金纳米颗粒在聚合物太阳能电池中的应用
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摘要
将太阳能直接转化为电能的太阳能电池是解决当今世界日益严重的能源危机的一条重要途径。聚合物太阳能电池由于具有制备工艺简单、成本低廉、柔韧性好等优点,受到科学家们的广泛关注。然而聚合物太阳能电池相比于商业化的无机太阳能电池,其较低的能量转换效率仍然是制约其实用化的一个重要原因。影响聚合物太阳能电池效率提高的一个重要因素是其活性层的光吸收厚度远大于激子的扩散长度,导致活性层必须牺牲对光的吸收来保证激子的有效扩散。因此,如何在不增加活性层厚度的情况下增强光吸收是提高聚合物太阳能电池性能的一条有效途径。
贵金属纳米材料具有独特的表面等离子体共振(LSPR)特性,LSPR可以在纳米晶体的周围产生一个强电磁场,而此电磁场作用于周围的物质可以增强它们的光吸收。这一特性使贵金属纳米材料成为提高聚合物太阳能电池光吸收能力的一种有效选择。本论文从金纳米颗粒(Au NPs)的合成和组装出发,以提高聚合物太阳能电池的性能为目标,开展了一系列的工作。
论文第一章综述了聚合物太阳能电池的原理和器件结构,近几年来的研究进展,以及贵金属纳米材料在聚合物太阳能电池中的应用。
论文第二章研究了Au NPs Langmuir-Blodgett (LB)单层薄膜的引入对聚合物太阳能电池(ITO/PEDOT:PSS/MEH-PPV:PCBM/Al, ITO:indium tin-oxide; PEDOT:PSS:poly3,4-ethylenedioxy-thiophene:polystyrenesulfonate; MEH-PPV: poly(2-mthoxy-5(2'-ethylhexyloxy)-1,4-phenylenevinylene); PCBM:[6,6]-phenyl-C61-butyric acid methyl ester)性能的影响,结果显示在聚合物太阳能电池的阳极与阳极界面修饰层之间引入氧化金纳米颗粒LB单层薄膜可以增强器件的性能。研究发现氧化金纳米颗粒单层薄膜的加入可以同时提高器件的短路电流Jsc和开路电压Voc,其中Jsc的提高主要源于金纳米颗粒薄膜的LSPR效应,而Voc的增加则归因于插入了高功函的氧化金纳米颗粒薄膜层。
论文第三章研究了聚合物太阳能电池(ITO/PEDOT:PSS/P3HT:PCBM/Al, P3HT:poly(3-hexylthiophene))阳极界面修饰层(PEDOT:PSS)中掺杂不同粒径Au NPs对器件性能的影响。我们发现,只有当Au NPs粒径大于PEDOT:PSS层厚度时,Au NPs的LSPR效应才能引起活性层P3HT:PCBM吸收的增强；同时,Au NPs粒径的增大可以提高PEDOT:PSS薄膜表面粗糙度,增大其与活性层的接触面积,从而提高器件的空穴收集效率。但是,Au NPs粒径的进一步增大还会引起活性层形貌的变化,使给体/受体界面处的激子分离效率降低。因此,器件的Jsc和能量转化效率PCE的变化趋势是这两方面竞争的结果。
论文第四章研究了聚合物太阳能电池(ITO/PEDOT:PSS/P3HT:PCBM/Al)活性层(P3HT:PCBM)中掺杂Au NPs对器件性能的增强作用。研究表明,随着加入Au NPs浓度或粒径的增大,聚合物太阳能电池活性层的吸收强度会逐渐增大；但是同时活性层中的激子分离效率会逐渐降低。另外,器件的载流子迁移率也会随入Au NPs浓度增大先增加后减小。
论文第五章研究了Au NPs在有机-无机杂化太阳能电池(ITO/PEDOT:PSS/CdSe:PCPDTBT/Al, PCPDTBT:poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta [2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)])中的应用,将相同粒径的Au NPs分别掺杂于阳极界面修饰层(PEDOT:PSS)和活性层(CdSe:PCPDTBT)中,均可增强器件的性能。其中,PEDOT:PSS层掺杂低浓度Au NPs后,通过提高空穴的收集效率,使器件的效率从2.95%提高到了3.20%。而CdSe:PCPDTBT活性层掺杂低浓度Au NPs后,同时增加了活性层的光学吸收和空穴的迁移率,从而使器件的效率从2.91%提高到了3.16%。
Solar cell, which can directly convert solar energy into electricity, is one of the most significant approaches to solve the increasing serious energy crisis in the world. Due to their simple fabrication procedure, physical flexibility and low cost, polymer solar cells (PSCs) have attracted great attentions. However, compared with the inorganic solar cells, the low power conversion efficiency (PCE) of PSCs is still one of the main problems for practical applications. A major factor influencing the efficiency greatly is the limited light absorption due to the thin active layer which is limited by the short exciton diffusion length and low carries mobility of polymers. Therefore, it's an efficient approach to enhance performance of PSCs by improving the photon absorption efficiency of active layer while keeping their thickness still thin enough to maintain the effective exciton diffusion and charge transport.
