新型太阳能电池光阴极及纳米吸收层的基础研究
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摘要
太阳能电池由于具有清洁、廉价、高效等特点,作为一种可持续发展的能源替代方式,于近年来得到快速的发展。但目前还存在成本高,转换效率不高等缺点而没有被广泛应用。因此,降低太阳能电池的制备成本和提高太阳能电池的转换效率成为太阳能电池研究的关键,高效新型低成本太阳能电池包括染料敏化太阳能电池和纳米晶太阳能电池成为人们的研究热点。
在染料敏化太阳能电池中,多用贵金属铂作为光阴极,但其昂贵的价格限制了它的商业化应用。在薄膜太阳能电池中,CuInS2具有吸收系数大,禁带宽度与太阳光谱匹配,直接带隙半导体等优点,但使用高真空镀膜设备以及CuInS2材料的成分和光电特性对工艺过程的敏感限制了其产业化应用。
本论文在总结太阳能电池研究进展的基础上,开展了染料敏化太阳能电池中光阴极的基础研究,并采用一步化学法可控制备了不同大小的CuInS2纳米晶,通过简单的化学液滴涂布法制备了薄膜太阳能电池,并测试了其光学及电化学性能,主要内容如下：
(1)研究了NiPt薄膜作为染料敏化太阳能电池光阴极的行为。采用化学镀法在导电FTO玻璃基底上首先沉积一层Ni膜,后通过氧化还原法制备NiPt薄膜,改变不同的反应时间制备得到不同载铂量的Ni1-xPtx(x=0,0.02,0.04,0.06,0.08)膜。研究显示Ni0.94Pt0.06膜的载铂量为5.13 gg/cm2,作为光阴极表现出对I3-的高催化性能,高光反射和高的电荷传输性能,提高了电池的光电转换效率。使用Ni0.94Pt0.06膜作光阴极制备的染料敏化太阳能电池获得了8.21%的光电转化效率,高于传统的使用热分解得到的Pt光阴极的电池效率(7.73%),并且此类电池的稳定性较好。结果表明NiPt膜对于低价高效大面积制备染料敏化太阳能电池的光阴极探索具有一定的意义。
(2)研究了高比表面积微孔碳作为染料敏化太阳能电池光阴极的行为。使用玉米杆制备了廉价的高比表面积微孔碳,将其取代铂光阴极,测试了其电化学性能。结果表明以微孔碳为活性材料,Vulcan XC-72做导电剂,TiO2为粘结剂的光阴极具有高的催化性能。以微孔碳为活性材料的光阴极的染料敏化太阳能电池在AM1.5(100 mW cm-2)的光照下具有7.36%的转换效率,与使用铂作光阴极的太阳能电池的转换效率相当。其开路电压达到了798 mV,比使用铂作光阴极的太阳能电池的电压高约60 mV。使用高比表面积碳作为光阴极,避免了贵金属Pt的使用,对于降低染料敏化太阳能电池的制作成本有着重要的实际意义。
(3)研究了CuInS2纳米晶的制备及其光电应用。使用油酸铜,油酸铟和硫粉作为反应物在油酸和油胺的混合溶剂中采用一步反应化学法可控制备了单分散的2-10nm CuInS2纳米晶,讨论了油胺作为还原剂和包覆剂对于产物大小的影响。产物的紫外可见吸收和荧光光谱表明所制备的产物具有量子尺寸效应。同时,还采用相同的方法合成了CuIn(S,Se1-x)2 (x=0,0.3,0.5,0.7)和AgInS2纳米晶,测试表明所得化合物都是纯相,颗粒大小约为10 nm。利用化学液滴涂布法制备了新型纳米晶太阳能电池(Au/CuInS2纳米晶/TiO2纳米棒阵列/FTO),通过优化条件,所制备的薄膜太阳能电池在AM 1.5(100 mW cm-2)光强下达到了0.21%的光电转换效率,表明这类纳米晶材料具有低价薄膜太阳能电池的潜在优势。
(4)探索了新型结构的太阳能电池。采用简单的溶剂热法直接在导电FTO玻璃和丝网印刷的Ti02膜上沉积一层CuInS2膜(CuInS2/FTO和CuInS2/TiO2/FTO),研究结果表明FTO玻璃上的CuInS2由微米球和纳米片组成,膜的厚度可以通过反应物的浓度控制在1-8μm之间,并且膜在400-850 nm间有很强的吸收,带隙随着Cu/In的比(1.2-0.9)调节为1.45-1.61 eV。TiO2基底上的CuInS2膜是由纳米片组成。此外,还评价了这两种膜的光电性能,经过热处理后,所组装的电池Ag/CdS/CuInS2/FTO, Au/CuInS2/TiO2/FTO在AM1.5(100 mWcm-2)的光强下分别达到了0.33%和0.29%的光电转换效率。
Solar cells, as a way to replace energy for sustainable development, are developing rapidly in recent years, due to their cleaning, cheapness, and high efficiency. However, solar cells have not been widely used in the long run because of their shortcomings of high fabrication cost and low conversion efficiency. Therefore, reducing the preparation cost and improving the conversion efficiency of solar cells are the key points in the future study. The development of novel low-cost solar cells, which include dye-sensitized solar cells (DSCs) and nanocrystal solar cells, has become a research hotspot.
The photocathode of DSCs is usually platinum-based films. However, its high price limits its commercial application. While, in thin film solar cells, CuInS2, as a direct band-gap semiconductor, possesses the advantages of a large absorption coefficient and appropriate band gap to match the solar spectrum. However, the film preparation, which needs high vacuum sophisticated equipment, and the composition and optical properties of CuInS2 are sensitive to the preparation process, both limiting their industrial application.
