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http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/92432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 | 游鑫福 | zh_TW |
| dc.contributor.author | Hsin-Fu Yu | en |
| dc.date.accessioned | 2024-03-22T16:28:52Z | - |
| dc.date.available | 2024-03-23 | - |
| dc.date.copyright | 2024-03-22 | - |
| dc.date.issued | 2024 | - |
| dc.date.submitted | 2024-01-24 | - |
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| dc.identifier.uri | http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/92432 | - |
| dc.description.abstract | 紫精表現出顯著的顏色對比度和有益的電致色變性能，儘管紫精以其高顏色對比度而聞名，但聚集現象而導致的循環穩定性不佳仍然存在。本論文以探討紫精的電致色變材料與電致色變元件(electrochromic device, ECD)之特性，提升其光學特性和改善長期穩定性為目的之研究。因此，本論文開發兩種新型紫精電致色變元件，並研究其電致色變性能，包括高分子離子液體(polymeric ionic liquid, PIL)和紫精衍生物。高分子離子液體以不同比例的離子液體(BMIMBF4)和高分子(POE和PVdF‒HFP)混合或合成，並通過靜電紡絲技術製備奈米纖維薄膜作為紫精電致色變元件的助電解質。另一方面，紫精衍生物(TFMBzV、DTFMBzV、TFMPV和HOPV)是選取拉電子基團(CF3)和推電子基團(OC6H13)之不同取代基合成。
首先，為了提高紫精電致色變元件的長期穩定性，並研究助電解質對電致色變性能的影響，合成新型PIL並製備奈米纖維薄膜應用於電致色變元件中。此新型PIL以高分子PVdF‒HFP作為主鏈，在其主鏈上接枝BMIMBF4，使其對紫精離子之間產生分子相互作用，進而顯著減少衰退以實現長期穩定性。其次，為了研究紫精兩側之取代基對其電化學性質和光學性質的影響，選取兩個極端的取代基，即拉電子基團和推電子基團進行研究。在本論文的研究和討論中，成功地提出一個使用PFI‒BF4_1.5薄膜作為半固態電解質的PV/Fc ECD經過10,000圈和50,000圈循環操作後分別具有95.9%和88.3%的保留率，並且具有77.8%的ΔT和371.9 cm2 C‒1的ηe。此外，TFMPV/Fc ECD具有 77.8%的ΔT和371.9 cm2 C‒1的ηe，且通過PFI‒BF4_1薄膜作為半固態電解質引入TFMPV/Fc ECD中，其在10,000圈循環操作後保留率達到97.8%。在許多文獻當中，很少能做到50,000圈以上的循環操作後還能維持極高的穩定性(>80%)，並同時有高的光學對比度(>70%)。 | zh_TW |
| dc.description.abstract | Since the viologen itself demonstrate significant color contrast and beneficial electrochromic performance. Even though the viologens were well‒known for their high color contrast, their lack of cycling stability resulting from aggregation or aging process remains. In this dissertation, viologen‒based electrochromic devices (ECDs) were studied for the enhancement of optical properties and improvement of long‒term stability. Therefore, the electrochromic (EC) performance of two novel viologen‒based ECDs, including polymeric ionic liquid (PIL) and viologen derivatives, was investigated. The PIL was utilized through different ratios of the ionic liquid (BMIMBF4) and the polymer (POE and PVdF‒HFP) to form a nanofiber membrane by the electrospinning and be a supporting electrolyte in the viologen‒based ECDs. The viologen derivatives (TFMBzV, DTFMBzV, TFMPV, and HOPV) were synthesized with different substituents like the electron‒withdrawing group (CF3) and the electron‒donating group (OC6H13).
