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完整後設資料紀錄
DC 欄位 | 值 | 語言 |
---|---|---|
dc.contributor.advisor | 何國川 | zh_TW |
dc.contributor.advisor | Kuo-Chuan Ho | en |
dc.contributor.author | 林芳賢 | zh_TW |
dc.contributor.author | Fang-Sian Lin | en |
dc.date.accessioned | 2023-09-22T16:20:49Z | - |
dc.date.available | 2023-11-09 | - |
dc.date.copyright | 2023-09-22 | - |
dc.date.issued | 2023 | - |
dc.date.submitted | 2023-08-09 | - |
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dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/89840 | - |
dc.description.abstract | 本研究涉及多個方面的研究成果,主要集中在染料敏化太陽能電池(DSSCs)領域。首先,研究提出了一系列新型無金屬有機染料,這些染料基於3,3'-二硫代烷基-2,2'-二噻吩(SBT),通過結構改造和使用不同的烷基鏈和共軛噻吩單元,成功抑制了染料的聚集和界面電荷重組,並提高了光電轉換效率(η)。優化的染料與共吸附劑鵝去氧膽酸 (CDCA)結合,在1個太陽光強度下實現了9.46%的高轉換效率。因此,使用該染料和CDCA共吸附劑的DSSC的長期穩定性顯著優於傳統的N719染料。其中,引入了一種新型多功能聚合物離子液體,即聚(氧乙烯)-酰亞胺-2,2,6,6-四甲基-1-哌啶基氧基(POEI-TEMPO),作為准固態DSSCs的添加劑。電解質中的POEI段提供了機械強度,而TEMPO有機自由基則具有良好的氧化還原性能。含有POEI-TEMPO /碘化物電解質的DSSC在1個太陽光強度下表現出9.83%的高效率,室內條件下更達到了令人印象深刻的25.99%。此外,使用POEI-TEMPO作為添加劑的DSSC的長期穩定性非常優秀,表明它在收集周圍光能方面具有實際應用的潛力。此外,探討了以星狀分子3,6-雙(5-(4,4′-雙(3-偶氮丙基)-[1,1′:3′,1′-三聯苯]-5′-基)-噻吩-2-基)-2,5-雙(2-乙基己基)吡咯[3,4-c]吡咯-1,4(2H,5H)-二酮(DPPTPTA)結合電紡法製備的雙金屬銅-鈷磷化物修飾的碳奈米纖維(CuCoP/CNF)進行鉑(Pt)鍍層對電極(CE)的改性。DPPTPTA@CuCoP/CNF修飾的CE在CE/電解質界面上實現了高效的電荷傳遞,低電荷傳遞電阻和良好的電荷分離能力,使得光電轉換效率(η)在1個太陽光強度下達到9.50%,在室內條件下更達到了令人印象深刻的25.44%。改性層的多孔三維奈米纖維結構還確保了長期穩定性,凸顯了其在可再生能源應用中的潛力。最後,探討了有機染料的結構修飾和雙金屬鈷-釩硒化物(CoVSe2)作為DSSCs對電極(CE)的合成。有機染料中引入不同的烷基鏈和共軛噻吩單元抑制了染料聚集和界面電荷再結合。在CE中使用CoVSe2作為活性材料增強了電子傳輸動力學。優化的元件在1個太陽光強度下實現了10.57%的高效率,室內條件下更達到了令人印象深刻的25.89%。該元件還展示出優異的穩定性,在4000小時的測試後保持了大約88%的效率。總結來說,這些研究結果突出了各種修飾、材料和添加劑對於不同照明條件下提高DSSCs效率、穩定性和光收集能力的潛力。這些章節的整合提供了對影響DSSC性能的因素的全面了解,並為高效穩定的太陽能電池元件的開發提供了有價值的見解。 | zh_TW |
dc.description.abstract | This study encompasses various research findings primarily focused on the field of dye-sensitized solar cells (DSSCs). Firstly, a series of novel metal-free organic dyes based on 3,3'-disulfanyl-2,2'-bithiophene (SBT) were proposed. By modifying the structure and utilizing different alkyl chains and conjugated thiophene units, the aggregation and interfacial charge recombination of the dyes were successfully suppressed, leading to enhanced photoelectric conversion efficiency (η). The optimized dyes, in combination with the co-adsorbent chenodeoxycholic acid (CDCA), achieved a high conversion efficiency of 9.46% under 1 sun illumination. As a result, DSSCs utilizing this dye and CDCA co-adsorbent exhibited significantly improved long-term stability compared to traditional N719 dyes. Among them, a novel multifunctional polymer ionic liquid, poly(oxyethylene)-imide-2,2,6,6-tetramethyl-1-piperidinyloxyl (POEI-TEMPO), was introduced as Additives for quasi-solid-state DSSCs (QSS-DSSCs). The POEI segment in the electrolyte provided mechanical strength, while the TEMPO organic radical acted as a superior mediator with favorable redox properties. The DSSCs incorporating the POEI-TEMPO/iodide electrolyte exhibited a high efficiency of 9.83% under 1 sun and an impressive 25.99% under indoor conditions. Furthermore, the long-term stability of the DSSC with POEI-TEMPO as an additive was promising, indicating its potential for practical application in harvesting ambient light energy. In addition, the modification of the platinum (Pt) coated counter electrode (CE) was explored using a star-shaped molecule, 3,6-bis(5-(4,4′-bis(3-azidopropyl)-[1,1′:3′,1′-terphenyl]-5′-yl)-thien-2-yl)-2,5-bis(2-ethylhexyl)pyrrolo[3,4-c]pyrrole-1,4(2H,5H)-dione (DPPTPTA), in combination with electrospun bimetallic copper-cobalt phosphide decorated on carbon nanofibers (CuCoP/CNF). The DPPTPTA@CuCoP/CNF modified CE exhibited efficient charge transfer at the CE/electrolyte interface, low charge