Therefore, based on the summarization of the progress of solar cells, this thesis carried out the basic research on the photocathode in DSCs, and shape-controlled CuInS2 nanocrystals with different sizes by a one-step chemical method and their application in a new type of thin film solar cells fabricated by a simple chemical drop-casting method. In addition, the optical properties of the as-prepared CuInS2 nanocrystals and the photovoltaic properties of the solar cells were investigated. The main content of this thesis is as follows:
(1) NiPt films as the photocathode in DSCs were investigated. Films of Ni1-xPtx (x=0,0.02,0.04,0.06,0.08) were deposited on FTO glass substrates by a chemical plating and oxidation-reducation method. The Pt loading in NiPt films could be controlled by the reaction time. The results showed that the Ni0.94Pt0.06 film with a Pt loading of 5.13μm/cm2 exhibited high catalytic performance toward triiodide reduction, high light reflectance, and low charge-transfer resistance, thereby enhanced the conversion efficiency of DSC. The DSC based on the Ni0.94Pt0.06 photocathode showed an overall conversion efficiency of 8.21%, which was higher than that of the DSC with a pure Pt photocathode obtained by conventional thermal decomposition (7.33%). Furthermore, the DSC based on the Ni0.94Pt0.06 photocathode showed good stability. The results showed that the Nio.94Pt0.06 photocathode is potential in the fabrication of DSCs with large scale and low cost.
(2) High surface area microporous carbon as the photocathode in DSCs was investigated. High-surface-area microporous carbon, replacing conventional Pt photocathode, was fabricated by cornstalks, and the photovoltaic characterization in DSCs was measured. The photocathode, which contained microporous carbon active material, Vulcan XC-72 carbon black conductive agent, and TiO2 binder photocathode, showed a low charge-transfer resistance of 1.32Ωcm2. The DSCs assembled with the MC film photocathode presented an overall conversion efficiency of 7.36% under AM1.5 (100 mW cm-2), which was comparable to that of the DSCs with Pt photocathode prepared by conventional thermal decomposition. Especially, the open-circuit voltage reached 798 mV, which was increased by 60 mV compared to that of pure Pt photocathode. The use of high surface area carbon as a photocathode played an important role in the reduction of the fabrication cost of DSCs due to the avoiding use of precious metal Pt.
