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軸配位子で酸化物半導体表面に結合した色素を有する色素増感太陽電池の作製とその特性解明
https://doi.org/10.18997/00003769
https://doi.org/10.18997/00003769cd30fb71-7c0e-477f-985d-25090baf791a
| 名前 / ファイル | ライセンス | アクション |
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D-147_sei_k_174.pdf (9.5 MB)
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| Item type | 学位論文 = Thesis or Dissertation(1) | |||||||||
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| 公開日 | 2013-11-01 | |||||||||
| 資源タイプ | ||||||||||
| 資源タイプ識別子 | http://purl.org/coar/resource_type/c_db06 | |||||||||
| 資源タイプ | doctoral thesis | |||||||||
| タイトル | ||||||||||
| タイトル | Analysis for Axially Anchored Metal Complexed Macrocyclic Dyes on Surface of Mesoscopic Metal Oxide for DSSC | |||||||||
| 言語 | en | |||||||||
| タイトル | ||||||||||
| タイトル | 軸配位子で酸化物半導体表面に結合した色素を有する色素増感太陽電池の作製とその特性解明 | |||||||||
| 言語 | ja | |||||||||
| 言語 | ||||||||||
| 言語 | eng | |||||||||
| 著者 |
朴, 併煜
× 朴, 併煜
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| 抄録 | ||||||||||
| 内容記述タイプ | Abstract | |||||||||
| 内容記述 | With the increasing world population and standard of life, there is ever increasing demand for more and more energy. Amongst various sources of energy, fossil fuels as oil, coal, natural-gas and nuclear energy are the most important sources of energy. However, these major energy sources have limited supply for fulfilling the demand of modern and future society and industries. Renewable energies use energy sources that are continuously being replenished by nature and are being considered as “clean” or “green” having least environmental impact. We are using them much more rapidly than they are being created and their burning results in to increased greenhouse emission leading to the global warming. Sun is main source of life on the surface of the earth with its total energy capacity of 120,000 TWh, which dwarfs all other energy sources. The sun could be a singular solution to all our future energy needs provided that a suitable, cheap and sustainable technology could be realized for the efficient solar energy harvesting. Amongst various kind of solar cells, certified efficiency of 10.9 % for dye sensitized solar cells (DSSCs) with an active area larger than 1 cm^2 which is almost similar to amorphous Si solar cell has already been reported. Since efficiency of crystalline Si solar cells (25 %), is higher than those of DSSCs, enhancing their efficiencies are highly desired. The lower efficiency of DSSCs is mainly attributed to its lower photon harvesting window (400-800 nm) as compared to that of Si solar cells (500-1100 nm). Since covering the wide wavelength region by a single dye is not so easy, utilization of two or more dyes in the hybrid or tandem DSSC architecture have a potential to solve the problem. Tandem DSSCs are advantageous over hybrid DSSCs in order to circumvent the problem of inter-dye unfavorable interactions. It will be interesting to fabricate tandem DSSCs consisting of a TiO_2-based top electrode and a SnO_2-based bottom electrode having the photon harvesting in the wide wavelength region. Since the conduction band of SnO_2 is about 0.5 eV lower than that of TiO_2, it is possible to use dyes absorbing up to 1400 nm. Our final goal is to find suitable NIR dyes and anchoring systems for SnO_2 to fabricate efficient tandem DSSCs. Chapter 1 deals with the motivation, renewable energy, photovoltaics and the purpose of the present research work. Chapter 2 reviews the theoretical background for understanding the experimental results. Chapter 3 summarizes the experimental tools that are used throughout this work as well as the main advances that have been implemented to the existing pump-probe spectroscopy for the detailed insight about electron injection and recombination dynamics. Sensitizing dyes anchored on nanoporous metal oxide surface via suitable anchoring group (-COOH) play a pivotal role in the photon harvesting. Macrocyclic dyes are one of the strong candidates amongst the sensitizers owing to their high stability and molar extinction coefficients having ability of light absorption from the far-red to infra-red wavelength region. Introduction of suitable anchoring group at the right position of macrocyclic rings where, electron injections occur along with the maintenance of energetic cascade with metal oxide and redox electrolyte is also a cumbersome job. In the chapter 4, it was proved that axially anchored