Metallic nanoparticles (NPs) such as Au and Ag NPs exhibit localized surface plasmon resonance (LSPR) property. The LSPR effect can create strong near-field electromagnetic fields which can improve the optical properties of the surrounding materials. These properties make metallic NPs one of the potential candidates for improving the photon absorption efficiency of PSCs. In this thesis, we reported the performance enhancement of PSCs by incorporating Au NPs or Au NPs films in the hole transport layer (PEDOT:PSS) or the active layer.
In Chapter1, the working principle, device structure and recent progress of polymer solar cells are reviewed. The applications of noble metallic nanomaterials in PSCs are also summarized.
In Chapter2, we reported the enhanced performance of PSCs (ITO/PEDOT:PSS/MEH-PPV:PCBM/Al, ITO:indium tin-oxide; PEDOT:PSS:poly3,4-ethylenedioxy-thiophene:polystyrenesulfonate; MEH-PPV:poly(2-mthoxy-5(2'-ethylhexyloxy)-1,4-phenylenevinylene); PCBM:[6,6]-phenyl-C61-butyric acid methyl ester) by incorporation of a Langmuir-Blodgett assembled Au NPs monolayer between the anode and the hole transport layer. Our results show that both open-circuit voltage (Voc) and short-circuit current (Jsc) of PSCs can be improved after incorporating Au NPs monolayer. We attribute the improvement of Jsc to the LSPR effect of Au NPs films, while the improvement of Voc is due to the high work function of the incorporated oxidized Au NPs monolayer.
In Chapter3, we studied the performance enhancement phenomenon of PSCs (ITO/PEDOT:PSS/P3HT:PCBM/A1, P3HT:poly(3-hexylthiophene)) by incorporation of various sized Au NPs in the anode modification layer (PEDOT:PSS). We found that the light absorption of the active layer can't be improved until the size of Au NPs is larger than the thickness of the PEDOT:PSS layer; besides, as the size of Au NPs increased, the roughness of PEDOT:PSS increased, enlarging the interface areas between PEDOT:PSS and the active layer, and resulting in the improved hole collection efficiency at the anode. However, the morphology of the active layer would change to reduce the D/A interface area, leading to reduction of exciton dissociation efficiency, while further increasing the size of Au NPs. Therefore, the trends of Jsc and PCE of PSCs resulted from the competition between the two effects.
In Chapter4, we studied the performance enhancement effect of PSCs (ITO/PEDOT:PSS/P3HT:PCBM/A1) by incorporation of Au NPs in the active layer. Our work shows that the light absorption of the active layer can be improved while the exciton dissociation efficiency would be reduced, as increasing the concentration or size of Au NPs. Meanwhile, the carrier mobilities of PSCs were improved at low Au NPs concentration, but reduced while further increasing the Au NPs concentration.