(3) CuInS2 nanocrystals with different sizes and their photovoltaic application were investigated. Well-defined and monodisperse CuInS2 with sizes ranging from 2-10 nm were synthesized via a facile one-pot chemical approach using Cu-oleate, In-oleate, sulfur as the reactants in oleic acid and oleylamine media. The effects of oleylamine, which acted as a reductant and the capping agent, on the size and purity of the products were thoroughly investigated. UV-vis absorption and fluorescence spectra measurements showed that the products had the property of quantum confined effect. In addition, other types of pure ternary chalcogenide cmopounds CuIn(SxSe1-x)2(x=0,0.3,0.5,0.7), and AgInS2 nanocrystals with size of about 10 nm were synthesized by using the same method. Moreover, the as-prepared CuInS2 nanocrystals were assembled as a simple prototype thin-film solar cell (Au/CuInS2 nanocrystals/TiO2 nanorod arrays/FTO) by a facile drop-casting method. The obtained thin-film solar cells reached an overall conversion efficiency of 0.21% under AM1.5 (100 mW cm-2) illumination by optimizing the experimental conditions, indicating that the nanocrystals had potential application in thin film solar cells with low cost.
(4) A novel solar cell was explored. Two thin films (CuInS2/FTO and CuInS2/TiO2/FTO) were deposited by a facile solvothermal method. The results showed that the CuInS2 films deposited on the FTO conductive glass substrates were composed of nanoplates and microspheres. The thickness of the CuInS2/FTO films can be adjusted from 1-8μm by controlling the solution concentration of the reactants. While, the prepared 10μm thick CuInS2 film on the TiO2 film substrate consisted of nanoplates. The UV-vis absorption spectra revealed that the CuInS2 thin films had a strong absorption around 400-850 nm and the band-gap energy was tunable in the range of 1.45-1.61 eV with the variation of Cu/In ratio from 1.20 to 0.90. Furthermore, two types of thin film solar cells, which possessed separately the top-down composition of Ag/CdS/CuInS2/FTO and Au/CuInS2/TiO2/FTO were fabricated after heat-treatment. Under AM 1.5 irradiation (100mW cm-2), the conversion efficiencies of the as-prepared Ag/CdS/CuInS2/FTO and Au/CuInS2/TiO2/FTO were 0.33% and 0.29%, respectively.
在染料敏化太阳能电池中,多用贵金属铂作为光阴极,但其昂贵的价格限制了它的商业化应用。在薄膜太阳能电池中,CuInS2具有吸收系数大,禁带宽度与太阳光谱匹配,直接带隙半导体等优点,但使用高真空镀膜设备以及CuInS2材料的成分和光电特性对工艺过程的敏感限制了其产业化应用。
本论文在总结太阳能电池研究进展的基础上,开展了染料敏化太阳能电池中光阴极的基础研究,并采用一步化学法可控制备了不同大小的CuInS2纳米晶,通过简单的化学液滴涂布法制备了薄膜太阳能电池,并测试了其光学及电化学性能,主要内容如下：
