基于硅纳米线阵列的有机/无机杂化光伏电池的制备及性能表征研究
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摘要
太阳能因其清洁，无污染，可再生等独特优势受到人们的广泛关注与青睐。太阳能电池（也称光伏电池）作为利用太阳能的主要手段之一，在过去几十年内得到很大的发展。目前市场上销售的光伏电池主要是单晶或多晶硅光伏电池，其高昂的发电成本限制了电池的广泛使用。为降低硅光伏电池的成本,本文从两个方面对电池进行改性：第一，硅纳米阵列结构代替平面硅，硅纳米阵优异的光学和电学性能可降低电池中硅原料所需的厚度和纯度；第二，将有机/无机材料进行复合，制备杂化硅光伏电池，利用共轭分子可溶液制备的特性，简化硅光伏电池的制备过程。基于以上研究思想，本课题采用简单的溶液刻蚀法制备硅纳米线阵列，并对其表面进行钝化处理，在此基础上制备了一系列硅纳米结构/共轭分子光伏电池，其主要研究工作如下：
1、以离子液体作为电解液，制备准固态的硅/离子液体光电化学光伏器件，并研究了不同表面修饰的硅电极对器件性能的影响。经过优化，该光伏器件的转化效率已达到6%。硅表面的X射线光电子能谱与器件的稳定性测试表明，该方法制备的光伏器件的稳定性明显优于传统的以水或有机溶剂为电解液的光伏器件。
2、将一种共轭小分子（Spiro-OMeTAD）引入硅电池中，溶液法制备了全固态硅/共轭分子异质结光伏电池。通过比较核-壳径向异质结结构器件的性能与嵌入式以及平面结构异质结器件的性能，阐述了核-壳形成的径向异质结在器件中的独特的优势。经过优化，该光伏器件的转化效率可达9.7%，为同时期所报道的硅杂化光伏电池的最高转化效率。
3、基于硅/共轭高分子（PEDOT:PSS）肖特基光伏器件的制备及性能表征，研究出当前硅/PEDOT:PSS肖特基光伏器件性能不稳定的因素。在此基础上通过原子力显微镜对PEDOT:PSS形貌、电势进行表征，测试硅/PEDOT:PSS肖特基电池的电流密度-电压曲线、电容-电压曲线、瞬态衰减电压测试曲线，研究了PEDOT:PSS对该类电池性能的影响。
4、摸索出重现性较高硅/PEDOT:PSS肖特基光伏器件的制备条件，在该条件下器件的转换效率可稳定在~9%。对电池进行简单的理论模拟，研究PEDOT:PSS的功函对电池性能的影响。将Pt、TiC等颗粒引入PEDOT:PSS溶液中，对PEDOT:PSS膜进行掺杂，实验结果显示，掺杂后电池的性能得到明显的改善，电池的转换效率可提高14%，达到10.35%左右。
In recent years, due to the petroleum extinction and environmental pollutionproblem, photovoltaics (PV) have become a most pursued renewable energy technology.At present, crystallized silicon photovoltaics have hold more than80%market sharebecause of their non-toxic, abundant raw materials and the long-term stability.However，the cost of cell is still too high limiting its widespread use. In order to reducethe cell cost, oranic-inorganic hybrid solar cell based on silicon nanowire arrayarchitecture (SiNWs) and conjugated moleculas are investigated.
In the traditional high efficient planar silicon cells, in order to ensure collection ofthe photogenerated charge carriers, minority-carrier diffusion length needs to becompatible with the ultra long absorption optical depth (up to200μm), which isassociated with the indirect band gap semiconductor properties, therefore highlypurified crystalline as well as thick absorption sheet is required. Comparing with theplanar silicon cells, hybrid radial heterojunction solar cells based on SiNWs andconjugated moleculas have several advantages. First, the radical junction based onSiNWs which shows excellent light harvesting capability and efficient charge-carrierextraction can reduce the amount as well as the purify of silicon used in the cell. Second,the hybrid heterojunctions take advantage of the solution-based processes of conjugatedmoleculas, which simplify the fabrication processes and reduce the manufacturing costof the cell.
The main subject of this work is to fabricate the low-cost and high-efficiency PVcells composed of SiNWs and conjugated moleculas. Here, the SiNWs are fabricated bythe metal-assisted solution etching method and passivated by methylation. The majorwork can be summarized as follows:
1、Photoelectrochemical (PEC) cells based on different Si electrodes and ionicliquid (IL) are fabricated. The X-ray photoelectron spectrum measurement and thestability measurement of the cell shows that methylation and IL can protect the silicon from oxidation. The moderate efficiency and the excellent stability of the PEC celldemonstrate that the cell may have the potential of practical use.
2、Heterojunction solar cells based on SiNWs and Spiro-OMeTAD are fabricatedby a simple solution method. The devices with radial junction show excellent efficiencyof~10.0%. By comparing the performance of the device with core-shell structure to thatof the device with the embedded one as well as the planar one, the necessity of radialjunction with core-shell structure is outlined.