In Chapter5, we reported the enhanced performance of CdSe:PCPDTBT (PCPDTBT:poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)]) hybrid solar cells (HSCs) by incorporation of the same sized Au NPs in the PEDOT:PSS layer or the CdSe:PCPDTBT active layer. Compared to the control device, the PCE of HSCs improved from2.95%to3.20%after incorporating Au NPs in the PEDOT:PSS layer, due to the increased hole collection efficiency; while the PCE of HSCs improved from2.91%to3.16%after incorporating Au NPs in the CdSe:PCPDTBT active layer, resulting from the enhanced light absorption intensity and the improved hole mobility of the CdSe:PCPDTBT active layer.
贵金属纳米材料具有独特的表面等离子体共振(LSPR)特性,LSPR可以在纳米晶体的周围产生一个强电磁场,而此电磁场作用于周围的物质可以增强它们的光吸收。这一特性使贵金属纳米材料成为提高聚合物太阳能电池光吸收能力的一种有效选择。本论文从金纳米颗粒(Au NPs)的合成和组装出发,以提高聚合物太阳能电池的性能为目标,开展了一系列的工作。
论文第一章综述了聚合物太阳能电池的原理和器件结构,近几年来的研究进展,以及贵金属纳米材料在聚合物太阳能电池中的应用。
论文第二章研究了Au NPs Langmuir-Blodgett (LB)单层薄膜的引入对聚合物太阳能电池(ITO/PEDOT:PSS/MEH-PPV:PCBM/Al, ITO:indium tin-oxide; PEDOT:PSS:poly3,4-ethylenedioxy-thiophene:polystyrenesulfonate; MEH-PPV: poly(2-mthoxy-5(2'-ethylhexyloxy)-1,4-phenylenevinylene); PCBM:[6,6]-phenyl-C61-butyric acid methyl ester)性能的影响,结果显示在聚合物太阳能电池的阳极与阳极界面修饰层之间引入氧化金纳米颗粒LB单层薄膜可以增强器件的性能。研究发现氧化金纳米颗粒单层薄膜的加入可以同时提高器件的短路电流Jsc和开路电压Voc,其中Jsc的提高主要源于金纳米颗粒薄膜的LSPR效应,而Voc的增加则归因于插入了高功函的氧化金纳米颗粒薄膜层。
论文第三章研究了聚合物太阳能电池(ITO/PEDOT:PSS/P3HT:PCBM/Al, P3HT:poly(3-hexylthiophene))阳极界面修饰层(PEDOT:PSS)中掺杂不同粒径Au NPs对器件性能的影响。我们发现,只有当Au NPs粒径大于PEDOT:PSS层厚度时,Au NPs的LSPR效应才能引起活性层P3HT:PCBM吸收的增强；同时,Au NPs粒径的增大可以提高PEDOT:PSS薄膜表面粗糙度,增大其与活性层的接触面积,从而提高器件的空穴收集效率。但是,Au NPs粒径的进一步增大还会引起活性层形貌的变化,使给体/受体界面处的激子分离效率降低。因此,器件的Jsc和能量转化效率PCE的变化趋势是这两方面竞争的结果。
论文第四章研究了聚合物太阳能电池(ITO/PEDOT:PSS/P3HT:PCBM/Al)活性层(P3HT:PCBM)中掺杂Au NPs对器件性能的增强作用。研究表明,随着加入Au NPs浓度或粒径的增大,聚合物太阳能电池活性层的吸收强度会逐渐增大；但是同时活性层中的激子分离效率会逐渐降低。另外,器件的载流子迁移率也会随入Au NPs浓度增大先增加后减小。
论文第五章研究了Au NPs在有机-无机杂化太阳能电池(ITO/PEDOT:PSS/CdSe:PCPDTBT/Al, PCPDTBT:poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta [2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)])中的应用,将相同粒径的Au NPs分别掺杂于阳极界面修饰层(PEDOT:PSS)和活性层(CdSe:PCPDTBT)中,均可增强器件的性能。其中,PEDOT:PSS层掺杂低浓度Au NPs后,通过提高空穴的收集效率,使器件的效率从2.95%提高到了3.20%。而CdSe:PCPDTBT活性层掺杂低浓度Au NPs后,同时增加了活性层的光学吸收和空穴的迁移率,从而使器件的效率从2.91%提高到了3.16%。
Solar cell, which can directly convert solar energy into electricity, is one of the most significant approaches to solve the increasing serious energy crisis in the world. Due to their simple fabrication procedure, physical flexibility and low cost, polymer solar cells (PSCs) have attracted great attentions. However, compared with the inorganic solar cells, the low power conversion efficiency (PCE) of PSCs is still one of the main problems for practical applications. A major factor influencing the efficiency greatly is the limited light absorption due to the thin active layer which is limited by the short exciton diffusion length and low carries mobility of polymers. Therefore, it's an efficient approach to enhance performance of PSCs by improving the photon absorption efficiency of active layer while keeping their thickness still thin enough to maintain the effective exciton diffusion and charge transport.
