開發高穿透度聚苯胺/還原氧化石墨烯奈米複合對電極及設計最適化電解液配比實現具高光著色效率之光驅動電致色變元件

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研究生：	姜羽柔 Yu-Jou Chiang
論文名稱：	開發高穿透度聚苯胺/還原氧化石墨烯奈米複合對電極及設計最適化電解液配比實現具高光著色效率之光驅動電致色變元件 Developing Highly Transparent PANI/rGO Nanocomposite Counter Electrode and Designing Optimized Electrolyte Composition to Achieve High Photocoloration Efficiency Photoelectrochromic Devices
指導教授：	葉旻鑫 Min-Hsin Yeh
口試委員:	江志強 Jyh-Chiang Jiang 何國川 Kuo-Chuan Ho
學位類別：	碩士 Master
系所名稱：	工程學院 - 化學工程系 Department of Chemical Engineering
論文出版年：	2021
畢業學年度：	109
語文別：	英文
論文頁數：	121
中文關鍵詞：	染料敏化太陽能電池、電致色變元件、快速響應時間、高透光電催化材料、光驅動電致色變元件、光著色效率、聚苯胺、還原氧化石墨烯、自供電系統、智慧節能窗
外文關鍵詞：	Ｄye-sensitized solar cells, electrochromic device, fast response, highly transparent electrocatalytic layer, photoelectrochromic device, photocoloration efficiency, polyaniline, reduced graphene oxide, self-powered system, smart window
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光驅動電致色變元件(Photoelectrochromic devices, PECDs)為結合染料敏化太陽能電池(Dye-sensitized solar cells, DSSCs)與電致色變元件(Electrochromic devices, ECDs)的一種光電化學系統，讓此種元件兼具了DSSC轉換光能為電能的能力以及ECD通電產生氧化還原使其薄膜變色特性，使其在接收光能轉換成電能的同時，能直接驅動氧化還原反應進而產生光學響應的自供電智慧節能窗(Self-powered smart window)，從而達到節約能源並實現永續綠色建築的終極目標。然而，現今PECDs受限於光陽極穿透度、電致色變材料選擇、電解質組成以及電催化材料選擇上差異的緣故，因此無法達到如同ECDs的高光學對比與快速響應時間進而阻礙PECDs的可行性以及商業化的可能性。為了解決上述議題，本論文首先將從電催化材料的設計著手，開發一種兼具高光學穿透度與電催化能力之PANI/rGO複合電催化材料導入PECD中；此外，本論文並進一步探討並優化電解液添加劑與氧化還原對濃度以提高整體元件的光電轉換效率進而實現具高光著色效率的PECD。
一般而言，對於良好電催化Pt經常在PECD中作為對電極上的電催化材料來還原電解質中的I3-。然而，由於低透光度的Pt對電極將導致其PECD的整體光學對比度將受到限制。有鑑於此，在本論文第四章研究中將設計一種兼具有高光學穿透度以及優異電催化性能的PANI/rGO複合電催化材料來取代Pt並進一步提高PECD整體光學效能。由於成本相對低廉且可加工性高的PANI本身已具有催化I3-還原能力，為了使PANI電極在維持良好穿透度的前提下進一步增強其電催化能力，具有高透明度與良好的導電性的rGO將透過電聚合製程中一併將導入修飾PANI電極，期望能進一步使得PECD擁有更好的光學表現。在最適化rGO含量以及薄膜厚度後，由PANI/rGO對電極所組成的PECD具有比Pt對電極所組成的PECD更為出色的光學表現，其響應時間不僅可與搭配Pt對電極所組成的PECD相當，其光學對比度 (ΔT=26.8%)更顯著高於使用Pt對電極的PECD (ΔT=9.4 %)，顯示兼具高光學透度與電催化能力的PANI/rGO複合電催化薄膜具有取代傳統Pt並進一步應用於PECD對電極的潛力。
為了更進一步提升PECD的光著色效率，本論文第五章研究中將探討電解液中的添加劑以及氧化還原對濃度進而開發出最適化電解液配比來提升PECD的整體元件效能。從研究結果中可發現移除的電解液中I2能有效提高PECD的光電轉換效率 (Photoelectric conversion efficiency, η) 以及光著色效率 (Photocoloration efficiency, PhCE) 中，顯示傳統電解液中I2對於PECD中的光伏單元或是電致色變單元皆並無正向助益。此外，透過導入常用於DSSC中的電解質添加劑TBP於電解質研究中可發現隨著電解液中的TBP含量的增加，通過電化學阻抗譜 (Electrochemical impedance spectroscopy, EIS) 與暗電流量測，證明了光陽極電子再結合阻力增加以及TiO2費米能階的負移，顯示TBP的導入將能提高PECD的開環電位(Open-circuit voltage, VOC)並將有利於PECD於開路照光條件下的著色程度。透過最適化電解液組成並進一步導入PECD中，其VOC不僅從-0.56提升到-0.76 V且JSC幾乎不受影響，相對應的光學對比度更比原先顯著提升了40.7%且能夠同時具有出色的響應時間。結果顯示，透過最適化電解質組成與配比將能大幅提高PECD整體元件的光伏性能以及光著色效率。
綜上所述，只要透過尋求可能的補救方案將PECD中觀察到的不利現象降低，高光學對比度PECD的發展是觸手可及的。這項研究展示了一種自供電的高性能PECD，其特點不僅是具有相對較高的光電轉換效率，在光學表現上更展現出了快速的切換響應時間以及顯著的光學對比。隨著環境問題與綠能技術所受到的日益重視，此高性能的PECD光電化學系統的提出拓寬了未來應用多樣化的可能性。