Firstly, to improve the long‒term stability of the viologen‒based ECDs, and study the influence of the electrolyte on EC performance, a novel PIL was synthesized and formed a nanofiber membrane to utilize in an ECD. The novel PIL, using polymeric PVdF‒HFP as the main chain, was grafted with BMIMBF4 on the main chain to arouse the molecular interaction with the viologen ions, thereby significantly reducing recession for long‒term stability. Secondly, to study the influence of the substituent on both sides of viologen for its electrochemical properties and optical properties, thus, chosen two extreme substituents, an electron‒withdrawing group, and an electron‒donating group, were investigated. In the research and discussion in this thesis, we have successfully proposed the PV/Fc ECD with PFI‒BF4_1.5 membrane performs high retention of 95.9% and 88.3% after 10,000 and 50,000 cycles, respectively, and exhibits a 77.8% of ΔT and 371.9 cm2 C‒1 of ηe. In Addition, the proposed TFMPV/Fc ECD performed a high ΔT of 77.8% and a high ηe of 371.9 cm2 C‒1, and the retention was achieved at 97.8% after 10,000 cycles by the improvement of the PFI‒BF4_1 introduced in the ECD. It is noteworthy that few literatures achieve such high stability (>80%) after more than 50,000 cycles, while maintaining high optical contrast (>70%) simultaneously. | en |
| dc.description.provenance | Submitted by admin ntu (admin@lib.ntu.edu.tw) on 2024-03-22T16:28:52Z No. of bitstreams: 0 | en |
| dc.description.provenance | Made available in DSpace on 2024-03-22T16:28:52Z (GMT). No. of bitstreams: 0 | en |
| dc.description.tableofcontents | 論文口試委員審定書 I
ACKNOWLEDGEMENTS II 中文摘要 IV ABSTRACT V CONTENTS VII LIST OF FIGURES XII LIST OF TABLES XX LIST OF SCHEMES XXII NOMENCLATURES XXIII CHAPTER 1 INTRODUCTION 1 1.1 ELECTROCHROMISM 1 1.1.1 Optical contrast 3 1.1.2 Response time 4 1.1.3 Coloration efficiency 5 1.1.4 Cycling stability 6 1.1.5 Application 6 1.1.6 Electrochromic devices 9 1.2 VIOLOGEN 17 1.2.1 Viologen synthesis 18 1.2.2 Viologen properties 23 1.2.3 Electrolyte in the viologen system 26 1.2.4 Substituents for viologens 28 1.3 SCOPE OF THIS THESIS 29 CHAPTER 2 EXPERIMENTAL 36 2.1 MATERIALS 36 2.2 GENERAL EXPERIMENTAL FOR MATERIALS SYNTHESIS 38 2.3 GENERAL EXPERIMENTAL FOR ELECTROCHEMICAL/SPECTRA‒ELECTROCHEMICAL METHODS 38 2.4 GENERAL EXPERIMENTAL FOR MATERIAL CHARACTERIZATIONS 41 2.5 EXPERIMENTAL OF THE POLYMERIC IONIC LIQUIDS (PILS) AND THE VIOLOGEN DERIVATIVES 42 2.5.1 Experimental of the composite membranes based on POEI‒IBF4 and PVdF‒HFP 43 2.5.2 Synthesis and Experimental of the PFI‒based PIL membranes 44 2.5.3 Synthesis of the viologen derivatives 50 2.6 ASSEMBLY OF ECDS 57 CHAPTER 3 ELECTROSPUN NANOFIBERS COMPOSED OF POLY(VINYLIDENE FLUORIDE‒CO‒HEXAFLUOROPROPYLENE) AND POLY(OXYETHYLENE)‒IMIDE IMIDAZOLIUM TETRAFLUOROBORATE AS ELECTROLYTES FOR SOLID‒STATE ELECTROCHROMIC DEVICES 59 3.1 INTRODUCTION 59 3.2 RESULTS AND DISCUSSION 61 3.2.1 Characterization of the nanofibers 61 3.2.2 Working principle of the solid‒state ECD with N15Py 68 3.2.3 Performance of the quasi‒solid‒state ECD with N15P10 membrane (N15P10‒ECD) 75 3.3 CONCLUSION 83 CHAPTER 4 STABLE VIOLOGEN‒BASED ELECTROCHROMIC DEVICES: CONTROL OF COULOMBIC INTERACTION USING MULTI‒FUNCTIONAL POLYMERIC IONIC LIQUID MEMBRANES 85 4.1 INTRODUCTION 85 4.2 RESULTS AND DISCUSSION 90 4.2.1 Characterization of the PFI‒based PILs and membranes. 