染料敏化太阳能电池ZnO阳极的修饰与光电性能的研究
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摘要
染料敏化太阳能电池(DSSC)的光电转换研究已经成为国际性的热点课题。本研究以ZnO为染料敏化太阳能电池的光阳极，通过掺杂和共敏化两种方法分别对ZnO进行改性与修饰，并以此降低ZnO光阳极染料敏化太阳能电池的成本。本研究从单掺杂、双掺杂和共敏化三个方面对比改性修饰后的ZnO的性质以及染料敏化太阳能电池的光电性能，进而研究掺杂和共敏化对染料敏化太阳能电池光电性能的影响。
以ZnO粉体为初始反应物，氨气为掺杂源，在自制的反应容器中制备N掺杂ZnO，研究了N掺杂ZnO的合成条件与ZnO禁带带宽和光电转换效率之间的关系。通过改变氨气压强、煅烧温度和煅烧时间得到不同N掺杂量的ZnO，发现N掺杂ZnO的禁带宽度有不同程度的窄化，并通过改变N掺杂条件实现了对ZnO禁带宽度的可控调节。实验的N掺杂反应条件为：氨气压强0.6～1.2MPa，煅烧温度450～750℃，煅烧时间12～72h。实验结果表明，随着氨气压强、煅烧温度和时间的增加，N掺杂含量逐渐增加，ZnO的禁带宽度逐渐窄化，染料敏化太阳能电池光电转换效率随之增加。采用X射线粉末衍射、紫外-可见吸收光谱、X射线光电子能谱、表面光电压谱和瞬态光谱对N掺杂ZnO的晶体结构、掺杂价态、光学性质以及表面光生电子-空穴的性质进行了分析，研究发现：N掺杂到ZnO晶格中形成六方纤锌矿结构，N掺杂有效地降低了禁带宽度和导带能级，有利于电子-空穴对的生成，增加了载流子的传输，为提高电池性能奠定了基础。
采用低温溶液法对ZnO进行了N掺杂，并与高温煅烧掺杂方法进行对比研究。在低温溶液法中N的掺杂源为氨水，研究了溶液pH值对掺杂效果的影响。结果表明，随着溶液pH的增加，N掺杂含量增加，但溶液pH=7时，光电转换效率最高。实验还发现：低温溶液法制备的N掺杂ZnO的光电性能优于高温煅烧法。
采用Materials studio的Castep模块对N掺杂ZnO进行理论计算，对模拟的能带结构、态密度和光学性质进行计算分析。认为N掺杂产生的N2p轨道在价带顶和Zn3d轨道杂化，使得价带顶上移并同时引起导带底下降，窄化禁带，为N掺杂减小禁带宽度、降低导带底提供了一定的理论依据。
对ZnO进行了Pr和N元素的双掺杂。实验结果表明：Pr-N双掺杂ZnO为六方纤锌矿结构，禁带宽度和导带能级都有较大程度的下降，导致紫外-可见吸收光谱的吸收带边红移至可见光区，光吸收增强的同时也增加了导带内电子的注入效率，Pr-N双掺杂比N掺杂更能有效提高电池光电转换效率，光电转换效率最大达5.2%，较空白ZnO电池提高了100%。
以空白ZnO为光阳极，对电池染料的太阳光谱吸收谱带进行补充，采用配合物与N719对光阳极进行共敏化，填补电池在太阳光谱紫外高能光区的吸收空白，拓宽电池对太阳光谱的吸收响应范围。选取吡啶双亚胺类过渡金属配合物、含邻菲罗啉类过渡金属配合物和吡啶二甲酸类稀土金属配合物进行共敏化，单色光光电转换效率(IPCE)揭示共敏化通过提高电池在紫外光区的吸收来提高电池器件的光电转换效率。电化学循环伏安和紫外-可见吸收光谱联用表明配合物敏化剂能有效地进行电子的激发和注入，同时顺利被电解液还原。采用等效电路对交流阻抗进行模拟，分析电池阳极/染料/电解液界面的电子注入和传输性质，结果表明配合物、电池阳极和电解液之间具有很好的能级匹配，在阳极/染料/电解液界面电子能够顺利的注入和传输，共敏化能有效提高电池光电转换效率，具有较大共轭体系的配合物更有利于电池性能的提高。
本文通过阳极改性和染料共敏化等途径提高了ZnO染料敏化太阳能电池的光电性能，为其实际应用打下了一定的基础。
The dye-sensitized solar cell (DSSC) is a focus in the field of photovoltaicstudies. The research focus on ZnO photoanode of DSSC. In this work, doping andco-sensitizing are used to modify ZnO photoanode and reduce the costs of DSSC.The properties of modified-ZnO and photovolatic performance of DSSC is superiorcontrast to that of pure ZnO and DSSC based on pure ZnO. The influence of dopingand co-sensitizing on photovolatic performance are studied.
