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华东理工大学硕士学位论文 第 I 页
基于一维 TiO
2
量子点敏化太阳能电池的制备
摘要
量子点具有独特的光电性能,不同尺寸和组成的量子点可吸收不同能量的光子产生
多种波长的光,在生物标记、光电器件和太阳能电池领域具有重要的应用。量子点太阳
能电池的理论转换效率可达 44%,但目前的实验结果远远低于理论预测值。
本论文研究了量子点敏化纳米晶太阳能电池的制备工艺。合成了一维二氧化钛结构,
利用连续离子吸附反应法直接沉积 CdS/CdSe 量子点到二氧化钛光阳极,优化电解液和
对电极组装成完整电池,通过结构和性能的改进,提高了电池的效率。本论文还尝试了
环境友好型纳米晶 FeS
2
的合成,其吸收谱带与太阳光谱重合率高,对制备的电池进行
了性能测试与特性表征。
本文的主要研究内容和结论包括以下三个方面:
(1) 通过阳极氧化金属钛片的方法,在恒定电位和室温下,改变持续时间,获得了
不同形貌的锐钛矿二氧化钛纳米管。利用水热法一步合成了生长在透明 FTO 玻璃上的
锐钛矿二氧化钛纳米线,是制备太阳能电池的基础。
(2) 利用连续离子层吸附法,将 CdS/CdSe 量子点沉积到一维二氧化钛结构上。配
置多硫电解液和对电极,组装成三明治结构的太阳能电池。考察三种对电极对光电性能
的影响,发现相比传统的 Pt 电极,CoS/CuS 电极工艺简单,成本低廉,性能优异。通
过比较太阳光从光阳极和对电极入射的结果,实现了光阳极入射方式较优的光电性能,
其短路电流密度为 6.40 mA/cm
2
。
(3) 采用烧瓶溶剂法和水热法制备了粒径分别为 40-50nm 和 5-10nm 的黄铁矿 FeS
2
纳米晶,将其沉积在一维二氧化钛上制备成敏化电池,得到短路电流密度和开路电压分
别为 5.2 cm
2
和 26mV。
关键词:一维二氧化钛;量子点;FeS
2
纳米晶;敏化太阳能电池
第 II 页 华东理工大学硕士学位论文
Quantum-Dots Sensitized Solar Cells Based on One-Dimentional TiO
2
Abstract
Quantum dots(QDs) with special photoelectric properties show significant values in the
feilds of bio-labeling, photoelectric devices and solar cells. Different grain size and
composition of QDs can absorb photons with various energy and give off wide wavelength of
luminescence. The therotical conversion efficiency of QDs sensitized solar cell (QDSSCs)
predictes a high value of 44%, while the experimental results shows a much lower outcome.
This thesis reported the fabrication process of QDSSCs. One-dimentional TiO
2
structure
was synthesis and CdS/CdSe QDs directly deposited on TiO
2
photo-anode by successive ion
layer adsorption and reaction (SILAR). An entire solar cell was assembled after the
optimization of electrolyte and counter electrode. The improvment of cells' structure and
performance are carried out to enhance the conversion efficiency. Besides, the synthesis of
pyrite FeS2, a nanocrystal whose absorption bands are in high coincidence with the solar
spectrum, is conducted combining with solar cells characterization and performance test.
The main research contents and results are listed as follows:
(1) By hiring anodic oxidation treatment for Ti metal foils at certain voltage and ambient
temperature, 1D anatase TiO
2
nanotubes (TNTs) with different sizes were obtained. Then
1D-TiO
2
nanowire was synthesis directly on transparent FTO glasses, which is a necessery
precondition for the assemble of solar cells.
(2) The deposition of CdS/CdSe QDs to 1D-TiO
2
SILAR and assemble of sandwich type
solar cells was investigated with desirable electrolyte and counter electrode. Based on an
comarison of three types counter electrodes, CoS/CuS electrode shows better performance
rather than Pt or CuS electrode, combining with merit of simple process and cost-performance
compatibility. Oppose to rear-side irradiation direction, front-side way shows an improved
performance with a current density of 6.40mA/cm
2
.
(3)Pyrite FeS
2
nanocrystal can be obtained by both solvothermal and hydrothermal
method, with particles size of 40-50 nm and 5-10 nm, respectively. After deposited them onto
1D-TiO2, an FeS
2
sensitized solar cells was achieved with a current desity of 5.2mA/cm
2
and
an open voltage of 26mV.
