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  1. NTU Theses and Dissertations Repository
  2. 工學院
  3. 材料科學與工程學系
Please use this identifier to cite or link to this item: http://tdr.lib.ntu.edu.tw/jspui/handle/123456789/80136
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dc.contributor.advisor林金福(King-Fu Lin)
dc.contributor.authorHsin-Hsiang Huangen
dc.contributor.author黃信祥zh_TW
dc.date.accessioned2022-11-23T09:28:08Z-
dc.date.available2021-07-09
dc.date.available2022-11-23T09:28:08Z-
dc.date.copyright2021-07-09
dc.date.issued2021
dc.date.submitted2021-07-02
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dc.identifier.urihttp://tdr.lib.ntu.edu.tw/jspui/handle/123456789/80136-
dc.description.abstract"以有機銨碘化鉛作為光敏材料的鈣鈦礦太陽能電池(Perovskite solar cells, PSCs)具有較高的光電轉換效率和較低的加工成本,因此被認為具有商業化的潛力,但如何提升PSCs的元件使用壽命仍然為目前最重要的研究課題。蒙脫土(Montmorillonite, MMT)是一種天然的近晶粘土,具有多層堆疊的奈米片(厚度約為1 nm,橫向長度約為300 nm),脫層完的MMT (exfoliated MMT, exMMT)就像屏障一樣,可以阻止水分滲透到膜中。除此之外,exMMT還可以通過陽離子交換與有機碘化胺相互作用產生作用力(氫鍵)。本論文發現在鈣鈦礦層旋塗成膜之前,將exMMT參雜進MAPbI3的鈣鈦礦前驅溶液中,可以在鈣鈦礦的晶粒表面上形成一保護殼,使得未封裝的PSCs抗濕能力大幅提升,在相對濕度50%的環境下儲存半年後,效率仍然保持在17.29%以上。值得注意的是,MMT可以在水中溶脹後再利用超聲波的方式來達到脫層的效果,其方法簡單且成本低廉,整個脫層過程也受到Derjaguin-Landau-Verwey-Overbeek的理論支持。 接著,我們引入一種新的氟化富勒烯,用作鈣鈦礦(CsFAMA)光伏電池中的電子傳輸層(Electron transporting layer, ETL),效率可達21.27%,並顯著的提高了濕度,熱和離子遷移的耐久性。因氟化富勒烯的疏水特性使得未封裝的PSCs在相對濕度85%的條件下,仍然超過1,400個小時以上的溼度穩定性,且該設備在水下浸泡了600秒後仍保持其原始性能的70%。此外,我們也發現氟化的富勒烯可以固定鈣鈦礦中的有機離子並使表面缺陷鈍化,提升元件的光熱穩定性。結果對長期的光浸泡以及高溫老化表現出極好的耐受性,在氮氣的環境下持續的光照(1-sun)或在85oC加熱1,000小時,可保持其超過95%的初始效率。由於氟化富勒烯的電子傳導層在PSCs中的成功可以激發進一步的研究,為未來的光伏技術帶來真正的動力。 我們進一步利用原位同步加速器X射線表徵來明確揭示鈣鈦礦薄膜在不同相對濕度的退火過程中材料轉變和結晶過程,水的結合對晶粒尺寸和轉化率表現出顯著的促進作用。我們確定了鈣鈦礦的晶體取向、晶格常數、晶粒尺寸和退火過程中的轉變速率與水分子之間的相關性,在當相對濕度為40%的氮氣中退火時,鈣鈦礦晶體顯示出較好的取向性和較大的晶粒尺寸。我們的工作對於鈣鈦礦薄膜在結晶過程中的水混入效果提出了深入地瞭解,更重要的是,透過簡易的水結合方式即可大幅提升元件的光穩定性和熱穩定性,使得原本較為不穩定的MAPbI3鹵化物鈣鈦礦可與他人所使用較為穩定的鈣鈦礦系統(CsFAMA)所提出的研究成果相提並論。"zh_TW
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dc.description.tableofcontents口試委員審定書 i 摘要 ii ABSTRACT iv CONTENTS vii LIST OF FIGURES x LIST OF TABLES xxv Chapter 1 Introduction 1 1.1 Renewable energy 1 1.2 Photovoltaics 3 1.2.1 Theory and working principles of photovoltaics 6 1.2.2 Solar spectra 7 1.2.3 Photovoltaic parameters 8 1.3 Introduction of perovskite solar cells 12 1.3.1 Fundamentals of organometal halide perovskites and their origin 12 1.3.2 Phase transition 14 1.3.3 Band position and bandgap tuning 18 1.3.4 Compositional engineering 20 1.3.5 Evolution of architecture design 23 1.3.6 Solution chemistry 28 1.3.7 Preparation methods 32 1.3.8 Issues and challenges 35 1.4 Objectives and Scope 39 Chapter 2 Experimental Methods 44 2.1 Materials 44 2.1.1 MMT Preparation and Characterization 48 2.2 Device fabrication 52 2.2.1 HTL fabrication 53 2.2.2 Perovskite layer 53 2.2.3 ETL fabrication 55 