混成薄膜太陽能電池之電極緩衝層及主動層研究｜國立臺灣科技大學博碩士論文系統

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研究生：	王瑋婷 Wei-Ting Wang
論文名稱：	混成薄膜太陽能電池之電極緩衝層及主動層研究 Investigation of the Electrode Buffer Layers and Active Layers of Hybrid Solar Cells
指導教授：	戴龑 Yian Tai
口試委員:	吳春桂 Chun-Guey Wu 郭宗枋 Tzung-Fang Guo 陳家浩 Chia-Hao Chen 黃柏仁 Bohr-Ran Huang 何國川 Kuo-Chuan Ho 楊重光 Chung-Kuang Yang 王立義 Lee-Yih Wang
學位類別：	博士 Doctor
系所名稱：	工程學院 - 化學工程系 Department of Chemical Engineering
論文出版年：	2018
畢業學年度：	106
語文別：	英文
論文頁數：	165
中文關鍵詞：	有機太陽能電池、鈣鈦礦太陽能電池、高分子結構及形態、溶劑工程、成分工程
外文關鍵詞：	Organic solar cells, Perovskite solar cells, Polymer structure and configuration, Solvent engineering, Composition engineering
相關次數：	點閱：246 下載：2
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本論文旨在開發新型有機半導體材料及元件製程方法，以擴展混成薄膜太陽能電池緩衝層的通用性及提升大氣製程下鈣鈦礦元件的光電轉換效率與再現性。
首先，研究一種奈米技術以調整水/醇可溶的共軛高分子自組裝形態，並鑒定了該高分子自組裝形態及量測其電性，主要包括：利用高解析穿透式電子顯微鏡(HRTEM)證明自組裝奈米球的形成、透過水接觸角(Water Contact Angle)證明奈米球具有兩種完全不同的親疏水組成、利用紫外光能譜儀(UPS)推論奈米球可透過奈米技術配置以調整電極功函數及使用空間電荷限制電流(SCLC)量測奈米球的載子傳輸特性。依據奈米球的電性表徵結果，分別將其應用於有機太陽能電池、有機發光二級體及鈣鈦礦太陽能電池的陰陽極緩衝層。其元件數據結果與傳統電極緩衝層相似甚至有更高的光電轉換效率，進而證明該材料具有廣泛應用性。
基於上述太陽能元件研究結果，光電轉換效率除了受到電極緩衝層影響外，主動層材料的種類也是至關重要的。對於以鈣鈦礦材料為主動層的太陽能元件，其製程易受環境(濕氣)影響，進而造成元件效率及再現性不佳。因此本論文亦針對碘化鉛及鈣鈦礦薄膜在大氣環境下塗佈的形成機制、薄膜形態以及結晶性質進行深入研究與探討，並成功開發了新型溶劑工程與成分工程方法以提升碘化鉛及鈣鈦礦薄膜的品質。具體地，在溶劑工程中，乾燥的異丙醇溶劑塗佈於碘化鉛薄膜表面，可提升其表面平整性、降低其結晶度；另一方面，利用成分工程方法，將氧化鋅奈米粒子摻雜於碘化鉛前驅溶液中，可得到無孔洞的薄膜。結果顯示，兩種新型方法均利於高品質鈣鈦礦薄膜的轉化，大幅提升鈣鈦礦太陽能元件效率。為了驗證這兩種方法的通用性，本論文進一步將其應用於不同基材及元件結構上，結果顯示元件效率得到大幅提升，最高達到18 %以上。
上述所提及之研究內容，已完成並發表於Energy Environ. Sci. 11 (2018) 682-691; Nano Energy 49 (2018) 109-116; ACS Appl. Mater. Interfaces 9 (2017) 10743-10751.

The present thesis aims to develop novel organic semiconductors and processes of device fabrication for extending the universality of electrode buffer layers in hybrid solar cells and enhancing the photon-to-electron conversion efficiency of fully ambient-processed perovskite solar cells with high reproducibility.
First, we utilized a nanotechnology to adjust the self-assemblies of the water/alcohol-soluble conjugated polymers, and characterized their morphologies and electronic properties, including i) high-resolution transmission electron microscopy (HRTEM) to prove the self-assemblies of nanospheres, ii) water contact angle (CA) to illustrate the surface hydrophilicities of nanospheres, iii) ultraviolet photoelectron spectrometer (UPS) to demonstrate the tunability of electrode work function and iv) space-charge-limited current (SCLC) to measure the charge carrier mobilities of nanospheres. According to the electronic properties of nanospheres, we used them as both cathode and anode buffer layers of organic solar cells, organic light-emitting diodes and perovskite solar cells, which exhibited comparable and even exceeding performance to the devices using traditional buffer layers, indicative of their universality.
In terms of these organic and perovskite solar cells, we find that not only the electrode buffer layers strongly influence the device performance, but also the active layer materials are crucial to enhance the power conversion efficiency (PCE). For instance, the fabrication processes of perovskite solar cells are vulnerable to humidity and consequently their performance and reproducibility are not controllable. Therefore, in the present thesis, we further investigated the formation mechanism, film morphology and crystallinity of fully ambient-processed lead iodide and perovskite films. Afterward, we successfully developed promising solvent and composition engineering techniques to enhance the qualities of lead iodide and perovskite films. In particular, the solvent engineering technique treated lead iodide film surface with dry isopropanol, which increased its flatness and reduced its crystallinity; on the other hand, the composition engineering technique doped zinc oxide nanoparticles into the lead iodide precursor and obtained a pinhole-free film. The results indicate that both of the techniques are benefit for the transformation of perovskite and remarkably enhance the solar cell performance. Moreover, the versatility of two techniques was illustrated by fabricating various devices with different substrates and architectures. And the significantly improved device performance revealed a best PCE over 18%.
The above mentioned studies have been finished and published in Energy Environ. Sci. 11 (2018) 682-691; Nano Energy 49 (2018) 109-116; ACS Appl. Mater. Interfaces 9 (2017) 10743-10751.