Keywords: One dimentional TiO
2
, Quantum dots, sensitized solar solar cells, pyrite
FeS
2
华东理工大学硕士学位论文 第 III 页
目录
摘要 ........................................................................................................................ I
Abstract................................................................................................................. II
目录 ..................................................................................................................... III
第 1 章 绪论 ......................................................................................................... 1
1.1 研究背景与课题来源 ......................................................................................................... 1
1.2 半导体纳米晶的基本概念 ................................................................................................. 2
1.3 敏化太阳能电池的原理和结构 ......................................................................................... 3
1.4 量子点在太阳能电池中的应用效应 ................................................................................. 5
1.4.1 禁带宽度可调效应 .......................................................................................................... 6
1.4.2 冲击离化效应及俄歇复合效应 ...................................................................................... 6
1.4.3 微带效应 .......................................................................................................................... 8
1.5 量子点敏化太阳能电池的研究现状 ................................................................................. 8
1.5.1 量子点材料的选择与匹配 .............................................................................................. 9
1.5.2 量子点的合成与敏化 .................................................................................................... 10
1.5.3 纳米结构光阳极 ............................................................................................................ 11
1.5.4 电解质 ............................................................................................................................ 13
1.5.5 对电极的研究 ................................................................................................................ 13
1.6 研究内容和意义 ............................................................................................................... 14
第 2 章 实验方法及表征手段 ........................................................................... 16
2.1 实验药品与实验设备 ....................................................................................................... 16
2.2 电池材料及性能的表征 ................................................................................................... 17
2.2.1 纳米颗粒的表征 ............................................................................................................ 17
2.2.2 太阳能电池性能的表征 ................................................................................................ 20
2.3 本章小结 ............................................................................................................................ 23
第 3 章 一维 TiO
2
光阳极的制备 ..................................................................... 25
3.1 前言 .................................................................................................................................... 25
3.2 有机电解质制备 TiO
2
纳米管 ......................................................................................... 27
3.2.1 实验过程 ........................................................................................................................ 27
3.2.2 实验现象 ........................................................................................................................ 27
3.2.3 二氧化钛纳米管阵列薄膜的表征与分析 .................................................................... 28
3.2.4 二氧化钛纳米管生成机理分析 .................................................................................... 31
3.3 二氧化钛纳米管薄膜的脱落 ........................................................................................... 34
第 IV 页 华东理工大学硕士学位论文
3.3.1 实验过程 ........................................................................................................................ 34
3.3.2 热处理前的二氧化钛纳米管阵列薄膜 ........................................................................ 35
3.4 水热法制备 TiO
2
纳米线 ................................................................................................. 38
3.4.1 实验过程 ........................................................................................................................ 38
3.4.2 二氧化钛纳米线的表征与分析 .................................................................................... 39
3.5 本章小结 ........................................................................................................................... 41
第 4 章 基于一维 TiO
2
量子点敏化太阳能电池的制备 ................................. 42
4.1 引言 ................................................................................................................................... 42
4.2 实验过程 ........................................................................................................................... 43
4.2.1 CdS/CdSe 量子点的合成 .............................................................................................. 43
4.2.2 电解质的配置 ................................................................................................................ 44
4.2.3 Pt 和 CoS/CuS 对电极的制备 ....................................................................................... 44
4.2.4 电池的封装 .................................................................................................................... 44
4.3 结果与讨论 ....................................................................................................................... 45
4.3.1 不同对电极电池性能比较 ............................................................................................ 45
4.3.2 不同氧化时间二氧化钛光阳极量子点敏化电池性能研究 ........................................ 47
4.3.4 基于透明 FTO 玻璃 TiO
2
纳米线光阳极的太阳能电池 ............................................ 52
4.4 本章小结 ........................................................................................................................... 56
第 5 章 窄带系量子点 FeS
2
敏化太阳能电池研究 ......................................... 57
5.1 前言 ................................................................................................................................... 57
5.2 烧瓶溶剂热法制备 FeS
2
黄铁矿纳米晶 .......................................................................... 58
5.2.1 实验过程 ........................................................................................................................ 58
5.2.2 FeS
2
黄铁矿纳米晶的形貌分析 ..................................................................................... 59
5.3 水热法制备 FeS
2
黄铁矿纳米晶 ...................................................................................... 60
5.3.1 实验过程 ........................................................................................................................ 60
5.3.2 水热法制备 FeS
2
相结构和形貌表征 ........................................................................... 61
5.4 FeS
2
敏化太阳能电池的制备 ............................................................................................ 62
5.4.1 实验过程 ........................................................................................................................ 62
5.4.2 结果分析 ........................................................................................................................ 63
5.5 本章小结 ........................................................................................................................... 63
第 6 章 总结与展望 ........................................................................................... 64
6.1 总结 ................................................................................................................................... 64
6.2 创新点 ............................................................................................................................... 65
6.3 展望 ................................................................................................................................... 65
参考文献 ............................................................................................................. 66
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