聚合物基柔性染料敏化太阳能电池光阳极的性能优化
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摘要
染料敏化太阳能电池(Dye-sensitized solar cell，简称DSC)是一种新型低成本的光化学太阳能电池。凭借其轻质、便携性和可折叠等优点，柔性DSC比刚性DSC拥有更加广阔的应用前景。但是由于金属基板不透明，金属基柔性DSC只能采用背射方式，光电转化效率相对较低。因而柔性DSC研究的焦点更多的集中于低温(<150oC)制备导电性良好的透明导电聚合物基柔性DSC光阳极，解决当前存在的薄膜机械强度较差、颗粒间连接性较差、DSC光电转换效率较低等问题。本论文紧密围绕以上问题，主要研究了聚合物基柔性DSC级配结构光阳极中不同尺寸纳米颗粒的分散性对薄膜内纳米颗粒的连接性、光阳极薄膜结构和柔性DSC光电性能的影响以及电子传递和复合的的影响机理，分别通过浆料改性和薄膜改性的方法，改善了级配结构薄膜表面形貌和内部颗粒的连接性，提高光电转换效率。
浆料改性方面，系统研究了匀浆分散、硝酸改性和调节浆料溶剂比例对聚合物基级配结构光阳极纳米颗粒分散性和连接性以及光电性能的影响。研究结果表明：(1)匀浆分散处理显著改善了薄膜内三种颗粒，特别是小颗粒的分散性，改善薄膜内部纳米颗粒间的连接性，减少薄膜内的裂纹和空隙，提高了光阳极薄膜的机械强度和稳定性；(2)级配浆料中硝酸的加入能够加速电子传递和抑制电子复合，有利于改善柔性DSC的光电性能，然而过量硝酸的加入也可能会导致对ITO层的腐蚀，从而严重的影响DSC的光电性能；(3)改变溶剂中水和叔丁醇的比例，可以调节浆料在基板表面的接触角和涂覆性能，从而改变氧化钛薄膜与基板的连接性；同时混合溶剂中水和叔丁醇相对比例改变，也会造成薄膜在干燥过程内部应力分布发生改变，从而改变光阳极薄膜形貌和表面裂纹数量，直接影响光电转化效率。
薄膜改性方面，系统研究了压制处理和UV-O3照射对聚合物基级配结构光阳极结构和内部颗粒连接以及光电性能的影响。研究结果表明：(1)压制处理导致级配结构表面裂纹被氧化钛纳米颗粒填充，使薄膜趋向于致密化，同时氧化钛纳米颗粒配位数提高，相应的增加了光生电子传递通道，降低了薄膜内的电荷传递电阻，促成了光电性能的改善；(2)UV-O3照射处理能够提高基板的亲水性，使浆料在基板表面的涂覆均匀性增强，同时有效的去除低温烧结光阳极薄膜中残余的有机物，改善薄膜的导电性及其内部纳米颗粒之间的连接，提高了光电转化效率。
Dye-sensitized solar cell (DSC) is promising regarded as a kind of novelphotochemical solar cell with low cost. Flexible DSCs have shown much more potentialapplication than rigid DSC because of their advantages such as portability, light weightand flexibility. The enhancement of energy conversion efficiency of flexible DSCs withthin metal substrate is restricted due to the opacity of nature defects, which decreasesthe adsorption efficiency of visible light, and results in poor energy conversionefficiency. Therefore, the research is focused on how to prepare flexible DSCphotoanode with transparent conductive polymer substrate such as ITO-PEN. Since theheat treatment temperature for these substrates is generally limited to a temperaturelower than150oC, the interparticle connections in the film still stays at a poor level,which slows down the transport of photo-induced electrons in the film and gives rise toelectron recombination. Graded structure composed of different sized nanoparticles is aporous structure with good mechanic performance, which is favorable for flexible DSCphotoanode. In this thesis, we investigated the dispersion effects of different sizednanoparticles in graded structured photoanode on the connectivity among TiO_2nanoparticles, the film structure and photovoltaic performance as well as the electrontransfer and recombination mechanism. The effects of paste optimization and posttreatment modification of film are studied in detail to improve the internal nanoparticleconnections, so as to optimize the preparation and enhance the photovoltaicperformance.
In the part of paste optimization, the effects of dispersion treatment, HNO3addition,and solvent ratio optimization on the nanoparticle dispersion and photovoltaicperformance of graded structured photoanode are systematically studied. Firstly, thedispersion of three kinds of different sized nanoparticles, especially the smallnanoparticles is greatly improved by the dispersion treatment. The dispersion treatmentalso enhances the connectivity of internal nanoparticles and reduces the cracks in thegraded structured film, which gives high mechanical strength and stability ofphotoanode. Secondly, the electron transport is accelerated by means of increasing nitricacid, which increases the coordination number of TiO_2nanoparticles and provides more possible electron transfer pathways in the photoanode. This was confirmed by thecharge transport resistance in the TiO_2film (Rt). However, excessive nitric acid alsoleaded to a corrosion of the ITO substrate and impaired the photovoltaic performance ofthe flexible devices. Thirdly, the ratio between water and tertiary butanol in the pastecan control the contact angle and coating uniformity on the surface of polymer substrate,which directly affects the connectivity between film and substrate. Changing the solventratio also leads to the change of internal stress distribution during crying, thus changingthe surface morphology and cracks density in the photoanode, consequently influencingthe energy conversion efficiency.