ZnO powders were used and NH3gas was used as dopants. N-doped ZnO wasprepared in self-designed devices. The relationship between preparation condition ofN doped ZnO, band gap of N doped ZnO, and conversion efficiency of DSSC wasinvestigated. The different N doping concentration of ZnO was obtained by varyingNH3gas presure, annealing temperature, and annealing time. The band gap of ZnOwas narrowed by N doping and the controlled band gap of ZnO was achieved byvarying the doping conditions. The NH3gas pressure was from0.6MPa to1.2MPa,the reaction temperature was from450℃to750℃, reaction time wasfrom12h to72h. The results shows that N doping concentration and the narrowing of band gapincreased with NH3gas presure, annealing temperature, and annealing time, theconversion efficiency of DSSC increase correspondingly. The structure andcompositions of the material were characterized by X-ray diffraction analysis (XRD)and X-ray photoelectron spectroscopy (XPS). UV-visible absorption spectroscopy(UV-vis), surface photovoltage spectroscopy (SPS), and the transient photovoltage(TPV) were used to characterize the optical property, performance of photoproducedelectron-hole separation, transfer, and recombination. It was found that N atomswere doped into the lattice of ZnO crystals, N doping effectively reduced the bandgap and energy level of conduction band, produced electron-hole pairs, andenhenced charge carriers transport. This established the foundation for improvingthe performances of DSSC.
The solution method for N doping was compared with the annealing method.The ammonia acted as the source of N dopant in the solution method. The effect ofthe pH of the solution on N doping was studied. The results showed N dopingconcentration increase with pH value of the solution. The conversion efficiency ofDSSC was highest when pH value was7. The photovolatic performances of N dopedZnO by solution method was better than that of annealing method.
The band structure, density of states, and optical perporty of N doped ZnOwere calculated by Castep of Materials Studio software. The results indicated the topof the valence band for N-doped ZnO was composed of N2p orbital followed by Zn 3d orbital. The Zn3d and N2p electrons in the upper valence band form the p-drepulsion, led to the uplift of the valence band top and narrowing of the band gap.The calculation results conformed shift conduction band and band gap narrowing byN doping.
The Pr-N co-doped ZnO was prepared. The Pr-N co-doped ZnO still possesseda hexagonal wurtzite structure. The co-doping of Pr and N significantly influencethe optical properties of ZnO. UV-visible absorption spectroscopy (UV-vis) revealedthat co-doping of Pr and N led to a red shift of the absorption edge of ZnO andnarrowing of band gap. The conversion efficiency of Pr-N co-doped ZnO show thehighest conversion efficiency of DSSC of5.2%, an onefold increase compared tothat of pure ZnO.
The metal complexes and N719co-sensitized ZnO photoelectrode showbroadened absorption band of DSSC and extended the response of DSSC. The metaltypes of complexes were transition metal complexes with2,6-bis(imino)pyridylligands, transition metal complexes with phen, and lanthanide metal complexesconstructed by pyridine-2,6-dicarboxylic acid ligands. IPCE revealed thatco-sensitization improved the conversion of DSSC by improving the UV lightabsorption and extended absorption response of DSSC to UV light region. Theperformance of electron injection and transport in photoanode/dye/electrolyteinterface was investigated by AC impedence and equivalent circuit. The resultsshowed that electrons were more easily injected and transferred in the interface ofphotoanode/dye/electrolyte, so that the conversion efficiency of DSSC wasimproved. The results showed that the metal complexe with large conjugated systemwas positive for improving the performance of the DSSC.
