聚合物太阳能电池的界面修饰研究
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摘要
界面修饰在高性能的有机太阳能电池的制备，提升器件稳定性等方面起到关键作用。但界面修饰材料及其应用仍面临限制需要进一步研究改进。例如如何改进界面层制备过程，避免真空蒸镀过程使其适用于低成本大规模的溶液法器件制备；改进材料本身及作用于有机太阳能电池器件后的稳定性；改善界面层制备工艺，避免对界面层的后处理对活性层产生破坏；制备适用于不同材料体系的太阳能电池界面材料，突破很多界面材料只对特殊体系有效的限制。
本论文中，针对如何克服以上界面构筑中面临的问题，我们做了如下工作。
1.在有机太阳能电池界面引入两亲性自组装分子层PAH-D，改善器件活性层表面浸润性，使水相的高导电PEDOT：PSS可以通过溶液旋涂法制备并作为电极，实现全溶液无真空过程有机太阳能电池的构筑。PAH-D是一种可溶液法制备可以沉积在亲水及疏水表面的自组装分子，通过沉积PAH-D使表面转换为两亲性，为构筑多功能层的太阳能电池提供了普遍适用的手段。
2.通过原位聚合，引入自组装界面修饰分子等方法，优化有机聚合物与无机材料的界面进而控制活性层相分离尺度及电荷传输性质。首先通过原位聚合方法，控制基于PPV以及TiO2的太阳能电池活性层相分离，避免了传统聚合物与无机纳米晶之间共混因界面表面能差异引起的大尺度相分离。此外，我们通过引入两亲性极性自组装分子修饰ZnO表面，构筑了极性可控的聚合物纳米晶界面，得到了相分离尺度可控P3HT：ZnO复合活性层。通过优化自组装分子能级构筑阶梯状的器件能级结构，改进给受体之间的电荷传输，避免传统绝缘分子修饰引起的阻碍电荷传输及电子陷阱作用。
3.首次制备了基于P（VDF-TrFE）的有机铁电纳米晶并作为界面层引入有机太阳能电池。通过溶液旋涂将其制备与活性层表面，铁电纳米晶可在电池内部引入一个电场有效促进激子分离，提升电荷收集效率。相对之前工作，溶液法纳米晶界面层避免了LB拉膜过程中水氧对活性层的破坏，以及热退火处理对窄带隙材料的破坏。
Interfacial modification play a key role in fabricating multilayerarchitecture devices, improving the PCE of polymer solar cells (PSCs) andoptimizing the stability and lifetime of devices. However there still someissues to be improved: the fabrication of interfacial layer shouldcompatible with solution processed PSC. Improve the stability of materialsof interfacial layer. Avoid the post treatment such as thermal annealingwhich make damage to active layer. Developing novel interfacial materialswhich compatible with most materials systems.
In this thesis, we made efforts to improve above aspects:
1. We introduce PAH-D layer to modify the active layer surface ofP3HT:PCBM and convert the hydrophobic surface to amphiphilic and a aqueousPEDOT:PSS PH500can be deposited on surface of active layer as electrode.All-spin-coating vacuum-free processed semi-transparent PSCs wasfabricated. PAH-D is a amphiphilic self assembly molecules which can bedeposited onto both hydrophobic or hydrophilic surface. By introducingamphiphilic PAH-D as interfacial layer, we can convert the hydrophobic orhydrophilic surface to amphiphilic. So solution with different surfaceenergy can be deposited layer by layer according solution process such asspin coating which providing a method for constructing multilayer solutionprocess device architectures and making all solution processed PSCs.
2. The interface between polymer and nano crystals （NCs） was optimizedby using in-suit polymerization, introducing the SAM modifier to modifythe surface of NCs. By in-suit polymerization, the phase separation betweenpolymer and NCs can be controlled and avoid the large scale aggressioncaused by the naturally differences of their surface energy. The surfacemodification by SAM modifier can construct an aligned energy levelstructures and beneficial for the charge transport as well as optimize themorphology of PSCs.
3. We make the preformation of P(VDF-TrFE50:50) NCs by a solutionchemistry method and their application in low bandgap PSCs to avoid hightemperature, post-deposition thermal annealing. To the best of ourknowledge, this is the first time that ferroelectric polymer NCs weresynthesized by a very simple solution method and applied in FE-OPVs. Thesize of P(VDF-TrFE) NPs and their crystallinity can be easily controlledbefore they are inserted into the PSCs. The coverage of the P(VDF-TrFE)ferroelectric interlayer can then be precisely manipulated to maximize theefficiency of FE-OPVs. It is easy to deposit the NC layer using solutionprocess. The best PCE reached6.64%, which is among the highest valuesreported for PCDTBT-based solar cells.
