NiO/TiO_2光电极与染料敏化光阳极的光电化学特性研究
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摘要
利用太阳光发电和制氢是根本解决人类未来能源需求和环保问题的一个重要途径,也是纳米科技领域的前沿热点之一。本论文主要针对光解水制氢及染料敏化太阳电池领域中,提高光电化学性能和光电转换效率的关键问题展开研究。主要内容如下:
(1)以HF+NaH_2PO_4水溶液为电解液,通过阳极氧化过程在钛箔表面制备出TiO_2纳米管阵列;采用化学镀镍并结合空气中热处理过程,在TiO_2纳米管阵列表面复合生长出NiO纳米颗粒层。这种新颖的NiO/TiO_2光电极相对于TiO_2纳米管阵列表现出显著的光吸收红移,并在可见光范围光吸收明显增强。对引起红移和可见光范围的光吸收增强的可能机理进行了讨论。
(2)在AM 1.5G照射下,NiO/TiO_2光电极的短路电流为2.82 mA/cm2,开路电压为0.755 V,光电转化效率为1.41%。NiO/TiO_2光电极表现出远比TiO_2更好的光电化学性质,其机理在于,NiO/TiO_2光电极有较宽的光吸收范围,使更多的光子能被利用;而且在NiO与TiO_2复合界面区域,形成了很多微型的p-n结,有利于在光阳极中形成的光生电子-空穴对的高效率分离,并抑制光生电子-空穴对的重新复合。
(3)对比了相同电子给体相同共轭π结构不同电子受体的三种染料的电化学能带、光谱吸收和电物理特性,发现染料分子结构中的电子受体对HOMO位置影响不大,主要影响LUMO的位置。而染料的HOMO和LUMO位置进一步影响到器件的电荷输运特性。采用腈基丙烯酸做的电子受体的染料Dye1表现出较好的光电特性。研究了相关DSC器件光电性质随温度的变化规律。
(4)用丝网印刷将粒径为15-20 nm的ZnO纳米颗粒印刷在FTO导电玻璃上,350℃退火得到ZnO薄膜电极来取代传统500℃退火的TiO_2薄膜电极。由这种新颖的电极通过C106敏化得到的DSC器件具有较优异的光电转换性质,光电池效率为5.26%。
Nowadays, one of man’s endeavors is to cope with the energy crisis and environmental pollution for the sustainable development of human society, in which energy is vital. Solar and hydrogen energy are considered as the‘Green energy’which is most likely to gradually replace fossil fuels. Currently, the conversion of solar to electrical energy and the hydrogen production from water splitting using solar light are the two most promising research directions.
Developing the efficient, low-cost and practical photoelectrode is absolutely vital for hydrogen production from water. TiO_2-based nanostructure semiconductors have been extensively studied due to their excellent chemical stability, nontoxicity, low-cost, and high photocatalytic activities. They were considered as particularly versatile materials with technological application prospects in solar cell and hydrogen production from water photolysis, and more. Especially over the past few years, highly ordered, vertically oriented TiO_2 nanotube arrays fabricated by electrochemical anodization constitute a material architecture that offers a large specific surface area, favorable surface chemistry and narrow distribution of diffusion path not only for entering the tubular depth but also for species to be transported through the tube wall, have attracted tremendous efforts. However the low efficient due to the narrow photo absorption, it is urge to expand the reponse spectrum. Based on the previouse researches, we functionalized the self-organized TiO_2 nanotube arrays with 200 nm NiO nanopartice layer by electroless plating and annealing. Compared with the TiO_2 electrode, this noval NiO/TiO_2 junction electrode demonstrated red-shift photoresponse. The short-circuit photocurrent density (Jsc), open-circuit photovoltage (Voc) of NiO/TiO_2 junction electrode under an irradiance of AM 1.5G full sunlight are 2.82 mA cm~(-2), 755 mV, yielding an overall conversion efficiency (η) of 1.41%.