In this paper, modification of photoanodes and co-sensitizing of dyes are usedto improve the photovolatic performance of DSSC based on ZnO photoanode, whichwill find wide provides potential applications in devices.
以ZnO粉体为初始反应物，氨气为掺杂源，在自制的反应容器中制备N掺杂ZnO，研究了N掺杂ZnO的合成条件与ZnO禁带带宽和光电转换效率之间的关系。通过改变氨气压强、煅烧温度和煅烧时间得到不同N掺杂量的ZnO，发现N掺杂ZnO的禁带宽度有不同程度的窄化，并通过改变N掺杂条件实现了对ZnO禁带宽度的可控调节。实验的N掺杂反应条件为：氨气压强0.6～1.2MPa，煅烧温度450～750℃，煅烧时间12～72h。实验结果表明，随着氨气压强、煅烧温度和时间的增加，N掺杂含量逐渐增加，ZnO的禁带宽度逐渐窄化，染料敏化太阳能电池光电转换效率随之增加。采用X射线粉末衍射、紫外-可见吸收光谱、X射线光电子能谱、表面光电压谱和瞬态光谱对N掺杂ZnO的晶体结构、掺杂价态、光学性质以及表面光生电子-空穴的性质进行了分析，研究发现：N掺杂到ZnO晶格中形成六方纤锌矿结构，N掺杂有效地降低了禁带宽度和导带能级，有利于电子-空穴对的生成，增加了载流子的传输，为提高电池性能奠定了基础。
采用低温溶液法对ZnO进行了N掺杂，并与高温煅烧掺杂方法进行对比研究。在低温溶液法中N的掺杂源为氨水，研究了溶液pH值对掺杂效果的影响。结果表明，随着溶液pH的增加，N掺杂含量增加，但溶液pH=7时，光电转换效率最高。实验还发现：低温溶液法制备的N掺杂ZnO的光电性能优于高温煅烧法。
采用Materials studio的Castep模块对N掺杂ZnO进行理论计算，对模拟的能带结构、态密度和光学性质进行计算分析。认为N掺杂产生的N2p轨道在价带顶和Zn3d轨道杂化，使得价带顶上移并同时引起导带底下降，窄化禁带，为N掺杂减小禁带宽度、降低导带底提供了一定的理论依据。
对ZnO进行了Pr和N元素的双掺杂。实验结果表明：Pr-N双掺杂ZnO为六方纤锌矿结构，禁带宽度和导带能级都有较大程度的下降，导致紫外-可见吸收光谱的吸收带边红移至可见光区，光吸收增强的同时也增加了导带内电子的注入效率，Pr-N双掺杂比N掺杂更能有效提高电池光电转换效率，光电转换效率最大达5.2%，较空白ZnO电池提高了100%。
以空白ZnO为光阳极，对电池染料的太阳光谱吸收谱带进行补充，采用配合物与N719对光阳极进行共敏化，填补电池在太阳光谱紫外高能光区的吸收空白，拓宽电池对太阳光谱的吸收响应范围。选取吡啶双亚胺类过渡金属配合物、含邻菲罗啉类过渡金属配合物和吡啶二甲酸类稀土金属配合物进行共敏化，单色光光电转换效率(IPCE)揭示共敏化通过提高电池在紫外光区的吸收来提高电池器件的光电转换效率。电化学循环伏安和紫外-可见吸收光谱联用表明配合物敏化剂能有效地进行电子的激发和注入，同时顺利被电解液还原。采用等效电路对交流阻抗进行模拟，分析电池阳极/染料/电解液界面的电子注入和传输性质，结果表明配合物、电池阳极和电解液之间具有很好的能级匹配，在阳极/染料/电解液界面电子能够顺利的注入和传输，共敏化能有效提高电池光电转换效率，具有较大共轭体系的配合物更有利于电池性能的提高。
本文通过阳极改性和染料共敏化等途径提高了ZnO染料敏化太阳能电池的光电性能，为其实际应用打下了一定的基础。
The dye-sensitized solar cell (DSSC) is a focus in the field of photovoltaicstudies. The research focus on ZnO photoanode of DSSC. In this work, doping andco-sensitizing are used to modify ZnO photoanode and reduce the costs of DSSC.The properties of modified-ZnO and photovolatic performance of DSSC is superiorcontrast to that of pure ZnO and DSSC based on pure ZnO. The influence of dopingand co-sensitizing on photovolatic performance are studied.