In the part of film modification, compression method and UV-O3illuminationtreatment on the graded structured photoanode have been applied to construct highlyefficient DSCs. The compression treatment can make the cracks filled with TiO_2nanoparticles, in order to make a denser film and increase the coordination number ofnanoparticles. As a result, more possible electron transfer pathways are provided and theRtin the photoanode decreases. Under UV-O3illumination treatment, the substratesurface hydrophily is improved greatly, leading to a more uniform coating of TiO_2pasteon the substrate. Meanwhile, the remaining impurity after drying in the film is removedeffectively with UV-O3illumination treatment, which enhances the connectivity ofinternal nanoparticles, consequently constructing highly efficient DSCs.
浆料改性方面，系统研究了匀浆分散、硝酸改性和调节浆料溶剂比例对聚合物基级配结构光阳极纳米颗粒分散性和连接性以及光电性能的影响。研究结果表明：(1)匀浆分散处理显著改善了薄膜内三种颗粒，特别是小颗粒的分散性，改善薄膜内部纳米颗粒间的连接性，减少薄膜内的裂纹和空隙，提高了光阳极薄膜的机械强度和稳定性；(2)级配浆料中硝酸的加入能够加速电子传递和抑制电子复合，有利于改善柔性DSC的光电性能，然而过量硝酸的加入也可能会导致对ITO层的腐蚀，从而严重的影响DSC的光电性能；(3)改变溶剂中水和叔丁醇的比例，可以调节浆料在基板表面的接触角和涂覆性能，从而改变氧化钛薄膜与基板的连接性；同时混合溶剂中水和叔丁醇相对比例改变，也会造成薄膜在干燥过程内部应力分布发生改变，从而改变光阳极薄膜形貌和表面裂纹数量，直接影响光电转化效率。
薄膜改性方面，系统研究了压制处理和UV-O3照射对聚合物基级配结构光阳极结构和内部颗粒连接以及光电性能的影响。研究结果表明：(1)压制处理导致级配结构表面裂纹被氧化钛纳米颗粒填充，使薄膜趋向于致密化，同时氧化钛纳米颗粒配位数提高，相应的增加了光生电子传递通道，降低了薄膜内的电荷传递电阻，促成了光电性能的改善；(2)UV-O3照射处理能够提高基板的亲水性，使浆料在基板表面的涂覆均匀性增强，同时有效的去除低温烧结光阳极薄膜中残余的有机物，改善薄膜的导电性及其内部纳米颗粒之间的连接，提高了光电转化效率。
Dye-sensitized solar cell (DSC) is promising regarded as a kind of novelphotochemical solar cell with low cost. Flexible DSCs have shown much more potentialapplication than rigid DSC because of their advantages such as portability, light weightand flexibility. The enhancement of energy conversion efficiency of flexible DSCs withthin metal substrate is restricted due to the opacity of nature defects, which decreasesthe adsorption efficiency of visible light, and results in poor energy conversionefficiency. Therefore, the research is focused on how to prepare flexible DSCphotoanode with transparent conductive polymer substrate such as ITO-PEN. Since theheat treatment temperature for these substrates is generally limited to a temperaturelower than150oC, the interparticle connections in the film still stays at a poor level,which slows down the transport of photo-induced electrons in the film and gives rise toelectron recombination. Graded structure composed of different sized nanoparticles is aporous structure with good mechanic performance, which is favorable for flexible DSCphotoanode. In this thesis, we investigated the dispersion effects of different sizednanoparticles in graded structured photoanode on the connectivity among TiO_2nanoparticles, the film structure and photovoltaic performance as well as the electrontransfer and recombination mechanism. The effects of paste optimization and posttreatment modification of film are studied in detail to improve the internal nanoparticleconnections, so as to optimize the preparation and enhance the photovoltaicperformance.
In the part of paste optimization, the effects of dispersion treatment, HNO3addition,and solvent ratio optimization on the nanoparticle dispersion and photovoltaicperformance of graded structured photoanode are systematically studied. Firstly, thedispersion of three kinds of different sized nanoparticles, especially the smallnanoparticles is greatly improved by the dispersion treatment. The dispersion treatmentalso enhances the connectivity of internal nanoparticles and reduces the cracks in thegraded structured film, which gives high mechanical strength and stability ofphotoanode. Secondly, the electron transport is accelerated by means of increasing nitricacid, which increases the coordination number of TiO_2nanoparticles and provides more possible electron transfer pathways in the photoanode. This was confirmed by thecharge transport resistance in the TiO_2film (Rt). However, excessive nitric acid alsoleaded to a corrosion of the ITO substrate and impaired the photovoltaic performance ofthe flexible devices. Thirdly, the ratio between water and tertiary butanol in the pastecan control the contact angle and coating uniformity on the surface of polymer substrate,which directly affects the connectivity between film and substrate. Changing the solventratio also leads to the change of internal stress distribution during crying, thus changingthe surface morphology and cracks density in the photoanode, consequently influencingthe energy conversion efficiency.
In the part of film modification, compression method and UV-O3illuminationtreatment on the graded structured photoanode have been applied to construct highlyefficient DSCs. The compression treatment can make the cracks filled with TiO_2nanoparticles, in order to make a denser film and increase the coordination number ofnanoparticles. As a result, more possible electron transfer pathways are provided and theRtin the photoanode decreases. Under UV-O3illumination treatment, the substratesurface hydrophily is improved greatly, leading to a more uniform coating of TiO_2pasteon the substrate. Meanwhile, the remaining impurity after drying in the film is removedeffectively with UV-O3illumination treatment, which enhances the connectivity ofinternal nanoparticles, consequently constructing highly efficient DSCs.
引文
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