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研究生:Mulu Alemayehu Abate
研究生(外文):Mulu Alemayehu Abate
論文名稱:水相合成三元(I-III-VI2)量子點於量子點敏化太陽能電池
論文名稱(外文):Aqueous synthesis of ternary (I-III-VI2) quantum dots for quantum dots-sensitized solar cells
指導教授:張家耀張家耀引用關係
指導教授(外文):Jia-Yaw Chang
口試委員:葉旻鑫王丞浩江志強林正嵐黃志清張家耀
口試委員(外文):Min-Hsin YehChen-Hao WangJyh-Chiang JiangCheng-Lan LinChih-Ching HuangJia-Yaw Chang
口試日期:2019-10-23
學位類別:博士
校院名稱:國立臺灣科技大學
系所名稱:化學工程系
學門:工程學門
學類:化學工程學類
論文種類:學術論文
論文出版年:2019
畢業學年度:108
語文別:英文
論文頁數:174
中文關鍵詞:Quantum dotsQuantum dot sensitized solar cellsDouble passivation shellAgInSe2Lattice mismatchAgInSe2CuInS2CuInSe2Intermediate band
外文關鍵詞:Quantum dotsQuantum dot sensitized solar cellsDouble passivation shellLattice mismatchAgInSe2CuInS2CuInSe2Intermediate band
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於現今量子點敏化太陽能電池(QDSSCs)之研究中,設計出一高效能太陽能電池其元件組成間之界面反應為最重要的因素,其元件主要分為三個部分–光電極、背電極及電解液,而本研究主要針對元件之光電極進行改善,研究內容會分為三個部分進行探討。
第一部分是探討AgInSe2 (AISe)量子點與雙鈍化層(CdS、ZnS)之間的晶格不匹配程度與光電轉換效率之關係。本實驗主要在AISe量子點與ZnS鈍化層中嵌入一CdS鈍化層並形成AISe/CdS/ZnS (core/shell/shell)雙鈍化層的形式,並藉此CdS鈍化層不僅可逐步改善原本AISe/ZnS間晶格不匹配程度高之原因,亦可大幅降低量子點的導帶上的電子被電解液的氧化還原電位所捕獲(逆電流)。而此AISe/CdS/ZnS雙鈍化層之太陽能電池其效率(PCE)為6.27 %,是目前量子點敏化劑以銀為主的QDSSCs中最高之效率。
第二部分是在量子點敏化劑中利用錳(Mn)摻雜於銅銦硒(CuInSe2, CISe)量子點,並探討其Mn濃度與PCE的變化。在QDSSCs中的光電極部分,其量子點敏化劑會因Mn的摻雜並在TiO2與CISe量子點的導帶間產生中間能階,再分別利用IMPS和IMVS檢測可發現Mn摻雜不僅可縮短受光激發後電子注入TiO2的時間,並加快其注入的速率以利電子傳導至導電玻璃,以避免受光激發至量子點導帶的電子再與量子點價帶之電洞再結合,因此亦同時可發現其電子-電洞再結合之時間有增長的現象,且其最高光電轉換效率為6.28 %。
第三部分是比較不同鈍化層披覆量子點表面並觀察PCE之變化。利用新穎的三元素CdZnS鈍化層披覆於量子點表面,不僅可有效抑制光電極與電解液之界面間的電子電洞再結合,還可提升光子捕獲的機率,使其QDSSCs之PCE從沒有鈍化層的3.99 %提升至8.83 %。
In the present study, Interfacial engineering of the photoanode has been one of the most important strategies in designing high-performance quantum dot (QD)-sensitized solar cells (QDSSCs). In this work, we demonstrated a promising route to enhance the photovoltaic performance by inserting an additional CdS inner shell between AgInSe2 (AISe) QDs and a ZnS outer shell to obtain an AISe/CdS/ZnS core/shell/shell QDSSC. These double passivation shells not only provided a gradual stepwise change in the lattice parameter to suppress the interface strain but also acted as a stepped potential barrier to prevent current leakage from the QDs to the electrolyte. As a result, the AISe QDSSC with CdS/ZnS double passivation shells exhibited a remarkably high conversion efficiency (6.27%), which is significantly higher than those of devices without a passivation shell (1.02%) and with CdS (4.37%) or ZnS (5.23%) single passivation shells. To the best of the authors’ knowledge, this efficiency is one of the highest values obtained for an Ag-based QDSSC.
The second part of this thesis presents, herein, we present a direct aqueous synthesis of manganese (Mn) doped CuInSe2 (Mn-CISe) quantum dots (QDs) under microwave irradiation to improve photochemical properties of the solar cells. As a result of Mn doping, the narrower bandgap energy in Mn-CISe leads to higher visible light absorption. The Mn-CISe QDs are then used as photosensitizers in quantum dot- sensitized solar cells (QDSSCs), exhibiting an enhanced performance that is dependent on the Mn concentration. To the best of our knowledge, this is the first time to construct an Mn-CISe sensitized-TiO2 photoanode to boost the photovoltaic performance in QDSSCs. The incorporation of Mn into CISe increases short-circuit current which is ascribed to effective injection of excited electrons from QDs to TiO2 and the consequent higher electron lifetime, likely through a newly formed Mn midgap in the CISe band structure. Compare to the undoped QDs, Mn-CISe QDSSCs show a shorter electron transport time (τt) and a longer electron recombination time (τr) which are studied by the intensity-modulated photocurrent spectroscopy (IMPS) and intensity-modulated photovoltage spectroscopy (IMVS), respectively. Actually, a combination of higher light-harvesting efficiency, slower charge recombination, and longer electron lifetime give rise to the maximum photovoltaic performance of 6.28%.
