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研究生： 法漢特
Mahmoud Elsayed Farhat
論文名稱： 有機太陽能電池性能提昇之研究：三種有機小分子，無鹵素溶劑，無毒溶液及多功能添加物之組合
Enhanced Performance of Organic Solar Cells via Various Processing Techniques: Functional Additive, Ternary Approach, Halogen-Free Solvents and Green Solvent Mixtures
指導教授： 朱治偉
Chih-Wei Chu
李志浩
Chih-Hao Lee
口試委員: 林建村
Lin, Jiann-T'suen
李志浩
Chih-Hao Lee
陳錦地
Chen, Chin-Ti
朱治偉
Chih-Wei Chu
陳方中
Fang-Chung Chen
學位類別： 博士
Doctor
系所名稱： 原子科學院 - 工程與系統科學系
Department of Engineering and System Science
論文出版年： 2016
畢業學年度： 104
語文別： 英文
論文頁數： 142
中文關鍵詞： 有機太陽能電池 、無鹵素溶劑 、無毒溶液及 、添加物之組合
外文關鍵詞： nanomorphology, green solvents, eco-freindly solvents
相關次數： 點閱：2  下載：0 
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    • Over the past decade, organic photovoltaics (OPVs) experienced significant development in performance reaching the threshold needed for commercialization [power conversion efficiencies (PCE) ˃10%]. Due to their light weight, flexibility and low cost, OPV technology is highly promising in terms of industrial aspects. Besides, OPVs have the advantage of being able to be fabricated on flexible substrates which facilitate the use of mass production techniques such ink jet printing or various roll-to-roll techniques. All these attractive advantages urged researchers worldwide to address challenges facing OPVs technology commercialization such as achieving high performances, replacing toxic processing solvents and upscaling with low costs. In this thesis, we introduced two main issues discussing processing techniques for high device performances and replacing toxic processing solvents with more eco-friendly counterparts.
    Solvent additive with "dual functionality" has been introduced in small-molecule solar cells with significant enhancement in performance. The first function of this additive was that it controlled the morphology: the addition of 0.1% CP3MS (the additive) was sufficient to improve the film’s crystallinity and morphology. The second function was the spontaneous migration of the CP3MS molecules from the bulk to the interface between the active layer and the Al cathode, forming an ultrathin interlayer that acted as a buffer layer. PCE enhanced from 2.75% for devices without additives to 4.55% for devices containing 0.1% CP3MS.
    As promising approach to widen the light absorption in organic solar cells, "ternary approach" has been introduced as technique to enhance device performance. We combined two small-molecule donors with acceptor to form all-small molecule ternary solar cells. Improvement in device performance mainly attributed to the complementary absorption of the two donors. After addition of the molecular donor as third component to form the ternary blend, the crystallinity and morphology of the active layer were enhanced. This means that the molecular donor in the ternary blend has effective role on both the absorption and the morphology. Devices produced PCE of 6.3% in ternary blend system relative to 4.55% in binary blend system.
    As most of highest OPVs performances achieved using halogenated toxic solvents which are big obstacle toward industrialization and mass production. Replacing these toxic solvents with more eco-friendly solvents is urgent need for the upscaling OPVs. Toluene (Tol), a halogen-free solvent, was employed in the fabrication of molecular solar cells, achieving power conversion efficiency PCE higher than that obtained when using chlorinated counterparts. Halogen-free solvents have been also used for solvent vapor annealing (SVA) to control the morphology. We succeeded to achieve one of the highest PCE in molecular solar cells processed form halogen-free solvents (˃ 7%). The enhancement arose mainly from the improvement in the fill factor, due to morphological tailoring and favorable phase separation. PCE higher than 7% is one of the highest achieved so far when using halogen-free solvents for molecular solar cells processing
    A new green solvent, cyclopentyl methyl ether (CPME), has been also introduced as successful alternative to replace toxic halogenated solvent for efficient molecular solar cells. Tol as co-solvent has been introduced with various amounts in CPME forming different green solvent mixtures. Tol incorporation as a co-solvent with CPME combined with thermal annealing effect led to PCE of greater than 8% which is the highest to date for molecular solar cells processed from green solvent mixtures. Morphology plays the key role in the performance improvement under the effects of co-solvent and thermal annealing.

