PVP-capped Pt Nano-Clusters as Catalyst for Counter Electrode of Dye Sensitized Solar Cell and Grid-type DSSC Module

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研究生：	藍若琳 Lan, Jo-Lin
論文名稱：	PVP-capped Pt Nano-Clusters as Catalyst for Counter Electrode of Dye Sensitized Solar Cell and Grid-type DSSC Module 高分子包覆奈米鉑簇運用於染料敏化太陽能電池與模組之陰極研究
指導教授：	萬其超 Wan, Chi-Chao
口試委員:	王詠雲刁維光顏溪成胡啟章梁榮昌
學位類別：	博士 Doctor
系所名稱：	工學院 - 化學工程學系 Department of Chemical Engineering
論文出版年：	2011
畢業學年度：	100
語文別：	英文
論文頁數：	182
中文關鍵詞：	染料敏化太陽能電池及模組、奈米鉑對電極
相關次數：	點閱：3 下載：0
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We have developed (Poly-N-vinyl-2-pyrrolidone) PVP-capped Pt nano-clusters on transparent conductive oxide (TCO) glasses via a simple “2-step dip coating process” as counter electrode for DSSC. This new counter electrode was examined by transmission electron microscopy (TEM), inductively coupled plasma-atomic emission spectroscopy (ICP-AES), electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), thermal gravimetric analysis (TGA), and current-voltage curve (I-V curve). The TEM results reveal that PVP-capped Pt nano-clusters’ size is about 3nm, and the amount of Pt deposited on ITO glass is about 5 μg/cm2. TGA results show that the optimum annealing condition for PVP-capped Pt nanoclusters counter electrode (PVP-Pt CE) is around 270oC 15mins, and charge transfer resistance (RCT) was found below 1 ohm-cm2 and the power conversion efficiency with this counter electrode could exceed 9%.
Besides being deposited on TCO glass, PVP-capped Pt nano-clusters can also be coated on flexible carbon fiber paper via the same “2-step dip coating process”. This kind of counter electrode has not only acceptable catalytic activity, but low sheet resistance, cheap cost and flexibility. In addition, the production can employ by continuous spinning technology under ambient conditions in the future. Hence mass production will be much easier and less expensive.
Furthermore, the durability of PVP-Pt CE on TCO glass for dye-sensitized solar cell (DSSC) has been extensively evaluated including electrochemical reaction durability, thermal stress durability and light soaking durability. It is revealed that PVP-Pt CE exhibits both electrochemical and thermal durability by cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) test. As for the device thermal durability, both low-volatile and non-volatile electrolyte systems were tested and the results show that the relative efficiency can remain above 85 % after accelerated thermal test at 85oC for 1000 hours, and 110% after 60oC for 1000 hours. For the light soaking test under 60oC after 1000 hours, the relative efficiency can still be maintained at 94%.
We also applied PVP- Pt CE to large scale grid-type DSSC module, and studied the correlation between the resistive loss and the output power by altering the Ag grid pattern. Further indoor application of grid-type DSSC module was integrated with a fluorescent lamp stand. In order to improve the DSSC performance at various incident light conditions, the relationship between the power conversion efficiency and the electrochemical impedance spectrum was explored, and we found that the iodine concentration in the electrolyte was key factor affecting the DSSC performance. Therefore, by optimizing the composition of electrolyte for low incident light condition, we can improve the output power by nearly 15% for each DSSC module.

Abstract   I
中文摘要   III
Table of Contents   V
List of Tables   XI
List of Figures   XIII

Chapter 1     Introduction of solar energy and solar cell    1
1-1    Solar Energy    1
1-2    Working Mechanism of Solar Cell: P-N Junction    3
1-3    Generations of Solar Cells    4
1-4    Market of Solar Cells in 2009    7