phthalocyanines (model compounds) bonded to SnO_2 nanoparticle surfaces with short metal-O-metal linkage and inject electrons from dyes to SnO_2 layers spatially. In this chapter investigations pertaining to the utilization phthalocyanine based dyes for DSSC fabrication through axial ligation have been systematically conducted. Differential behavior of photon harvesting by such dyes upon adsorption on to the nanoporous TiO_2 and SnO_2 electrodes was investigated using transition absorption spectroscopy. In chapter 5, efforts have been made to investigate the influence of extension of π-conjugation in the macrocyclic ligands on the light absorption and photon harvesting utilizing metal complexed macrocyclic dyes. Electronic absorption spectra of various macrocyclic dyes in solution as well as ligated axially on metal oxide surface have been measured. The energy Eg of these dyes has been found to be varying depending on the nature of macrocyclic ligands under investigation. Moreover, these dyes could successfully adsorb on mesoscopic SnO_2 thin film without aggregation since the Q-band peaks of adsorbed dyes were nearly similar to that observed in the dye solutions without any hypsochromic shift. The amount of adsorbed PcSnCl_2 dye on mesoscopic SnO_2 surfaces has been estimated to be about 2~3 times higher than that of NcSnCl_2(t-Bu). To estimate the extent of adsorbed NcSn(t-Bu) dye onto SnO_2 nanoparticles quantitatively, Langmuir adsorption isotherm was measured. The chapter 6 deals with the fabrication of novel hybrid DSCs involving linearly linked two dyes where one of the dyes (NcSn) was axially anchored on the nanoporous metal oxide surface by a metal-O-metal linkage while the other dye (Ruthenium dye, N719) was bonded to the NcSn by a classical ester linkage. The photo-action spectra of the hybrid DSC in this novel device architecture suggested that electrons are injected from both of the N719 and NcSn to SnO_2 nanoparticles. To understand interfacial charge transfer, the ultrafast photoexcited electron dynamics was investigated using transient absorption (TA) and an improved transient grating (TG) techniques. By comparing the TA and TG kinetics of NcSn, N719, and hybrid NcSn-N719 molecules adsorbed onto both of the SnO_2 and ZrO_2 nanocrystalline films, the kinetics of forward and backward electron transfer dynamics were clarified which led to the conclusion that there are two pathways for electron injection from the linearly-linked two dye molecules (NcSn-N719) to SnO_2. In the last chapter logical discussions have been made pertaining to the future prospects for the continuation of this research. | |||||||||
| 目次 | ||||||||||
| 内容記述タイプ | TableOfContents | |||||||||
| 内容記述 | 1. Introduction||2. Dye-sensitized solar cells||3. Experiment and Measurements||4. DSSCs fabricated with phthalocyanine dyes anchored axially with the metal oxide nanoparticles||5. Fabrication of DSSCs based on axially anchored macrocyclic dyes with extended NIR light harvesting||6. DSSCs based on two molecules structure via axially anchored macrocyclic dye onto metal oxide surface||7. Conclusion and future outlook | |||||||||
| 備考 | ||||||||||
| 内容記述タイプ | Other | |||||||||
| 内容記述 | 九州工業大学博士学位論文 学位記番号:生工博甲第174号 学位授与年月日:平成24年3月23日 | |||||||||
| キーワード | ||||||||||
| 主題Scheme | Other | |||||||||
| 主題 | Axially Anchored | |||||||||
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| 主題Scheme | Other | |||||||||
| 主題 | Macrocyclic Dyes | |||||||||
| キーワード | ||||||||||
| 主題Scheme | Other | |||||||||
| 主題 | DSSC | |||||||||
| キーワード | ||||||||||
| 主題Scheme | Other | |||||||||
| 主題 | Phthalocyanine | |||||||||
| キーワード | ||||||||||
| 主題Scheme | Other | |||||||||
| 主題 | Napahthalocyanine | |||||||||
| アドバイザー | ||||||||||
| 早瀬, 修二 | ||||||||||
| 学位授与番号 | ||||||||||
| 学位授与番号 | 甲第174号 | |||||||||
| 学位名 | ||||||||||
| 学位名 | 博士（工学） | |||||||||
| 学位授与年月日 | ||||||||||
| 学位授与年月日 | 2012-03-23 | |||||||||
| 学位授与機関 | ||||||||||
| 学位授与機関識別子Scheme | kakenhi | |||||||||
| 学位授与機関識別子 | 17104 | |||||||||
| 学位授与機関名 | 九州工業大学 | |||||||||
| 学位授与年度 | ||||||||||
| 内容記述タイプ | Other | |||||||||
| 内容記述 | 平成23年度 | |||||||||
| 出版タイプ | ||||||||||
| 出版タイプ | VoR | |||||||||
| 出版タイプResource | http://purl.org/coar/version/c_970fb48d4fbd8a85 | |||||||||
| アクセス権 | ||||||||||
| アクセス権 | open access | |||||||||
| アクセス権URI | http://purl.org/coar/access_right/c_abf2 | |||||||||
| ID登録 | ||||||||||
| ID登録 | 10.18997/00003769 | |||||||||
| ID登録タイプ | JaLC | |||||||||