90 4.2.2 Electrochromic performance of the PFI‒based ECDs. 98 4.2.3 Charge transfer in the PFI‒based ECDs. 107 4.2.4 Cyclic voltammetry for the PFI‒based ECDs. 109 4.2.5 Long‒term optical stability of the PFI‒based ECDs. 112 4.3 CONCLUSION 115 CHAPTER 5 EFFECT OF TRIFLUOROMETHYL SUBSTITUENTS IN BENZYL‒BASED VIOLOGEN ON THE ELECTROCHROMIC PERFORMANCE: OPTICAL CONTRAST AND STABILITY 117 5.1 INTRODUCTION 117 5.2 RESULTS AND DISCUSSION 120 5.2.1 Electrochemical performance of benzyl‒based viologens 120 5.2.2 Electrochromic characterization of benzyl‒based viologen ECDs 135 5.2.3 Long‒term stabilities of benzyl‒based viologen ECDs 143 5.3 CONCLUSIONS 150 CHAPTER 6 EFFECT OF THE ELECTRON‒WITHDRAWING AND ELECTRON‒DONATING N‒SUBSTITUENTS FOR THE PHENYL VIOLOGEN‒BASED ELECTROCHROMIC DEVICES 151 6.1 INTRODUCTION 151 6.2 RESULTS AND DISCUSSION 154 6.2.1 Electrochemical performance of viologen derivatives (PV, HOPV, TFMPV) 154 6.2.2 Electrochromic characterization of phenyl‒based viologen ECDs 164 6.2.3 Effects of substitution on phenyl‒based viologen properties 171 6.2.4 The long‒term performance of phenyl‒based viologen ECDs 175 6.3 CONCLUSIONS 182 CHAPTER 7 CONCLUSIONS AND SUGGESTIONS 183 7.1 CONCLUSIONS 183 7.2 SUGGESTIONS 184 REFERENCE 186 APPENDIX A 227 | - |
| dc.language.iso | en | - |
| dc.subject | 半固態電解質 | zh_TW |
| dc.subject | 取代基 | zh_TW |
| dc.subject | 靜電紡絲技術 | zh_TW |
| dc.subject | 電致色變元件 | zh_TW |
| dc.subject | 紫精 | zh_TW |
| dc.subject | 高分子離子液體 | zh_TW |
| dc.subject | Viologen | en |
| dc.subject | Electrochromic devices | en |
| dc.subject | Electrospinning | en |
| dc.subject | Polymeric ionic liquid | en |
| dc.subject | Quasi‒solid‒state electrolyte | en |
| dc.subject | Substituents | en |
| dc.title | 紫精電致色變材料與元件之研究 | zh_TW |
| dc.title | Study for Viologen-based Electrochromic Materials and Devices | en |
| dc.type | Thesis | - |
| dc.date.schoolyear | 112-1 | - |
| dc.description.degree | 博士 | - |
| dc.contributor.oralexamcommittee | 廖英志;戴子安;林正嵐;李君婷 | zh_TW |
| dc.contributor.oralexamcommittee | Ying-Chih Liao;Chi-An Dai;Cheng-Lan Lin;Chun-Ting Li | en |
| dc.subject.keyword | 電致色變元件,靜電紡絲技術,高分子離子液體,半固態電解質,取代基,紫精, | zh_TW |
| dc.subject.keyword | Electrochromic devices,Electrospinning,Polymeric ionic liquid,Quasi‒solid‒state electrolyte,Substituents,Viologen, | en |
| dc.relation.page | 232 | - |
| dc.identifier.doi | 10.6342/NTU202400170 | - |
| dc.rights.note | 同意授權(限校園內公開) | - |
| dc.date.accepted | 2024-01-25 | - |
| dc.contributor.author-college | 工學院 | - |
| dc.contributor.author-dept | 化學工程學系 | - |
| dc.date.embargo-lift | 2029-01-22 | - |
| 顯示於系所單位： | 化學工程學系 | |
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