Chapter 2     Introduction of Dye-sensitized Solar Cell    ...9
2-1    Working Mechanism of DSSCs    ...9
2-2    Material and Process…….    .11
2-2-1    Electrode Substrate    .11
2-2-2    Meso-porous Semiconductor Film— Photo-anode    12
2-2-2-1 Material    12
2-2-2-2 Preparation of Anatase TiO2 Paste    16
2-2-2-3 Preparation of Meso-porous TiO2 Film    17
2-2-2-4 Structure of Meso-porous TiO2 Film    17
2-2-2-4-1 Titania Nanotube Arrays in DSSCs    17
2-2-2-4-2 Morphology of Titania Nanoparticles Film    19
2-2-2-5 Pre- and Post-treatment for Meso-porous TiO2 Film    21
2-2-3    Dye- the sensitizer    22
2-2-4    Counter Electrode    25
2-2-4-1 Platinum-based Counter Electrode    26
2-2-4-2 Carbon-based Counter Electrode    29
2-2-4-3 Conducting Polymer-based Counter Electrode    30
2-2-5    Electrolyte    31
2-2-5-1 Redox Couple    31
2-2-5-2 Liquid-based Electrolyte    32
2-2-5-3 Quasi- Solid State Electrolyte    33
2-2-5-4 Solid State and Electrolyte    33
2-2-5-5 Additive & Cation Effect in the Electrolyte    34
2-3    Recombination Reaction (Back Reaction) of DSSCs    37
2-4    Configuration of DSSCs    39
2-4-1 Tandem cell    39
2-4-2 DSSC Module    40
2-5    Stability of DSSCs    43
2-5-1 Degradation Mechanism – Component Analysis    43
2-5-2 The Standard Environmental and Endurance Test for DSSCs    46
2-6    Outdoor Performance of DSSC Module    48
2-6-1 Temperature Effect    48
2-6-2 Light Intensity Effect    49
2-6-3 Angle of Light Incidence Effect    50
2-7    Analysis of DSSCs    52
2-7-1 Photoelectrochemical Characterization- IV curve    52
2-7-2 Incident Photon-to-Current Conversion Efficiency (IPCE)    56
2-7-3 ac-Impedance Spectrum and Model of a Standard Dye-sensitized
 Solar Cell    57
2-7-4 Electron Diffusion Length- IMPS, IMVS    62
2-8    Motivation of this study    64

Chapter 3    High Efficiency and Low Cost PVP-capped Pt Nano-clusters Counter Electrode for Dye-sensitized Solar Cell    66
3-1    Introduction    67
3-2    Experimental    69
3-2-1    Materials & Reagents    69
3-2-2    Preparation of PVP-capped Pt nano-clusters Counter Electrode    69
3-2-3    Preparation of the Solaronix Thermal Cluster Pt-catalyst
 T/SP Counter Electrode    70
3-2-4    Electrodes Preparation and Assembly of DSSCs    70
3-2-5    Characterization    71
3-3    Results and Discussions    72
3-3-1    PVP-capped Pt Nano-particle Size Measurement in Suspension    72
3-3-2    The Pt Loading on TCO glass with Various Preparations of
Counter Electrode    73
3-3-3    The Cyclic Voltammetry Results with Various Preparations
 of Counter Electrode    73
3-3-4    The Electrochemical Impedance Spectroscopy (EIS) Analysis
with Various Preparations of Counter Electrode    75
3-3-5    The Photocurrent-voltage (I-V) Curves with Various Preparations
 of Counter Electrode    77
3-3-6    Thermal Treatment of PVP-capped Pt Counter Electrode     78
3-3-7    The Electrochemical Impedance Spectroscopy (EIS) Analysis
with Various Thermal Treatment for PVP-Pt CE    80
3-3-8    Cell Efficiency of PVP capped-Pt Counter Electrode    82
3-4    Conclusions    84

Chapter 4    Platinum Nano-clusters on Flexible Carbon Fiber Paper without Transparent Conducting Oxide Glass as Counter Electrode for Dye-sensitized Solar Cells    85
4-1    Introduction    86
4-2    Experimental    88
4-2-1 Materials and Reagents    88
4-2-2 Sample Preparation    88
4-2-2-1 PVP-capped Pt Nano-clusters Suspension    88
4-2-2-2 Preparation of the PVP-capped Pt Nan-oclusters
Counter Electrode    88
4-2-2-3 Preparation of the Porous TiO2 Photo-anode    89
4-2-2-4 Cell Assembling    90
4-2-2-5 Characterization    90
4-3    Results and Discussions    91
4-3-1 The SEM Image    91
4-3-2 The Pt Loading on Different Substrate    92
4-3-3 The Electrochemical Impedance Spectroscopy (EIS) Analysis    92
4-3-4 The Photocurrent-voltage (I-V) Characteristics    ..93
4-4 Conclusions    ..95