2.2.4 Hole blocking layer and electrode 56 2.3 Instrument 56 Chapter 3 Boosting the ultra-stable unencapsulated perovskite solar cells by using montmorillonite CH3NH3PbI3 nanocomposite as photoactive layer 64 3.1 Motivation 64 3.2 Results and Discussion 65 3.2.1 Superior environmental stability of exMMT/MAPbI3 films 69 3.2.2 Superior photovoltaic stability of PSCs with exMMT 75 3.2.3 ExMMTs formed as a shell on the surface of MAPbI3 film 79 3.2.4 Damp-heat tests of PSCs 83 3.2.5 Light soaking tests of PSCs 87 3.3 Summary 88 Chapter 4 Robust un-encapsulated perovskite solar cells protected by fluorinated fullerene electron transporting layer 90 4.1 Motivation 90 4.2 Results and Discussion 94 4.2.1 Surface segregation of fluorinated fullerene 94 4.2.2 Device performance 98 4.2.3 Photovoltaic thermal stability 104 4.2.4 Environmental stability 113 4.2.5 Photo-induced ion migration 125 4.3 Summary 136 Chapter 5 Mild Water Intake Orients Crystal Formation and Imparts Highly Tolerable Unencapsulated Halide Perovskite Solar Cells 137 5.1 Motivation 137 5.2 Results and Discussion 141 5.2.1 Impact of humidity on crystal formation and orientation 141 5.2.2 Crystal structure analysis and optical property characterizations 151 5.2.3 Device performance 161 5.2.4 Stability of perovskite solar cells 166 5.3 Summary 173 Chapter 6 Conclusion 175 References 180
dc.language.isoen
dc.subject定向晶體形成zh_TW
dc.subject鈣鈦礦太陽能電池zh_TW
dc.subject奈米蒙脫土zh_TW
dc.subject氟化富勒烯電子傳輸層zh_TW
dc.subject長效穩定性zh_TW
dc.subject原位掠入射廣角X射線散射zh_TW
dc.subjectmontmorilloniteen
dc.subjectorients crystal formationen
dc.subjectin situ grazing incidence wide-angle X-ray scatteringen
dc.subjectlong-term operation stabilityen
dc.subjectfluorinated fullerene electron transporting layeren
dc.subjectperovskite solar cellsen
dc.title延長有機金屬鹵化物鈣鈦礦太陽能電池壽命之研究zh_TW
dc.titleEnhancement in Operation Lifespan of Organometal Halide Perovskite Solar Cellsen
dc.date.schoolyear109-2
dc.description.degree博士
dc.contributor.author-orcid0000-0003-1863-1006
dc.contributor.advisor-orcid林金福(0000-0002-4187-9424)
dc.contributor.coadvisor王立義(Leeyih Wang)
dc.contributor.coadvisor-orcid王立義(0000-0002-6368-0141)
dc.contributor.oralexamcommittee林維芳(Hsin-Tsai Liu),鄭弘隆(Chih-Yang Tseng),陳志平,柯崇文,施彥辰
dc.subject.keyword鈣鈦礦太陽能電池,奈米蒙脫土,氟化富勒烯電子傳輸層,長效穩定性,原位掠入射廣角X射線散射,定向晶體形成,zh_TW
dc.subject.keywordperovskite solar cells,montmorillonite,fluorinated fullerene electron transporting layer,long-term operation stability,in situ grazing incidence wide-angle X-ray scattering,orients crystal formation,en
dc.relation.page224
dc.identifier.doi10.6342/NTU202101239
dc.rights.note同意授權(全球公開)
dc.date.accepted2021-07-05
dc.contributor.author-college工學院zh_TW
dc.contributor.author-dept材料科學與工程學研究所zh_TW
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