3、In addition to the AFM and SKPM images of PEDOT:PSS films, by analyzingthe current density-voltage curves, the capantance-voltage measurements and thetransient photovoltage measurements of the Schottky cells composed of Silicon andPEDOT:PSS, the poor reproducibility of Si/PEDOT:PSS cell as well as the the influenceof PEDOT:PSS film is investragated.
4、The method which shows good repeatability of the Silicon/PEDOT:PSS cells isdemonstrated. Simply simulate the work function of PEDOT:PSS affection to theSilicon/PEDOT:PSS cell. The efficiency can be increased14%when the particles of Ptand TiC are added to the PEDOT:PSS films, attaining the value of10.35%.
1、以离子液体作为电解液，制备准固态的硅/离子液体光电化学光伏器件，并研究了不同表面修饰的硅电极对器件性能的影响。经过优化，该光伏器件的转化效率已达到6%。硅表面的X射线光电子能谱与器件的稳定性测试表明，该方法制备的光伏器件的稳定性明显优于传统的以水或有机溶剂为电解液的光伏器件。
2、将一种共轭小分子（Spiro-OMeTAD）引入硅电池中，溶液法制备了全固态硅/共轭分子异质结光伏电池。通过比较核-壳径向异质结结构器件的性能与嵌入式以及平面结构异质结器件的性能，阐述了核-壳形成的径向异质结在器件中的独特的优势。经过优化，该光伏器件的转化效率可达9.7%，为同时期所报道的硅杂化光伏电池的最高转化效率。
3、基于硅/共轭高分子（PEDOT:PSS）肖特基光伏器件的制备及性能表征，研究出当前硅/PEDOT:PSS肖特基光伏器件性能不稳定的因素。在此基础上通过原子力显微镜对PEDOT:PSS形貌、电势进行表征，测试硅/PEDOT:PSS肖特基电池的电流密度-电压曲线、电容-电压曲线、瞬态衰减电压测试曲线，研究了PEDOT:PSS对该类电池性能的影响。
4、摸索出重现性较高硅/PEDOT:PSS肖特基光伏器件的制备条件，在该条件下器件的转换效率可稳定在~9%。对电池进行简单的理论模拟，研究PEDOT:PSS的功函对电池性能的影响。将Pt、TiC等颗粒引入PEDOT:PSS溶液中，对PEDOT:PSS膜进行掺杂，实验结果显示，掺杂后电池的性能得到明显的改善，电池的转换效率可提高14%，达到10.35%左右。
In recent years, due to the petroleum extinction and environmental pollutionproblem, photovoltaics (PV) have become a most pursued renewable energy technology.At present, crystallized silicon photovoltaics have hold more than80%market sharebecause of their non-toxic, abundant raw materials and the long-term stability.However，the cost of cell is still too high limiting its widespread use. In order to reducethe cell cost, oranic-inorganic hybrid solar cell based on silicon nanowire arrayarchitecture (SiNWs) and conjugated moleculas are investigated.
In the traditional high efficient planar silicon cells, in order to ensure collection ofthe photogenerated charge carriers, minority-carrier diffusion length needs to becompatible with the ultra long absorption optical depth (up to200μm), which isassociated with the indirect band gap semiconductor properties, therefore highlypurified crystalline as well as thick absorption sheet is required. Comparing with theplanar silicon cells, hybrid radial heterojunction solar cells based on SiNWs andconjugated moleculas have several advantages. First, the radical junction based onSiNWs which shows excellent light harvesting capability and efficient charge-carrierextraction can reduce the amount as well as the purify of silicon used in the cell. Second,the hybrid heterojunctions take advantage of the solution-based processes of conjugatedmoleculas, which simplify the fabrication processes and reduce the manufacturing costof the cell.
The main subject of this work is to fabricate the low-cost and high-efficiency PVcells composed of SiNWs and conjugated moleculas. Here, the SiNWs are fabricated bythe metal-assisted solution etching method and passivated by methylation. The majorwork can be summarized as follows:
1、Photoelectrochemical (PEC) cells based on different Si electrodes and ionicliquid (IL) are fabricated. The X-ray photoelectron spectrum measurement and thestability measurement of the cell shows that methylation and IL can protect the silicon from oxidation. The moderate efficiency and the excellent stability of the PEC celldemonstrate that the cell may have the potential of practical use.
2、Heterojunction solar cells based on SiNWs and Spiro-OMeTAD are fabricatedby a simple solution method. The devices with radial junction show excellent efficiencyof~10.0%. By comparing the performance of the device with core-shell structure to thatof the device with the embedded one as well as the planar one, the necessity of radialjunction with core-shell structure is outlined.
3、In addition to the AFM and SKPM images of PEDOT:PSS films, by analyzingthe current density-voltage curves, the capantance-voltage measurements and thetransient photovoltage measurements of the Schottky cells composed of Silicon andPEDOT:PSS, the poor reproducibility of Si/PEDOT:PSS cell as well as the the influenceof PEDOT:PSS film is investragated.
4、The method which shows good repeatability of the Silicon/PEDOT:PSS cells isdemonstrated. Simply simulate the work function of PEDOT:PSS affection to theSilicon/PEDOT:PSS cell. The efficiency can be increased14%when the particles of Ptand TiC are added to the PEDOT:PSS films, attaining the value of10.35%.
引文
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