Chapter 5    Durability Test of PVP-capped Pt Nano-clusters Counter Electrode for Highly Efficiency Dye-sensitized Solar Cell        ..96
5-1    Introduction    …..97
5-2    Experimental    ..99
5-2-1 PVP-capped Pt Nano-clusters Suspension    ..99
5-2-2 Preparation of the PVP-capped Pt Nano-clusters Counter Electrode .99
5-2-3 Preparation of the Porous TiO2 Photo-anode    ..99
5-2-4 Electrolyte    100
5-2-5 Characterization    101
5-3    Results and Discussions    102
5-3-1 Catalytic Performance of PVP-Pt CE After Post Heat Treatment    102
5-3-2 The Power Conversion Efficiency of DSSC with PVP-Pt CE    104
5-3-3 Durability Test    105
5-3-3-1 Electrochemical Durability–Cyclic Voltammetry    105
5-3-3-2 Thermal Durability: 60oC and 85oC Thermal Stress Test    108
5-3-3-2-1 Symmetric Cell Test    108
5-3-3-2-2 The Whole Cell Test    110
5-3-4 Light Soaking Experiment    112
5-4   Conclusions    113

Chapter 6    The Electrochemical Impedance Spectroscopy of Dye-Sensitized Solar Cell With Respect to Iodine Concentrations and Light Intensities    114
6-1      Introduction    ..115
6-2      Experimental    ..117
6-2-1 Preparation of the PVP-capped Pt Nano-clusters Counter Electrode.117
6-2-2 Preparation of the Porous TiO2 Photo-anode………………………..117
6-2-3 Electrolyte    ..118
6-2-4 Characterization    ..118
6-3      Results and Discussions    ..119
6-3-1 EIS of a Standard Dye-sensitized Solar Cell    ..119
6-3-2 Power Conversion Efficiency and Impedance Spectrum at 1 Sun
(AM 1.5)    ..120
6-3-3 Power Conversion Efficiency and Impedance Spectrum at 0.5
Sun    126
6-3-4 Comparison of Efficiency and Impedance under Various
     Sun Conditions    128
6-4      Conclusions    130

Chapter 7    Fabrication of Grid Type Dye Sensitized Solar Modules with 7% Conversion Efficiency by Utilizing Commercially Available Materials and its Application for Indoor Fluorescent Lamp    131
7-1     Introduction    132
7-2     Experimental    134
7-2-1 Preparation of Photo-anode    134
7-2-2 Preparation of the PVP-capped Pt Nanoclusters Counter Electrode.135
7-2-3 Module Fabrication………………………………………………...136
7-2-4 Electrolyte Composition……………………………………………138
7-2-5 Module Characterization……………………………………………138
7-3     Results and Discussions    139
7-3-1 Performance Comparison of Different Design Grid-type
DSSC modules    139
7-3-2 Further Improvement on Conversion Efficiency    144
7-3-3 Thermal Stability of Grid-type DSSC Module    146
7-3-4 Grid-type DSSC Lamp Module and Its application for
Indoor Fluorescent Lamp    148
7-3-4-1 The Design of Grid-type DSSC Lamp Module    148
7-3-4-2 I-V Parameters under 1 Sun Condition    149
7-3-4-3 I-V Parameters under Fluorescent Light Condition    151
7-3-4-4 DSSC Lamp Module Connected in Series    152
7-4     Conclusions    153


Chapter 8    Conclusions and Future Works    154
8-1    Conclusions    154
8-2    Suggestions for Further Experiments    156

Chapter 9    References    157
Chapter 10 Publications    177

                                

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