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研究生： 何宗曄
Tsung-Yeh Ho
論文名稱： 以硫化銅鋅錫敏化之二氧化鈦奈米柱進行光電水分解之研究
The study of Cu2ZnSnS4 sensitized TiO2 nanorods photoanode on photoelectrochemical water splitting
指導教授： 陳良益
Liang-Yih Chen
口試委員: 劉豫川
陳浩銘
陳詩芸
江志強
學位類別： 博士
Doctor
系所名稱： 工程學院 - 化學工程系
Department of Chemical Engineering
論文出版年： 2017
畢業學年度： 106
語文別： 英文
論文頁數： 158
中文關鍵詞： 硫化銅鋅錫 、二氧化鈦 、水分解 、產氫 、表面修飾
外文關鍵詞： hydroge
相關次數： 點閱：194  下載：0 
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    • 本研究主要探討以硫化銅鋅錫(Cu2ZnSnS4)作為二氧化鈦奈米柱之敏化材料於光電水分解產氫之應用。硫化銅鋅錫(Cu2ZnSnS4)為p型直接能隙半導體，由於其具有低成本、無毒性、材料來源充足及合適的能隙值(~1.5 eV)之優點，因此非常適合作為光伏元件或光電水分解之吸收材料。於本研究中吾人首先利用水熱法合成長一維二氧化鈦奈米柱於透明導電基板上，並藉由不同的黏著層（硫化銅、硫化二銅、硫化鎘）的輔助，將硫化銅鋅錫奈米粒子以化學浴沈積法(CBD)均勻的沉積於二氧化鈦奈米柱上。最後吾人利用硫化鋅(ZnS)做為表面修飾來提升元件的效率。於不同的黏著層中，以硫化二銅(Cu2S)做為黏著層的元件擁有最佳的效率。其光電流密度可以達到5.81 mA/cm2。藉由電化學阻抗頻譜（EIS）分析中吾人得知，硫化二銅黏著層可以輔助硫化銅鋅錫中的電子與電洞分離，而硫化鋅表面修飾可以輔助硫化銅鋅錫中的電洞傳遞至電解液中。此外吾人利用硫化鋅以及二氧化矽雙層修飾來更進一步提昇元件的效率以及穩定度。在經過硫化鋅以及二氧化矽雙層修飾後，二氧化鈦/硫化銅鋅錫電極的表面活性及界面化學電容值（chemical capacitance）皆有所下降。因此吾人推測二氧化矽可以修飾電極表面之表面態（surface state）並減低電極表面的載子再結合發生。經過硫化鋅以及二氧化矽雙層修飾後的電極，其光電流密度可以提升到7.95 mA/cm2。而經過4小時的穩定性量測後，其光電流密度仍然能夠保持其起始值的82 %。

    Cu2ZnSnS4 (CZTS), which owning suitable bandgap and band position, high absorption coefficient, is a suitable sensitizer for photovoltaic or photoelectrochemical (PEC) application. In this study, CZTS nanoparticles were decorated on TiO2 NRAs with adhesion layer by using solvothermal method. Different kinds of adhesion layers, such as CdS, CuS, Cu2S, were employed to enhance the uniformity of CZTS. Finally, ZnS layer was used as passivation layer for increasing conversion efficient. By using Cu2S adhesion layer and ZnS passivation layer, the photocurrent density of TiO2/Cu2S(6)/CZTS/ZnS(5) electrode can reach 5.81 mA/cm2 @1.23 V vs RHE. According to electrochemical impedance spectroscopy (EIS) analysis, the Cu2S adhesion layer assisted the charge separation in CZTS due to the cascade band structure, and the ZnS passivation layer helped the photogenerated hole transfer from CZTS to the electrolyte. Besides, the stability of the CZTS in the electrolyte solution is one of the major problems for long time usage. To further improve the stability as well as the PEC performance of CZTS sensitized TiO2 electrode, the ZnS and SiO2 dual passivation layers are employed to passivate the surface of the CZTS. The tafel measurement and electrochemical impedance spectroscopy are used to understand the mechanism of the SiO2 over layer. After the SiO2 decoration, the activity of the device decrease a little and the surface state chemical capacity also decrease. Therefore, the SiO2 Over layer seems to be a surface passivation layer, which can passivate the surface defect and increase the efficient of the device. The photocurrent of the device with ZnS and SiO2 dual passivation layers can reach 7.92 mA/cm2 @1.23 V vs. RHE. The photocurrent density of the photoelectrode with dual passivation remained 82% of its initial value after 4 hours measurement.

    口試委員會審定書 # 誌謝 i 中文摘要 ii ABSTRACT iii CONTENTS iv LIST OF FIGURES viii LIST OF TABLES xvi NOMENCLATURE xvii Chapter 1 Introduction 1 1-1 Climate change 1 1-2 Hydrogen energy 5 1-3 Photoelectrochemical hydrogen generation 10 1-4 Literature reviews 16 1-5 Focus of this thesis 23 1-6 Reference 24 Chapter 2 Theory and Experiment 31 2-1 Theory of photoelectrochemical (PEC) cell 31 2-1-1 Semiconductor physics 31 2-1-2 Semiconductor/electrolyte interface 33 2-1-3 Water splitting reaction 36 2-1-4 Solar to hydrogen conversion efficiency 37 2-2 Experimental schematic diagram 39 2-3 Chemical reagents and apparatus 40 2-3-1 Chemical reagents 40 2-3-2 Apparatus 45 2-3-3 Analysis instruments 46 2-4 References 60 Chapter 3 Growth of Oriented Single-Crystalline Rutile TiO2 Nanorod Arrays for PEC water splitting 62 3-1 Introduction 62 3-2 Experimental section 63 3-2-1 Preparation of TiO2 NR arrays 63 3-2-2 Characteristics 64 3-3 Results and discussion 65 3-3-1 Effect of initial reactant concentration 67 3-3-2 Effect of the amount of HCl solution 69 3-3-3 Effect of the growth time 70 3-4 Conclusions 72 3-5 References 73 Chapter 4 The Effect of Different Adhesion Layer on CZTS Sensitized TiO2 PEC Water Splitting 75 4-1 Introduction 75 4-2 Experimental section 77 4-2-1 Preparation of TiO2 NR arrays 77 4-2-2 Deposition of adhesion layer 77 4-2-3 Deposition of CZTS absorption layer and ZnS passivation layer 78 4-2-4 Characteristics 79 4-3 Results and discussion 80 4-3-1 CdS as adhesion layer 84 4-3-2 CuS and Cu2S as adhesion layer 94 4-4 Conclusions 105 4-5 References 106 Chapter 5 CZTS sensitized TiO2 Photoanode with ZnS and SiO2 Dual Passivation Layer for Water Splitting 111 5-1 Introduction 111 5-2 Experimental section 112 5-2-4 Deposition of SiO2 passivation layer 113 5-2-5 Characteristics 113 5-3 Results and discussion 114 5-4 Conclusions 124 5-5 References 125 APPENDIX A 127 APPENDIX B 128 APPENDIX C 134

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    無法下載圖示 全文公開日期 2022/11/17 (校內網路)
    全文公開日期 2027/11/17 (校外網路)
    全文公開日期 2027/11/17 (國家圖書館：臺灣博碩士論文系統)
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