transfer resistance, and good charge separation ability, resulting in a photoelectric conversion efficiency (η) of 9.50% under 1 sun conditions and an impressive 25.44% under indoor conditions. The porous three-dimensional nanofiber structure of the modified layer also ensured long-term stability, highlighting its potential for renewable energy applications. Finally, explored the structural modification of organic dyes and the synthesis of bimetallic cobalt vanadium diselenide (CoVSe2) for the counter electrode (CE) in DSSCs. The introduction of different alkyl chains and conjugated thiophene units in the organic dyes suppressed significant dye aggregation and interfacial charge recombination. The use of CoVSe2 as an active material in the CE enhanced the electron transport dynamics. The optimized device achieved a high efficiency of 10.57% under 1 sun conditions and an impressive 25.89% under indoor conditions. The device also demonstrated excellent stability, retaining approximately 88% of its efficiency after 4000 h of testing. Overall, these findings highlight the potential of various modifications, materials, and additives for enhancing the efficiency, stability, and light-harvesting capabilities of DSSCs in different lighting conditions. The integration of these chapters provides a comprehensive understanding of the factors influencing DSSC performance and offers valuable insights for the development of efficient and stable solar cell devices. | en |
dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2023-09-22T16:20:49Z No. of bitstreams: 0 | en |
dc.description.provenance | Made available in DSpace on 2023-09-22T16:20:49Z (GMT). No. of bitstreams: 0 | en |
dc.description.tableofcontents | Acknowledgements I
中文摘要 III Abstract V Table of Contents VII List of Tables XI List of Figures XIII List of Schemes XXI Nomenclatures XXII Chapter 1 Introduction 1 1-1 Basic background and working principle of DSSCs 1 1-2 Organic dyes application 6 1-3 Multifunctional polymer ionic liquid electrolyte 7 1-4 Multifunctional conjugated molecules and transition metal compounds 11 1-5 Organic dyes and transition metal compounds 16 1-6 Research motivation and design 20 Chapter 2 Metal free efficient dye sensitized solar cells based on thioalkylated bithiophenyl organic dyes 25 2-1 Abstract of Chapter 2 25 2-2 Experimental Section 26 2-2-1 Design of SBT dyes 26 2-2-2 Synthesis and material description 27 2-2-3 Characterization 27 2-2-4 General procedure for Stille cross-coupling reactions of (9a-e) 27 2-2-5 General procedure for 10a-e 28 2-2-6 General procedure for final target compounds 1-5 29 2-2-7 Cell assembly description 29 2-3 Results and Discussion 30 2-3-1 Optical and electrochemical characterization 30 2-3-2 Molecular orbital computations and crystal structure 32 2-3-3 Photovoltaic properties 34 2-3-4 Photovoltaic performance at different illumination powers 42 2-3-5 Long-term stability of different dyes 44 2-4 Summary of Chapter 2 45 2-5 Supporting information of Chapter 2 46 Chapter 3 A novel multifunctional polymer ionic liquid as an additive in iodide electrolyte combined with silver-mirror coating counter electrodes for quasi-solid-state dye-sensitized solar cells 64 3-1 Abstract of Chapter 3 64 3-2 Experimental section 65 3-2-1 Materials 65 3-2-2 Synthesis of POEI-TEMPO polymer 67 3-2-3 Preparation of POEI-TEMPO-based gel type electrolytes 67 3-2-4 Fabrication of PtCE/SMC electrode 68 3-2-5 Cell assembly 69 3-3 Results and discussions 70 3-3-1 Characterization of POEI-TEMPO 70 3-3-2 Electrochemical properties of gel type POEI-TEMPO-based electrolytes 73 3-3-3 Charge transfer properties of gel type POEI-TEMPO-based electrolytes in DSSCs 79 3-3-4 Photovoltaic performance of gel