    Over the past decade, organic photovoltaics (OPVs) experienced significant development in performance reaching the threshold needed for commercialization [power conversion efficiencies (PCE) ˃10%]. Due to their light weight, flexibility and low cost, OPV technology is highly promising in terms of industrial aspects. Besides, OPVs have the advantage of being able to be fabricated on flexible substrates which facilitate the use of mass production techniques such ink jet printing or various roll-to-roll techniques. All these attractive advantages urged researchers worldwide to address challenges facing OPVs technology commercialization such as achieving high performances, replacing toxic processing solvents and upscaling with low costs. In this thesis, we introduced two main issues discussing processing techniques for high device performances and replacing toxic processing solvents with more eco-friendly counterparts.
    Solvent additive with "dual functionality" has been introduced in small-molecule solar cells with significant enhancement in performance. The first function of this additive was that it controlled the morphology: the addition of 0.1% CP3MS (the additive) was sufficient to improve the film’s crystallinity and morphology. The second function was the spontaneous migration of the CP3MS molecules from the bulk to the interface between the active layer and the Al cathode, forming an ultrathin interlayer that acted as a buffer layer. PCE enhanced from 2.75% for devices without additives to 4.55% for devices containing 0.1% CP3MS.
    As promising approach to widen the light absorption in organic solar cells, "ternary approach" has been introduced as technique to enhance device performance. We combined two small-molecule donors with acceptor to form all-small molecule ternary solar cells. Improvement in device performance mainly attributed to the complementary absorption of the two donors. After addition of the molecular donor as third component to form the ternary blend, the crystallinity and morphology of the active layer were enhanced. This means that the molecular donor in the ternary blend has effective role on both the absorption and the morphology. Devices produced PCE of 6.3% in ternary blend system relative to 4.55% in binary blend system.
    As most of highest OPVs performances achieved using halogenated toxic solvents which are big obstacle toward industrialization and mass production. Replacing these toxic solvents with more eco-friendly solvents is urgent need for the upscaling OPVs. Toluene (Tol), a halogen-free solvent, was employed in the fabrication of molecular solar cells, achieving power conversion efficiency PCE higher than that obtained when using chlorinated counterparts. Halogen-free solvents have been also used for solvent vapor annealing (SVA) to control the morphology. We succeeded to achieve one of the highest PCE in molecular solar cells processed form halogen-free solvents (˃ 7%). The enhancement arose mainly from the improvement in the fill factor, due to morphological tailoring and favorable phase separation. PCE higher than 7% is one of the highest achieved so far when using halogen-free solvents for molecular solar cells processing
    A new green solvent, cyclopentyl methyl ether (CPME), has been also introduced as successful alternative to replace toxic halogenated solvent for efficient molecular solar cells. Tol as co-solvent has been introduced with various amounts in CPME forming different green solvent mixtures. Tol incorporation as a co-solvent with CPME combined with thermal annealing effect led to PCE of greater than 8% which is the highest to date for molecular solar cells processed from green solvent mixtures. Morphology plays the key role in the performance improvement under the effects of co-solvent and thermal annealing.