(1)研究了NiPt薄膜作为染料敏化太阳能电池光阴极的行为。采用化学镀法在导电FTO玻璃基底上首先沉积一层Ni膜,后通过氧化还原法制备NiPt薄膜,改变不同的反应时间制备得到不同载铂量的Ni1-xPtx(x=0,0.02,0.04,0.06,0.08)膜。研究显示Ni0.94Pt0.06膜的载铂量为5.13 gg/cm2,作为光阴极表现出对I3-的高催化性能,高光反射和高的电荷传输性能,提高了电池的光电转换效率。使用Ni0.94Pt0.06膜作光阴极制备的染料敏化太阳能电池获得了8.21%的光电转化效率,高于传统的使用热分解得到的Pt光阴极的电池效率(7.73%),并且此类电池的稳定性较好。结果表明NiPt膜对于低价高效大面积制备染料敏化太阳能电池的光阴极探索具有一定的意义。
(2)研究了高比表面积微孔碳作为染料敏化太阳能电池光阴极的行为。使用玉米杆制备了廉价的高比表面积微孔碳,将其取代铂光阴极,测试了其电化学性能。结果表明以微孔碳为活性材料,Vulcan XC-72做导电剂,TiO2为粘结剂的光阴极具有高的催化性能。以微孔碳为活性材料的光阴极的染料敏化太阳能电池在AM1.5(100 mW cm-2)的光照下具有7.36%的转换效率,与使用铂作光阴极的太阳能电池的转换效率相当。其开路电压达到了798 mV,比使用铂作光阴极的太阳能电池的电压高约60 mV。使用高比表面积碳作为光阴极,避免了贵金属Pt的使用,对于降低染料敏化太阳能电池的制作成本有着重要的实际意义。
(3)研究了CuInS2纳米晶的制备及其光电应用。使用油酸铜,油酸铟和硫粉作为反应物在油酸和油胺的混合溶剂中采用一步反应化学法可控制备了单分散的2-10nm CuInS2纳米晶,讨论了油胺作为还原剂和包覆剂对于产物大小的影响。产物的紫外可见吸收和荧光光谱表明所制备的产物具有量子尺寸效应。同时,还采用相同的方法合成了CuIn(S,Se1-x)2 (x=0,0.3,0.5,0.7)和AgInS2纳米晶,测试表明所得化合物都是纯相,颗粒大小约为10 nm。利用化学液滴涂布法制备了新型纳米晶太阳能电池(Au/CuInS2纳米晶/TiO2纳米棒阵列/FTO),通过优化条件,所制备的薄膜太阳能电池在AM 1.5(100 mW cm-2)光强下达到了0.21%的光电转换效率,表明这类纳米晶材料具有低价薄膜太阳能电池的潜在优势。
(4)探索了新型结构的太阳能电池。采用简单的溶剂热法直接在导电FTO玻璃和丝网印刷的Ti02膜上沉积一层CuInS2膜(CuInS2/FTO和CuInS2/TiO2/FTO),研究结果表明FTO玻璃上的CuInS2由微米球和纳米片组成,膜的厚度可以通过反应物的浓度控制在1-8μm之间,并且膜在400-850 nm间有很强的吸收,带隙随着Cu/In的比(1.2-0.9)调节为1.45-1.61 eV。TiO2基底上的CuInS2膜是由纳米片组成。此外,还评价了这两种膜的光电性能,经过热处理后,所组装的电池Ag/CdS/CuInS2/FTO, Au/CuInS2/TiO2/FTO在AM1.5(100 mWcm-2)的光强下分别达到了0.33%和0.29%的光电转换效率。
Solar cells, as a way to replace energy for sustainable development, are developing rapidly in recent years, due to their cleaning, cheapness, and high efficiency. However, solar cells have not been widely used in the long run because of their shortcomings of high fabrication cost and low conversion efficiency. Therefore, reducing the preparation cost and improving the conversion efficiency of solar cells are the key points in the future study. The development of novel low-cost solar cells, which include dye-sensitized solar cells (DSCs) and nanocrystal solar cells, has become a research hotspot.
The photocathode of DSCs is usually platinum-based films. However, its high price limits its commercial application. While, in thin film solar cells, CuInS2, as a direct band-gap semiconductor, possesses the advantages of a large absorption coefficient and appropriate band gap to match the solar spectrum. However, the film preparation, which needs high vacuum sophisticated equipment, and the composition and optical properties of CuInS2 are sensitive to the preparation process, both limiting their industrial application.
