以金屬離子作為均相共催化劑提升赤鐵礦電極分解水效率之研究

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研究生：	鄭宇容 Cheng, Yu Jung
論文名稱：	以金屬離子作為均相共催化劑提升赤鐵礦電極分解水效率之研究 Enhanced Water Splitting Efficiency of Hematite Electrodes with Metal Ions via Photoelectrochemical process
指導教授：	王竹方 Wang, Chu Fang
口試委員:	蔣本基 Chiang, Pen Chi 談駿嵩 Tan, Chung Sung
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：	89
中文關鍵詞：	光電化學、赤鐵礦、鈍化、表面態
外文關鍵詞：	Photoelectrochemistry, hematite, passivation, surface states
相關次數：	點閱：2 下載：0
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表面態的鈍化(passivation surface state )可以降低起始光電流電位，利用減緩荷姆霍茲層(Helmholtz layer)費米能階釘化現象(Fermi level pinning effect)，抑制載子再結合損失而增加光電流效率。本研究發現溶液中的金屬離子可以作為現地表面態的均相鈍化劑，提高赤鐵礦電極的光電效能，在所研究的金屬離子中，利用鉻離子、亞鐵離子、鈷離子、銅離子以及鋅離子作為現地表面態的均向鈍化劑顯著提升赤鐵礦光電流30 ~ 300 %，但高濃度的鎳離子則導致的赤鐵礦光電極的光電流大幅下降，而錳離子對光電流並沒有明顯的影響。因此，本研究推測，表面態可能與赤鐵礦表面的高親和性吸附位置相關，而表面態透過吸附反應吸附金屬離子因而鈍化，被吸附的金屬離子在赤鐵礦/溶液界面同時誘發蕭特基能障效應(Schottky barrier effect)延伸能帶彎曲，因此顯著提升光電化學效能。此外，表面態鈍化效應也與金屬離子本身的化學特性有高度的相關性。

Surface states passivation is known capable of reducing onset photocurrent potential through reducing Fermi level pinning effect occurring at Helmholtz layer and enhancing photocurrent plateau via suppressing recombination loss at space charge region. In this preliminary study, we noted that solution metal ions could function as in situ homogeneous surface passivation reagents and thus improve photoelectrochemical performance of hematite electrodes. Among examined metal ions, Cr(III), Fe(II), Co(II), Cu(II) and Zn(II) were found to enhance the photocurrent by 30 - 300 % while Ni(II) significantly reduces the PEC performance and Mn(II) has no significant influence. We further hypothesized that these surface states might be high affinity adsorption sites on hematite surfaces. Once they are occupied with solution metal ions, surface states are passivated along with the induced Schottky barrier effect at the hematite/solution interface created by adsorbed metal ions and therefore PEC performance is greatly enhanced.

中文摘要                                            I
ABSTRACT                                    II
謝誌                                            III
CONTENTS                                    V
FIGURE INDEX                                    VIII
CHAPTER  1 INTRODUCTION                         1
CHAPTER  2 LITERATURE REVIEW                    5
2.1 WATER SPLITTING                            5
2.2 SURFACE STATE EFFECT ON PHOTOANODE            11
2.3 HEMATITE PHOTOANODES                    13
CHAPTER  3 EXPERIMENTAL                            15
3.1 CHEMICAL REAGENTS                            15
3.2 EXPERIMENTAL INSTRUMENTS                    16
3.2.1 Inductively coupled plasma-Mass Spectroscopy (ICP-MS)                                            16
3.2.2 X-Ray Diffraction (XRD)                18
3.2.3 Scanning electron microscope (SEM)    20
3.2.4 Electrochemical Analyzer/Workstation    21
3.2.5 X-ray photoelectron spectroscopy (XPS)    22
3.3 EXPERIMENTAL METHODS                    24
3.3.1 Preparation of α-Fe2O3 photoanodes    24
3.3.2 Photoelectrochemical measurements      25
3.3.3 The metal ions adsorbed on hematite nanoparticles 26         
3.3.4 Electrochemical impedance spectroscopy         28
3.3.5 Structural and morphological characterization  28
CHAPTER  4 RESULT AND DISCUSSION            29
4.1 CHARACTERIZATIONS OF FABRICATED PHOTOANODES    29
4.1.1 Morphology of hematite photoanodes    29
4.1.2 Photoelectrochemical behaviour            31
4.1.3 Cyclic voltammetry                    37
4.2 METAL IONS ADSORPTION ON HEMATITE NANOPARTICLES  54
4.3 EFFECT OF METAL IONS ON HEMATITE PHOTOANODES     64
4.3.1 Concentration effect of metal ions on hematite 64
4.3.2 Oxidation states of metal ions on hematite     65
CHAPTER  5 CONCLUSIONS AND FUTURE WORKS      66
5.1 CONCLUSIONS                                 66
5.2 FUTURE WORKS                            67
REFERENCE                                    68
APPENDIX                                    86

                                

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