. An optimal carbon overlayer approximately 2~5 nm would lead the PEC performances up to around 2 mA/cm2 (0.4 V vs SCE), which is almost 10 times higher than those without carbon overlayers. While carbon overlayers would effectively passivate surface states, their degradation in the end of 90 minutes of illumination would lead a capacitor feature occurring at hematite/carbon overlayer interface and therefore compromises the PEC performance. Based on our results, characteristic of an effective carbon overlayer might include: (i) passivating surface states to reduce onset photocurrent potential, (ii) doping additional charges to enhance photocurrent plateau, and (iii) enhanced stability to sustain a long period of sunlight illumination.

目錄Contents
中文摘要                                                 I
Abstract                                               II
謝誌                                                  III
Chapter 1 Introduction                                  1
Chapter 2 Literature Review                             4
1 Water Splitting                                     4
1.1 Photocatalyst                                     4
1.2 Energy gap                                        5
1.3 Photoelectrochemical System                       7
2 Hematite                                            9
3 Hematite photoanodes                               11
3.1 The development of hematite photoanodes          11
3.2 The recent development of electrochemical methods to synthesize hematite                                 13
3.3 Element-doped hematite photoanode                15
3.4 Surface passivation of hematite photoanode       16
4 Organic acid                                       17
5 Electrochemical impedance spectroscopy (EIS)       17
5.1 Electrochemical impedance spectroscopy           17
5.2 Flat band potential                              21
Chapter 3 Experimental                                 23
1 Chemical Reagents and Instruments                  23
1.1 Chemical Reagents                                23
1.2 Experimental Instruments                         23
2 Preparation of hematite electrode                  24
3 PEC measurements                                   26
4 Experimental and Analysis Equipment                27
4.1 Zetasizer for zeta potential measurement         27
4.2 Electrochemical Analyzer/Workstation             28
4.3 Transmission electron microscopy (TEM)           29
4.4 Energy dispersive X-ray spectroscopy (EDX)       31
4.5 Total Organic Carbon (TOC) Analyzer              31
4.6 X-ray photoelectron spectroscopy (XPS)           33
4.7 Scanning electron microscope (SEM)               34
5 Experimental Methods                               35   
5.1. Zeta potential measurement                      35
5.2. Photoelectrochemical characterization           36
5.3 Adsorption experimen                             37
5.4 Electrochemical impedance spectroscopy (EIS)     38
5.5 Structural and morphological characterization    39
Chapter 4 Results and Discussion                       40
1 Identification of mechanism of preparing hematite electrode                                              40
2 Characters of hematite electrodes                  43
2.1 Photoelectrochemical behavior                    43
2.2 The thickness of carbon overlayer                45
2.3 The effect of thickness of carbon overlayer against PCE performance                                        52
2.4 Characteristic of effective carbon overlayer     54
3 The durability of hematite electrodes              71
3.1 PEC performance under long time illumination     71
3.2 The reasons of photocurrent degradation.         72
Chapter 5 Conclusions and Future Works                 75
1 Conclusions                                        75
2 Future Works                                       76
Chapter 6 Reference                                    77
Appendix                                               84


                                

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