A large amount of research and development efforts has been made to the mesoscopic dye-sensitized solar cell (DSC) ever since the seminal demonstration of its feasibility as a cost-effective photovoltaic technology. The most critical issues are designing dye molecul for high performance DSC device and comprehend the mechanism of device running. Three organic D-π-A dyes with different acceptors such as cyanoacrylic acid,quionolinylcarboxylic acid and phthalic acid have been prepared in combination with the dihexyloxy-substituted triphenylamine donor and the 2,2’-bis(3,4-ethylenedioxythiophene)π-conjugated linker. We have studied the influence of adsorbent units on spectral responses, energy levels, photocurrents, photovoltages and transient photoelectrical decay measurements. Temperature-dependent electrical impedance experiments have also been studied. Emporldering low-temperature annealed semicomductor to
replace traditional high-temperature annealed TiO_2 layer is a hot issue for flexible DSC research. In this thesis, a screen-printed layer of interconnected ZnO nanopaticles was synthesized by hot-solvent method. the short-circuit photocurrent density (Jsc), open-circuit photovoltage (Voc), fill factor (FF) and conversion efficiency (η) of DSC device based on ZnO electrode under an irradiance of AM 1.5G full sunlight are 12.18 mA cm~(-2)、636 mV,0.636,5.26%。
(1)以HF+NaH_2PO_4水溶液为电解液,通过阳极氧化过程在钛箔表面制备出TiO_2纳米管阵列;采用化学镀镍并结合空气中热处理过程,在TiO_2纳米管阵列表面复合生长出NiO纳米颗粒层。这种新颖的NiO/TiO_2光电极相对于TiO_2纳米管阵列表现出显著的光吸收红移,并在可见光范围光吸收明显增强。对引起红移和可见光范围的光吸收增强的可能机理进行了讨论。
(2)在AM 1.5G照射下,NiO/TiO_2光电极的短路电流为2.82 mA/cm2,开路电压为0.755 V,光电转化效率为1.41%。NiO/TiO_2光电极表现出远比TiO_2更好的光电化学性质,其机理在于,NiO/TiO_2光电极有较宽的光吸收范围,使更多的光子能被利用;而且在NiO与TiO_2复合界面区域,形成了很多微型的p-n结,有利于在光阳极中形成的光生电子-空穴对的高效率分离,并抑制光生电子-空穴对的重新复合。
(3)对比了相同电子给体相同共轭π结构不同电子受体的三种染料的电化学能带、光谱吸收和电物理特性,发现染料分子结构中的电子受体对HOMO位置影响不大,主要影响LUMO的位置。而染料的HOMO和LUMO位置进一步影响到器件的电荷输运特性。采用腈基丙烯酸做的电子受体的染料Dye1表现出较好的光电特性。研究了相关DSC器件光电性质随温度的变化规律。
(4)用丝网印刷将粒径为15-20 nm的ZnO纳米颗粒印刷在FTO导电玻璃上,350℃退火得到ZnO薄膜电极来取代传统500℃退火的TiO_2薄膜电极。由这种新颖的电极通过C106敏化得到的DSC器件具有较优异的光电转换性质,光电池效率为5.26%。
Nowadays, one of man’s endeavors is to cope with the energy crisis and environmental pollution for the sustainable development of human society, in which energy is vital. Solar and hydrogen energy are considered as the‘Green energy’which is most likely to gradually replace fossil fuels. Currently, the conversion of solar to electrical energy and the hydrogen production from water splitting using solar light are the two most promising research directions.
Developing the efficient, low-cost and practical photoelectrode is absolutely vital for hydrogen production from water. TiO_2-based nanostructure semiconductors have been extensively studied due to their excellent chemical stability, nontoxicity, low-cost, and high photocatalytic activities. They were considered as particularly versatile materials with technological application prospects in solar cell and hydrogen production from water photolysis, and more. Especially over the past few years, highly ordered, vertically oriented TiO_2 nanotube arrays fabricated by electrochemical anodization constitute a material architecture that offers a large specific surface area, favorable surface chemistry and narrow distribution of diffusion path not only for entering the tubular depth but also for species to be transported through the tube wall, have attracted tremendous efforts. However the low efficient due to the narrow photo absorption, it is urge to expand the reponse spectrum. Based on the previouse researches, we functionalized the self-organized TiO_2 nanotube arrays with 200 nm NiO nanopartice layer by electroless plating and annealing. Compared with the TiO_2 electrode, this noval NiO/TiO_2 junction electrode demonstrated red-shift photoresponse. The short-circuit photocurrent density (Jsc), open-circuit photovoltage (Voc) of NiO/TiO_2 junction electrode under an irradiance of AM 1.5G full sunlight are 2.82 mA cm~(-2), 755 mV, yielding an overall conversion efficiency (η) of 1.41%.
A large amount of research and development efforts has been made to the mesoscopic dye-sensitized solar cell (DSC) ever since the seminal demonstration of its feasibility as a cost-effective photovoltaic technology. The most critical issues are designing dye molecul for high performance DSC device and comprehend the mechanism of device running. Three organic D-π-A dyes with different acceptors such as cyanoacrylic acid,quionolinylcarboxylic acid and phthalic acid have been prepared in combination with the dihexyloxy-substituted triphenylamine donor and the 2,2’-bis(3,4-ethylenedioxythiophene)π-conjugated linker. We have studied the influence of adsorbent units on spectral responses, energy levels, photocurrents, photovoltages and transient photoelectrical decay measurements. Temperature-dependent electrical impedance experiments have also been studied. Emporldering low-temperature annealed semicomductor to
replace traditional high-temperature annealed TiO_2 layer is a hot issue for flexible DSC research. In this thesis, a screen-printed layer of interconnected ZnO nanopaticles was synthesized by hot-solvent method. the short-circuit photocurrent density (Jsc), open-circuit photovoltage (Voc), fill factor (FF) and conversion efficiency (η) of DSC device based on ZnO electrode under an irradiance of AM 1.5G full sunlight are 12.18 mA cm~(-2)、636 mV,0.636,5.26%。
引文
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