中文摘要    IV
Abstract    VI
Acknowledgement    VIII
Table of Contents    IX
List of Abbreviations    XII
List of Figures    XV
List of Tables    XXI
Chapter 1 Introduction and Literature Review    1
1 Global Energy Demend and Solar Energy    1
2 Air Mass and Solar Energy Distribution    3
2.1 Air Mass    3
2.2 Solar Energy Distribution    6
3 Potentiality of Photovoltaic Cells    6
4 Properties and Process in Organic and Organic-Inorganic Hybrid Photovaltaic Cells    8
4.1 n-Type and p-Type Organic Materials    8
4.1.1 Fermi-Level    9
4.1.2 Polymer Blending    10
4.1.3 Conjugated Polymers    12
4.1.4 Fullerene and Non-Fullerene Acceptors    13
4.1.5 Exciton Creation and Transport in Polymer    14
4.1.6 Transport of Charge and Hopping in Polymer    16
4.1.7 Free Charge Carrier Collection    16
4.2 Charge Generation and Transport in Organic and Orgniac-Inorganic Hybrid Photovoltaic Cells    18
4.2.1 Absoption of Photons    20
4.2.2 Exciton Diffusion    20
4.2.3 Charge Seperation    21
4.2.4 Charge Transport    22
4.2.5 Charge Collection    22
4.2.6 The Donor/Acceptor Interface    23
4.2.7 Schottky Barrier    24
4.2.8 Ohmic Contact    27
5 Determination of Photovoltaic Cell and Organic Light-Emitting Diode Efficiencies    28
5.1 Determination of Photovoltaic Cell    28
5.2 Determination of Organic Light-Emitting Diode Effieiencies    32
Chapter 2 Motivations for the Research    33
1 Current Trends of Photovoltaic Cells    33
1.1 Organic Photovoltaic Cells    34
1.2 Organic-Inorganic Hybrid Photovoltaic Cells    34
2 Motivation    35
Chapter 3 Experimental Section    38
1 Materials    38
2 Electrode Buffer Layers: Solution-Processed Organic and Perovskite Photovoltaic Cells    39
2.1 Synthesis and Characterization of Polymer    39
2.2 Preparation of A- and C-PDTON Solution    40
2.3 Device Fabrication    41
2.4 Film and Device Characterization    44
3 Active Layer: Fully Ambient-Processed Perovskite Photovoltaic Cells    46
3.1 Synthesis of CH3NH3I    46
3.2 Preparation of Sol-Gel ZnO and SnO2 Precursor Solutions    46
3.3 Synthesis of ZnO Nanoparticles    47
3.4 Device Fabrication for Solvent Engineering of Lead Iodide Thin Film— Fully Ambient-Processed Perovskite Film for Perovskite Solar Cells: Effect of Solvent Polarity on Lead Iodide    47
3.5 Device Fabrication for Composition Engineering of Lead Iodide Thin Film— Nanoparticle-Induced Fast Nucleation of Pinhole-Free PbI2 Film for Ambient-Processed Highly-Efficient Perovskite Solar Cell    48
3.6 Zinc Oxide Nanoparticle Characterization    49
3.7 Thin Film Characterization    49
3.8 Device Characterization    50
Chapter 4 Results and Discussion    52
1    Electrode Buffer Layers: Solution-Processed Organic and Perovskite Photovoltaic Cells    53
1.1 Solution-Processed Cathode Buffer Layers    53
1.1.1 Work Functions of PTFCN, PTFNN and PDTON Modified ITO    54
1.1.2 Organic Solar Cells Based on PTFCN, PTFNN and PDTON    55
1.2 Universal Electrode Buffer Layer Materials    56
1.2.1 PDTON Self-Assembly: A- and C-PDTON Nanospheres    59
1.2.2 Hole and Electron Mobility of PDTON    61
1.2.3 Organic Solar Cells Based on A- and C-PDTON    63
1.2.4 Organic Light-Emitting Diodes Based on A- and C-PDTON    65
1.2.5 Work Functions of PDTON Modified ITO for Perovskite Solar Cells    67
1.2.6 Mechanism    73
2    Active Layer: Fully Ambient-Processed Perovskite Photovoltaic Cells    75
2.1 Solvent Engineering of Lead Iodide Thin Film— Fully Ambient-Processed Perovskite Film for Perovskite Solar Cells: Effect of Solvent Polarity on Lead Iodide     77
2.1.1 Solvent Effect Based on Polarity Derivation    77
2.1.2 Significance of Utilizing Extra Dry IPA    83
2.1.3 Device Performance and Process Stability Analysis    85
2.1.4 Versatility of IPA100 Treatment for Inverted and Flexible Device Structures    89
2.1.5 Mechanism of Solvent-Engineering    95
2.2 Composition Engineering of Lead Iodide Thin Film— Nanoparticle-Induced Fast Nucleation of Pinhole-Free PbI2 Film for Ambient-Processed Highly-Efficient Perovskite Solar Cell    99
2.2.1 The Characteristics of Zinc Oxide Nanoparticles    99
2.2.2 The Morphology of PbI2 Thin Films    105
2.2.3 Morphology, Crystallinity and Electronic Properties of Perovskite Films    108
2.2.4 Nucleation Mechanism    115
2.2.5 Versatility of NIFN Approach in Fully Ambient-Processed Perovskite Solar Cells    119
2.2.6 Deep Insights into the Mechanism behind the Phenomena    123
Chapter 5 Conclusions and Outlook    127
References    129


                                

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