type POEI-TEMPO-based electrolytes in DSSCs 83 3-3-4-1 Cell performance with the gel type POEI-TEMPO-based electrolytes and liquid type iodide electrolytes 83 3-3-4-2 Variation in VOC of DSSCs with POEI-TEMPO-based gel type electrolytes 85 3-3-4-3 Variation in JSC for DSSCs with POEI-TEMPO-based gel type electrolytes 86 3-3-4-4 Variation in FF of DSSCs with POEI-TEMPO-based gel type electrolytes 88 3-4 Photovoltaic performance of DSSCs containing POEI-TEMPO-based gel type electrolytes under indoor-light conditions 89 3-5 Long-term stability of DSSCs containing POEI-TEMPO-based gel type electrolytes 92 3-6 Summary of Chapter 3 94 3-7 Supporting information of Chapter 3 95 Chapter 4 Multifunctional conjugated molecules combined with electrospun CuCoP/carbon nanofibers as a modifier of Pt counter electrode for dye-sensitized solar cells 100 4-1 Abstract of Chapter 4 100 4-2 Experimental section 101 4-2-1 Synthesis of DPPTPTA conjugated small molecule 101 4-2-2 Synthesis of CuCoP/CNF 104 4-2-3 Preparation of DPPTPTA@CuCoP/CNF modified layer coated PtCE 104 4-3 Results and discussion 105 4-3-1 Characterization of DPPTPTA conjugated molecules 105 4-3-2 Characterization of DPPTPTA@CuCoP/CNF composite 105 4-3-3 Electrochemical properties of DSSCs with DPPTPTA@CuCoP/CNF modified layer 115 4-3-4 Interfacial properties of DSSCs based on DPPTPTA@CuCoP/CNF modified layer 119 4-3-5 Photovoltaic properties of DSSCs with DPPTPTA@CuCoP/CNF modified layer 122 4-3-6 Long-term stability of DSSCs with DPPTPTA@CuCoP/CNF modified layer 128 4-4 Summary of Chapter 4 129 4-5 Supporting information of Chapter 4 130 Chapter 5 Alkyl (R)- and thioalkyl (SR)-substituted terthiophene (tT)-based organic dyes combined with hollow sphere-structured bimetallic cobalt vanadium selenide counter electrode for dye-sensitized solar cells 139 5-1 Abstract of Chapter 5 139 5-2 Experimental section 140 5-2-1 Synthesis of alkyl (R)- and thioalkyl (SR)-substituted terthiophene (tT)-based organic dyes 140 5-2-2 Synthesis of CoVSe2 hollow sphere structure 142 5-2-3 Integrating organic dyes with CoVSe2 modified counter electrode as optimized devices 142 5-3 Results and discussion 143 5-3-1 Characterization of organic dyes 143 5-3-2 Characterization of CoVSe2 composite 145 5-3-3 Photovoltaic performances of DTDRT/DTDST+CoVSe2-500 CE 151 5-3-4 Electrochemical properties 156 5-3-5 Density functional theory calculations 160 5-3-6 Long-term stability 166 5-4 Summary of Chapter 5 167 5-5 Supporting information of Chapter 5 168 Chapter 6 Conclusions and suggestions 197 6-1 Conclusions 197 6-2 Suggestions 199 References 201 Curriculum vitae 220 | - |
dc.language.iso | en | - |
dc.title | 探索多功能有機分子與多過渡金屬化合物應用於染料敏化太陽能電池 | zh_TW |
dc.title | Exploring Multifunctional Organic Molecules and Multitransitional Metal Compounds for Dye-sensitized Solar Cells | en |
dc.type | Thesis | - |
dc.date.schoolyear | 111-2 | - |
dc.description.degree | 博士 | - |
dc.contributor.coadvisor | 鄭如忠 | zh_TW |
dc.contributor.coadvisor | Ru-Jong Jeng | en |
dc.contributor.oralexamcommittee | 戴子安;陳銘洲;江志強 | zh_TW |
dc.contributor.oralexamcommittee | Chi-An Dai;Ming-Chou Chen;Jyh-Chiang Jiang | en |
dc.subject.keyword | 染料敏化太陽能電池,有機染料,聚合物離子液體,准固態電解質,共軛聚合物,過渡金屬化合物,可再生能源, | zh_TW |
dc.subject.keyword | Dye-sensitized solar cells (DSSCs),organic dye,polymer ionic liquid,quasi-solid-state electrolyte,conjugated polymer,transition metal compound,renewable energy, | en |
dc.relation.page | 225 | - |
dc.identifier.doi | 10.6342/NTU202303818 | - |
dc.rights.note | 未授權 | - |
dc.date.accepted | 2023-08-11 | - |
dc.contributor.author-college | 工學院 | - |
dc.contributor.author-dept | 高分子科學與工程學研究所 | - |
顯示於系所單位: | 高分子科學與工程學研究所 |
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