本论文中，针对如何克服以上界面构筑中面临的问题，我们做了如下工作。
1.在有机太阳能电池界面引入两亲性自组装分子层PAH-D，改善器件活性层表面浸润性，使水相的高导电PEDOT：PSS可以通过溶液旋涂法制备并作为电极，实现全溶液无真空过程有机太阳能电池的构筑。PAH-D是一种可溶液法制备可以沉积在亲水及疏水表面的自组装分子，通过沉积PAH-D使表面转换为两亲性，为构筑多功能层的太阳能电池提供了普遍适用的手段。
2.通过原位聚合，引入自组装界面修饰分子等方法，优化有机聚合物与无机材料的界面进而控制活性层相分离尺度及电荷传输性质。首先通过原位聚合方法，控制基于PPV以及TiO2的太阳能电池活性层相分离，避免了传统聚合物与无机纳米晶之间共混因界面表面能差异引起的大尺度相分离。此外，我们通过引入两亲性极性自组装分子修饰ZnO表面，构筑了极性可控的聚合物纳米晶界面，得到了相分离尺度可控P3HT：ZnO复合活性层。通过优化自组装分子能级构筑阶梯状的器件能级结构，改进给受体之间的电荷传输，避免传统绝缘分子修饰引起的阻碍电荷传输及电子陷阱作用。
3.首次制备了基于P（VDF-TrFE）的有机铁电纳米晶并作为界面层引入有机太阳能电池。通过溶液旋涂将其制备与活性层表面，铁电纳米晶可在电池内部引入一个电场有效促进激子分离，提升电荷收集效率。相对之前工作，溶液法纳米晶界面层避免了LB拉膜过程中水氧对活性层的破坏，以及热退火处理对窄带隙材料的破坏。
Interfacial modification play a key role in fabricating multilayerarchitecture devices, improving the PCE of polymer solar cells (PSCs) andoptimizing the stability and lifetime of devices. However there still someissues to be improved: the fabrication of interfacial layer shouldcompatible with solution processed PSC. Improve the stability of materialsof interfacial layer. Avoid the post treatment such as thermal annealingwhich make damage to active layer. Developing novel interfacial materialswhich compatible with most materials systems.
In this thesis, we made efforts to improve above aspects:
1. We introduce PAH-D layer to modify the active layer surface ofP3HT:PCBM and convert the hydrophobic surface to amphiphilic and a aqueousPEDOT:PSS PH500can be deposited on surface of active layer as electrode.All-spin-coating vacuum-free processed semi-transparent PSCs wasfabricated. PAH-D is a amphiphilic self assembly molecules which can bedeposited onto both hydrophobic or hydrophilic surface. By introducingamphiphilic PAH-D as interfacial layer, we can convert the hydrophobic orhydrophilic surface to amphiphilic. So solution with different surfaceenergy can be deposited layer by layer according solution process such asspin coating which providing a method for constructing multilayer solutionprocess device architectures and making all solution processed PSCs.
2. The interface between polymer and nano crystals （NCs） was optimizedby using in-suit polymerization, introducing the SAM modifier to modifythe surface of NCs. By in-suit polymerization, the phase separation betweenpolymer and NCs can be controlled and avoid the large scale aggressioncaused by the naturally differences of their surface energy. The surfacemodification by SAM modifier can construct an aligned energy levelstructures and beneficial for the charge transport as well as optimize themorphology of PSCs.
3. We make the preformation of P(VDF-TrFE50:50) NCs by a solutionchemistry method and their application in low bandgap PSCs to avoid hightemperature, post-deposition thermal annealing. To the best of ourknowledge, this is the first time that ferroelectric polymer NCs weresynthesized by a very simple solution method and applied in FE-OPVs. Thesize of P(VDF-TrFE) NPs and their crystallinity can be easily controlledbefore they are inserted into the PSCs. The coverage of the P(VDF-TrFE)ferroelectric interlayer can then be precisely manipulated to maximize theefficiency of FE-OPVs. It is easy to deposit the NC layer using solutionprocess. The best PCE reached6.64%, which is among the highest valuesreported for PCDTBT-based solar cells.
引文
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