Metallic nanoparticles (NPs) such as Au and Ag NPs exhibit localized surface plasmon resonance (LSPR) property. The LSPR effect can create strong near-field electromagnetic fields which can improve the optical properties of the surrounding materials. These properties make metallic NPs one of the potential candidates for improving the photon absorption efficiency of PSCs. In this thesis, we reported the performance enhancement of PSCs by incorporating Au NPs or Au NPs films in the hole transport layer (PEDOT:PSS) or the active layer.
In Chapter1, the working principle, device structure and recent progress of polymer solar cells are reviewed. The applications of noble metallic nanomaterials in PSCs are also summarized.
In Chapter2, we reported the enhanced performance of PSCs (ITO/PEDOT:PSS/MEH-PPV:PCBM/Al, ITO:indium tin-oxide; PEDOT:PSS:poly3,4-ethylenedioxy-thiophene:polystyrenesulfonate; MEH-PPV:poly(2-mthoxy-5(2'-ethylhexyloxy)-1,4-phenylenevinylene); PCBM:[6,6]-phenyl-C61-butyric acid methyl ester) by incorporation of a Langmuir-Blodgett assembled Au NPs monolayer between the anode and the hole transport layer. Our results show that both open-circuit voltage (Voc) and short-circuit current (Jsc) of PSCs can be improved after incorporating Au NPs monolayer. We attribute the improvement of Jsc to the LSPR effect of Au NPs films, while the improvement of Voc is due to the high work function of the incorporated oxidized Au NPs monolayer.
In Chapter3, we studied the performance enhancement phenomenon of PSCs (ITO/PEDOT:PSS/P3HT:PCBM/A1, P3HT:poly(3-hexylthiophene)) by incorporation of various sized Au NPs in the anode modification layer (PEDOT:PSS). We found that the light absorption of the active layer can't be improved until the size of Au NPs is larger than the thickness of the PEDOT:PSS layer; besides, as the size of Au NPs increased, the roughness of PEDOT:PSS increased, enlarging the interface areas between PEDOT:PSS and the active layer, and resulting in the improved hole collection efficiency at the anode. However, the morphology of the active layer would change to reduce the D/A interface area, leading to reduction of exciton dissociation efficiency, while further increasing the size of Au NPs. Therefore, the trends of Jsc and PCE of PSCs resulted from the competition between the two effects.
In Chapter4, we studied the performance enhancement effect of PSCs (ITO/PEDOT:PSS/P3HT:PCBM/A1) by incorporation of Au NPs in the active layer. Our work shows that the light absorption of the active layer can be improved while the exciton dissociation efficiency would be reduced, as increasing the concentration or size of Au NPs. Meanwhile, the carrier mobilities of PSCs were improved at low Au NPs concentration, but reduced while further increasing the Au NPs concentration.
In Chapter5, we reported the enhanced performance of CdSe:PCPDTBT (PCPDTBT:poly[2,6-(4,4-bis-(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)]) hybrid solar cells (HSCs) by incorporation of the same sized Au NPs in the PEDOT:PSS layer or the CdSe:PCPDTBT active layer. Compared to the control device, the PCE of HSCs improved from2.95%to3.20%after incorporating Au NPs in the PEDOT:PSS layer, due to the increased hole collection efficiency; while the PCE of HSCs improved from2.91%to3.16%after incorporating Au NPs in the CdSe:PCPDTBT active layer, resulting from the enhanced light absorption intensity and the improved hole mobility of the CdSe:PCPDTBT active layer.
引文
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