Therefore, based on the summarization of the progress of solar cells, this thesis carried out the basic research on the photocathode in DSCs, and shape-controlled CuInS2 nanocrystals with different sizes by a one-step chemical method and their application in a new type of thin film solar cells fabricated by a simple chemical drop-casting method. In addition, the optical properties of the as-prepared CuInS2 nanocrystals and the photovoltaic properties of the solar cells were investigated. The main content of this thesis is as follows:
(1) NiPt films as the photocathode in DSCs were investigated. Films of Ni1-xPtx (x=0,0.02,0.04,0.06,0.08) were deposited on FTO glass substrates by a chemical plating and oxidation-reducation method. The Pt loading in NiPt films could be controlled by the reaction time. The results showed that the Ni0.94Pt0.06 film with a Pt loading of 5.13μm/cm2 exhibited high catalytic performance toward triiodide reduction, high light reflectance, and low charge-transfer resistance, thereby enhanced the conversion efficiency of DSC. The DSC based on the Ni0.94Pt0.06 photocathode showed an overall conversion efficiency of 8.21%, which was higher than that of the DSC with a pure Pt photocathode obtained by conventional thermal decomposition (7.33%). Furthermore, the DSC based on the Ni0.94Pt0.06 photocathode showed good stability. The results showed that the Nio.94Pt0.06 photocathode is potential in the fabrication of DSCs with large scale and low cost.
(2) High surface area microporous carbon as the photocathode in DSCs was investigated. High-surface-area microporous carbon, replacing conventional Pt photocathode, was fabricated by cornstalks, and the photovoltaic characterization in DSCs was measured. The photocathode, which contained microporous carbon active material, Vulcan XC-72 carbon black conductive agent, and TiO2 binder photocathode, showed a low charge-transfer resistance of 1.32Ωcm2. The DSCs assembled with the MC film photocathode presented an overall conversion efficiency of 7.36% under AM1.5 (100 mW cm-2), which was comparable to that of the DSCs with Pt photocathode prepared by conventional thermal decomposition. Especially, the open-circuit voltage reached 798 mV, which was increased by 60 mV compared to that of pure Pt photocathode. The use of high surface area carbon as a photocathode played an important role in the reduction of the fabrication cost of DSCs due to the avoiding use of precious metal Pt.
(3) CuInS2 nanocrystals with different sizes and their photovoltaic application were investigated. Well-defined and monodisperse CuInS2 with sizes ranging from 2-10 nm were synthesized via a facile one-pot chemical approach using Cu-oleate, In-oleate, sulfur as the reactants in oleic acid and oleylamine media. The effects of oleylamine, which acted as a reductant and the capping agent, on the size and purity of the products were thoroughly investigated. UV-vis absorption and fluorescence spectra measurements showed that the products had the property of quantum confined effect. In addition, other types of pure ternary chalcogenide cmopounds CuIn(SxSe1-x)2(x=0,0.3,0.5,0.7), and AgInS2 nanocrystals with size of about 10 nm were synthesized by using the same method. Moreover, the as-prepared CuInS2 nanocrystals were assembled as a simple prototype thin-film solar cell (Au/CuInS2 nanocrystals/TiO2 nanorod arrays/FTO) by a facile drop-casting method. The obtained thin-film solar cells reached an overall conversion efficiency of 0.21% under AM1.5 (100 mW cm-2) illumination by optimizing the experimental conditions, indicating that the nanocrystals had potential application in thin film solar cells with low cost.
(4) A novel solar cell was explored. Two thin films (CuInS2/FTO and CuInS2/TiO2/FTO) were deposited by a facile solvothermal method. The results showed that the CuInS2 films deposited on the FTO conductive glass substrates were composed of nanoplates and microspheres. The thickness of the CuInS2/FTO films can be adjusted from 1-8μm by controlling the solution concentration of the reactants. While, the prepared 10μm thick CuInS2 film on the TiO2 film substrate consisted of nanoplates. The UV-vis absorption spectra revealed that the CuInS2 thin films had a strong absorption around 400-850 nm and the band-gap energy was tunable in the range of 1.45-1.61 eV with the variation of Cu/In ratio from 1.20 to 0.90. Furthermore, two types of thin film solar cells, which possessed separately the top-down composition of Ag/CdS/CuInS2/FTO and Au/CuInS2/TiO2/FTO were fabricated after heat-treatment. Under AM 1.5 irradiation (100mW cm-2), the conversion efficiencies of the as-prepared Ag/CdS/CuInS2/FTO and Au/CuInS2/TiO2/FTO were 0.33% and 0.29%, respectively.
引文
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