The photoelectrochromic devices (PECDs) were composed of electrochromic devices (ECDs) and dye-sensitized solar cells (DSSCs), which were categorized as a classic type of self-powered systems. Among various types of self-powered systems, the solar-driven self-powered systems of PECDs seems to be the practical platform by simply combining the photovoltaic unit and electrochromic device since photo-energy can be easily harvested from solar or indoor light and then employed to trigger the coloring/bleaching reaction during the charging/discharging process. However, the low optical contrast (ΔT) and the sluggish response of PECD retarded the progress of practical development. To resolve these bottlenecks, a highly transparent polyaniline/reduced graphene oxide (PANI/rGO) nanocomposite with outstanding electrocatalytic performance is designed as a counter electrode (CE) for PECD. Moreover, after understanding the role of additive and optimizing the concentration of redox couple in the electrolyte, the PECD with outstanding photocoloration efficiency (PhCE) can be achieved by improving its photoelectric conversion efficiency (η).
Conventionally, Pt was used as an electrocatalyst to reduce the I3- of electrolyte in PECD. However, the optical contrast of PECD with Pt-based CE was restricted by an intrinsic feature of opaque Pt. In view of this problem, in Chapter 4 of this thesis, a PANI/rGO nanocomposite electrocatalytic material with high optical transmittance and good electrocatalytic performance is designed to replace Pt CE for further improving the optical performance of corresponding PECD. Based on the advantages of low cost and promising electrocatalytic activity of PANI, highly transparent and remarkable conductive rGO was introduced to further boosting up its electrochemical performance. After systematically optimizing the film thickness and composition of PANI/rGO nanocomposite, the PECD with PANI/rGO based CE possesses better optical contrast (ΔT=26.8%) than that with Pt-based CE (ΔT=9.4%), which clearly revealed that PANI/rGO nanocomposites with high optical transparency and electrocatalytic ability has the great potential to replace traditional Pt CE in PECDs.
To further improve the photocoloration efficiency of PECD, in Chapter 5 of this thesis, the additive and redox couple concentration in the electrolyte for PECD will be systematically studied and then optimized to improve the overall performance of PECD. Accorrding to research results, it can be found that the I2-free electrolyte could effectively improve the photoelectric conversion efficiency (η) and the photocoloration efficiency (PhCE) at the same time, indicates that the removal ) and the photocoloration efficiency (PhCE) at the same time, indicates that the removal of I2 in the electrolyte is beneficial for boosting up both of photovoltaic unit and electrochromic unit. By introducing 4-tert-butylpyridine (TBP), a common additive in the electrolyte for inhibiting the recombination reaction on photoanode in DSSC, the recombination resistance between TiO2 and the electrolyte increases and the Fermi level of TiO2 gradually negative shifted by increasing the concentration of TBP, which would facilitate coloration process under illumination with open-circuit condition. By optimizing the composition of the electrolyte, the open-circuit voltage (VOC) of corresponding PECD was not only increased from -0.56 to -0.76 V with similar short-circuit current density (JSC), but also significantly improved the corresponding optical contrast by 40.7% with a similar response time. The results revealed that the improvement of PhCE and η for PECD could be for PECD could be effectively achieved by optimizing the electrolyte composition with additive concentration and redox couple ratio.