The third part of this thesis presents, the proper use of surface passivation layer in quantum dot (QD)-sensitized solar cells (QDSSCs) plays a crucial role in preventing surface charge recombination and, thus, improving the overall power conversion efficiency (PCE). In this work, we introduced a novel and facile ternary (CdZnS) passivation layer to enhance the photovoltaic performance of QDSSCs. Consequently, the device exhibits remarkably enhanced short-circuit current (JSC), open-circuit voltage (VOC), fill factor (FF), and power conversion efficiency (PCE). The QDSSCs with a CdZnS passivation layer confirmed strongly inhibited interfacial charge recombination and greatly enhanced light harvesting, resulting in a PCE of up to 8.83%, which is appreciably higher than 7.17% for the solar cells with a ZnS passivation layer and 3.99% for the solar cells without a passivation layer.
CHINESE ABSTRACT i
ABSTRACT iii
ACKNOWLEDGMENTS v
TABLE OF CONTENTS vi
LIST OF FIGURES xi
LIST OF TABLES xv
LIST OF SCHEMES xvi
LIST OF ABBREVIATIONS xvii
CHAPTER-ONE 1
INTRODUCTION 1
1.1. GENERAL INTRODUCTION 2
1.2. OBJECTIVE OF THE STUDY 5
1.3. STRUCTURE OF THE DISSERTATION 6
CHAPTER-TWO 8
LITERATURE REVIEW 8
2.1. NANOPARTICLES 9
2.2. Semiconductor Quantum dots (QDs) 10
2.3. Unique properties of quantum dots (QDs) 13
2.3.1. Quantum confinement effect 13
2.3.2. Multiple Exciton Generation (MEG) 15
2.4. Quantum Dot Sensitized Solar Cells (QDSSCs) 17
2.5. Recent progress in photoanodes, counter electrodes, and electrolytes of QDSSCs 20
2.5.1. Photoanodes 20
2.5.2. Counter electrodes (CEs) 22
2.5.3. Polysulfide electrolytes 25
2.6. Working mechanism of QDSSCs 28
2.7. QDSSCs photovoltaic performance measurements 29
2.8. Deposition of QD films and core/shell structure of QDs 32
2.8.1. Doctor blading, Screen printing and Spin coating 33
2.8.2. Chemical bath deposition (CBD) 35
2.8.3. Successive ionic layer deposition (SILAR) 36
2.8.4. Electrophoretic deposition (EPD) 37
2.8.5. Linker-molecule assisted self-assembly 38
2.9. Core/shell structure of QDs 43
2.10. Synthesis of I-III-VI2 QDs 44
2.10.1. Nucleation and growth 46
2.10.2. Hot injection method 48
2.10.3. Non-injection (heating up) approach 49
2.10.4. Solvothermal approach 50
2.10.5. Hydrothermal approach 51
2.10.6. Microwave irradiation approach 52
CHAPTER-THREE 55
Boosting the efficiency of AgInSe2 quantum dot sensitized solar cells via core/shell/shell architecture 55
3.1. INTRODUCTION 56
3.2. EXPERIMENTAL SECTION 60
3.2.1. Materials 60
3.2.2. Preparation of mesoporous TiO2 60
3.2.3. Preparation of AISe QDs 61
3.2.4. Photoanode sensitization 61
3.2.5. Device fabrication 62
3.2.6. Sample characterization 63
3.3. RESULTS AND DISCUSSION 64
3.4. SUMMARY 80
CHAPTER-FOUR 81
Aqueous synthesis of Mn-doped CuInSe2 quantum dots to enhance the performance of quantum dot sensitized solar cells 81
4.1. INTRODUCTION 82
4.2. EXPERIMENTAL SECTION 85
4.2.1. Materials 85
4.2.2. Preparation of mesoporous TiO2 85
4.2.3. Preparation of CISe and Mn-CISe QDs 86
4.2.4. Photoanode sensitization 86
4.2.5. Device fabrication 87
4.2.6. Sample characterization 87
4.3. RESULTS AND DISCUSSION 89
4.4. SUMMARY 100
CHAPTER-FIVE 101
Novel ternary passivation layer for the Cu-based (CuInS2 and CuInSe2) quantum dots to enhance the performance of quantum dot sensitized solar cells 101
5.1. INTRODUCTION 102
5.2. EXPERIMENTAL SECTION 105
5.2.1. Materials 105
5.2.2. Fabrication of TiO2 photoanode 106
5.2.3. Preparation of CIS QDs 106
5.2.4. Photoanode sensitization 107
5.2.5. Device fabrication 107
5.2.6. Sample characterization 108
5.3. RESULTS AND DISCUSSION 109
5.4. SUMMARY 120
CHAPTER-SIX 121
CONCLUSIONS AND FUTURE OUTLOOKS 121
6.1. Conclusions 122
6.2. Future outlooks 124
REFERENCES 126
APPENDIX 146
CURRICULUM VITA 153
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