ZnO powders were used and NH3gas was used as dopants. N-doped ZnO wasprepared in self-designed devices. The relationship between preparation condition ofN doped ZnO, band gap of N doped ZnO, and conversion efficiency of DSSC wasinvestigated. The different N doping concentration of ZnO was obtained by varyingNH3gas presure, annealing temperature, and annealing time. The band gap of ZnOwas narrowed by N doping and the controlled band gap of ZnO was achieved byvarying the doping conditions. The NH3gas pressure was from0.6MPa to1.2MPa,the reaction temperature was from450℃to750℃, reaction time wasfrom12h to72h. The results shows that N doping concentration and the narrowing of band gapincreased with NH3gas presure, annealing temperature, and annealing time, theconversion efficiency of DSSC increase correspondingly. The structure andcompositions of the material were characterized by X-ray diffraction analysis (XRD)and X-ray photoelectron spectroscopy (XPS). UV-visible absorption spectroscopy(UV-vis), surface photovoltage spectroscopy (SPS), and the transient photovoltage(TPV) were used to characterize the optical property, performance of photoproducedelectron-hole separation, transfer, and recombination. It was found that N atomswere doped into the lattice of ZnO crystals, N doping effectively reduced the bandgap and energy level of conduction band, produced electron-hole pairs, andenhenced charge carriers transport. This established the foundation for improvingthe performances of DSSC.
The solution method for N doping was compared with the annealing method.The ammonia acted as the source of N dopant in the solution method. The effect ofthe pH of the solution on N doping was studied. The results showed N dopingconcentration increase with pH value of the solution. The conversion efficiency ofDSSC was highest when pH value was7. The photovolatic performances of N dopedZnO by solution method was better than that of annealing method.
The band structure, density of states, and optical perporty of N doped ZnOwere calculated by Castep of Materials Studio software. The results indicated the topof the valence band for N-doped ZnO was composed of N2p orbital followed by Zn 3d orbital. The Zn3d and N2p electrons in the upper valence band form the p-drepulsion, led to the uplift of the valence band top and narrowing of the band gap.The calculation results conformed shift conduction band and band gap narrowing byN doping.
The Pr-N co-doped ZnO was prepared. The Pr-N co-doped ZnO still possesseda hexagonal wurtzite structure. The co-doping of Pr and N significantly influencethe optical properties of ZnO. UV-visible absorption spectroscopy (UV-vis) revealedthat co-doping of Pr and N led to a red shift of the absorption edge of ZnO andnarrowing of band gap. The conversion efficiency of Pr-N co-doped ZnO show thehighest conversion efficiency of DSSC of5.2%, an onefold increase compared tothat of pure ZnO.
The metal complexes and N719co-sensitized ZnO photoelectrode showbroadened absorption band of DSSC and extended the response of DSSC. The metaltypes of complexes were transition metal complexes with2,6-bis(imino)pyridylligands, transition metal complexes with phen, and lanthanide metal complexesconstructed by pyridine-2,6-dicarboxylic acid ligands. IPCE revealed thatco-sensitization improved the conversion of DSSC by improving the UV lightabsorption and extended absorption response of DSSC to UV light region. Theperformance of electron injection and transport in photoanode/dye/electrolyteinterface was investigated by AC impedence and equivalent circuit. The resultsshowed that electrons were more easily injected and transferred in the interface ofphotoanode/dye/electrolyte, so that the conversion efficiency of DSSC wasimproved. The results showed that the metal complexe with large conjugated systemwas positive for improving the performance of the DSSC.
In this paper, modification of photoanodes and co-sensitizing of dyes are usedto improve the photovolatic performance of DSSC based on ZnO photoanode, whichwill find wide provides potential applications in devices.
引文
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