    Acknowledgement .....................................................................................................................iii Abstract .......................................................................................................................................iv Table of content .........................................................................................................................vi List of Tables ................................................................................................................................x List of Figures ..............................................................................................................................xii Chapter 1: General Introduction................................................................................................1 1.1. Why Solar Energy? ...........................................................................................................1 1.2. Brief History of Organic Photovoltaics (OPVs) .............................................................2 1.3. Working Principle of OPVs ..............................................................................................5 1.4. OPVs Device Characteristics ..........................................................................................7 1.4.1. Short circuit current density (Jsc) ..........................................................................7 1.4.2. The open-circuit voltage (Voc) ..............................................................................8 1.4.3. Fill factor (FF) ......................................................................................................8 1.4.4. Power conversion efficiency (PCE; η) .................................................................8 1.5. Small Molecular Donors for OPVs...................................................................................9 1.6. OPVs Device Configurations............................................................................................9 1.7. Approaches to Enhance OPVs Device Performance........................................................10 1.7.1. Thermal Annealing................................................................................................11 1.7.2. Processing Additives.............................................................................................14 1.7.3. Choice of Processing Solvents..............................................................................17 1.7.4. Solvent Vapor Annealing (SVA) .......................................................................18 1.7.5. Co-solvent Effect ...............................................................................................20 1.7.6. Ternary Approach ..............................................................................................21 1.8. Environmentally-Friendly and Green Solvents for OPVs Processing...........................23 1.8.1 Hansen Solubility Parameter (HSP)...................................................................26 1.9. Thesis Organization........................................................................................................28 Chapter 2: Dual-Functional Additive for Efficient Molecular Solar Cells ........................30 2.1. Introduction ....................................................................................................................31 2.2. Experimental ..................................................................................................................33 2.2.1. Materials and Solutions .....................................................................................33 2.2.2. Device Fabrication ............................................................................................34 2.2.3. Characterizations ...............................................................................................34 2.3. Results and Discussion .................................................................................................35 2.3.1. Devices performance ........................................................................................35 2.3.2. UV-Vis Absorbance Spectra and EQEs ............................................................40 2.3.3. Crystallinity, Morphology, and Interfaces .......................................................41 2.4. Conclusion ....................................................................................................................49 Chapter 3: Ternary Approach for Efficient Molecular Solar Cells ..................................51 3.1. Introduction .................................................................................................................52 3.2. Experimental .................................................................................................................54 3.2.1. Materials and Solutions.....................................................................................54 3.2.2. Device fabrication.............................................................................................54 3.2.3. Characterization .............................................................................................55 3.3. Results and discussion ................................................................................................56 3.3.1. Device Performance .......................................................................................56 3.3.2. UV-Vis Absorbance Spectra ..........................................................................63 3.3.3. Photoluminescence Characteristics ................................................................65 3.3.4. Morphology, Carrier Mobility and Crystallinity ............................................67 3.4. Conclusion ..................................................................................................................73 Chapter 4: Halogen-Free Solvents for Efficient Molecular Solar Cells ..........................74 4.1. Introduction.................................................................................................................75 4.2. Experimental ..............................................................................................................78 4.2.1. Materials and Solutions ..................................................................................78 4.2.2. Device fabrication...........................................................................................78 4.2.3. Device characterization ..................................................................................79 4.3. Results and discussion ................................................................................................80 4.3.1. Halogenated Vs. Halogen-free; Device Performance and Morphology .........80 4.3.2. SVA Using Halogen-Free Solvents; Device Performance .............................86 4.3.3. SVA Using Halogen-Free Solvents; UV-Vis Absorbance .............................90 4.3.4. SVA Using Halogen-Free Solvents; AFM .....................................................91 4.3.5. SVA Using Halogen-Free Solvents; Photoluminescence Characteristics......93 4.3.6. SVA Using Halogen-Free Solvents; Morphology and Crystallinity ..............94 4.3.7. SVA Using Halogen-Free Solvents; Carrier Mobilities .................................99 4.3.8. SVA Using Halogen-Free Solvents; Device Stability ...................................101 4.4. Conclusion .................................................................................................................102 Chapter 5: Green Solvent Mixture for Efficient Molecular Solar Cells .........................103 5.1. Introduction .................................................................................................................104 5.2. Experimental ...............................................................................................................107 5.2.1. Materials and Solutions ..................................................................................107 5.2.2. Device fabrication ..........................................................................................108 5.2.3. Device characterization .................................................................................109 5.3. Results and discussion ................................................................................................110 5.3.1. Solvent Mixture Effect ...................................................................................110 5.3.2. Thermal Annealing Effect ..............................................................................121 5.4. Conclusion ..................................................................................................................130 Chapter 6: Conclusions and Perspectives ...........................................................................131 6.1. Conclusions .................................................................................................................131 6.2. Perspectives ................................................................................................................133 References ..............................................................................................................................135 List of Publications ...................................................................................................................141

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