中文摘要I
Abstract III
Table of Contents V
List of Tables VIII
List of Figures IX
Nomenclature XIV
Chapter 1 Introduction 1
1 Preface 1
2 Introduction of electrochromism 1
2.1 Development and application of electrochromic technology 2
2.2 Electrochromic materials 4
2.3 Types of electrochromic devices 5
3 Introduction of dye-sensitized solar cells 9
3.1 The background and current development of solar cells 10
3.2 Working mechanism of dye-sensitized solar cells 11
3.3 Types of dye-sensitized solar cells 14
4 Introduction of self-powered system 17
5 Introduction of photoelectrochromic devices 19
5.1 Types of photoelectrochromic devices 21
5.2 The background and current development of photoelectrochromic devices 22
Chapter 2 Literature Review and Research Scope 25
1 Impact of Composition on the Performance of Photoelectrochromic Devices 25
1.1 The effect of electrolytes on photoelectrochromic devices 25
1.2 The effect of counter electrodes on photoelectrochromic devices 28
2 Development of Bifacial Dye-sensitized Solar Cell 29
3 Motivation of Research 32
Chapter 3 Experimental Procedure 36
1 Experimental Chemicals and Instrument 36
1.1 Experimental and analytical instruments 36
1.2 Electrochemical analysis 37
1.3 Photovoltaic properties for PECDs 40
1.4 Ultraviolet-visible (UV-Vis) spectroscopy 41
1.5 Field emission - scanning electron microscopy (FE-SEM) 42
1.6 Raman spectroscopy 43
2 Experimental Materials 45
3 Experimental Procedure 46
3.1 Fabrication of photoelectrodes 46
3.2 Preparation of PEDOT-MeOH films on photoelectrodes 46
3.3 Preparation of PANI, PANI/rGO films as counter electrodes 47
3.4 Assembly of PECDs 47
4 Experimental Setup 47
4.1 UV-Vis spectroscopy analysis of electrochromic film in three-electrode system 47
4.2 UV-Vis spectroscopy analysis of photoelectrochromic device 48
4.3 Measurement of photovoltaic efficiency 49
Chapter 4 Development a highly transparent electropolymerized PANI/rGO nanocomposites as a Pt-free electrocatalytic layer in photoelectrochromic device 51
1 Motivation and Conceptual Design 51
2 Results and Discussion 52
2.1 Electrochemical and optical properties of PEDOT-MeOH film 52
2.2 Optimizing the thickness of PANI films for PECDs 53
2.3 Morphological and structural characterizations of PANI and PANI/rGO films 56
2.4 Optimizing the content of rGO in PANI CEs 58
2.5 The coloration kinetics of PECDs 61
3 Summary 65
Chapter 5 Optimize the molar ratio of I-/I3- and the contents of TBP in the electrolyte to realize both high optical contrast and fast-responsive control photoelectrochromic device 66
1 Motivation and Conceptual Design 66
2 Results and Discussion 67
2.1 Optimizing the concentration of I2 in electrolyte 67
2.2 Effects of I2 concentration on devices 70
2.3 Optimizing the concentration of TBP in electrolyte 71
2.4 Effects of TBP concentration on devices 74
2.5 Effects of excessive TBP on electrolyte and CE 75
3 Summary 77
Chapter 6 Conclusion and Suggestion 80
1 Conclusion 80
2 Suggestions and Prospects 81
Reference 84
Appendix A 101
                                

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全文公開日期 2026/08/31 (校內網路)
全文公開日期 2026/08/31 (校外網路)
全文公開日期 2026/08/31 (國家圖書館：臺灣博碩士論文系統)

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