新型无碘准固态电解质的研制及其在染料敏化太阳能电池中的应用
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摘要
二十世纪九十年代诞生的染料敏化太阳能电池(DSSCs)以其成本低廉、性能优越的特点成为硅基光伏器件最具竞争力的替代产品。但传统的含I-/13-氧还电对的有机液态电解质存在易挥发、有毒、吸光、侵蚀金属电流收集极和封装困难等缺陷,影响DSSC的规模化生产和长期稳定性。为此,本论文研发了一些新型不含碘单质(12)的准固态电解质,并探讨了电解质组分对其结晶行为、粘度、离子电导率及由其组装的DSSCs的光电化学性能的影响。获得的主要实验现象和研究结论归纳如下：
1.采用聚氧化乙烯(PEO)为胶凝剂,CuI为p-型空穴传输材料,LiC104为电荷传输助剂制备了CuI凝胶电解质。该电解质中的PEO能有效地抑制CuI的快速结晶,促进TiO2/CuI电解质形成良好的界面接触；而LiC104能将PEO转化为无定形基质以利于电荷传输。在含20wt%PEO的CuI凝胶电解质中掺杂3wt%LiClO4时获得了最高的离子电导率(8.7×10-3S cm-1),且吸附在Ti02表面的Li+能改善电子从激发态染料到Ti02的注入效率,极大地提高了DSSC的效率(2.81%)。与未加PEO(1.46%)或LiClO4(1.30%)的CuI电解质组装的DSSC相比,效率提高了96-116%。这种CuI凝胶电解质具有成本低、操作简便、环保高效等特点,为固态空穴传输材料在DSSC中的应用开辟了新的途径。
2.采用PEO为胶凝剂,离子液体1,2-二甲基-3-丙基咪唑碘(DMPⅡ)为电荷传输介质和碘源制备了离子液体凝胶电解质。由含20wt%PEO的离子液体凝胶电解质组装的DSSC能在不含12的情况下正常工作,并达到4.05%的效率,表明在电解质中去除12以规避其对DSSC困扰的思路是可行的。掺杂5wt%KI可极大地提高电解质的离子电导率(1.63×10-2S cm-1),且K+能抑制PEO的结晶、促进电子在TiO2/染料/电解质界面的迁移,从而将电池的效率提高到5.87%,效率改善了45%。这种离子液体凝胶电解质具有成分简单、操作简便和无毒不泄漏等特点,可为准固态DSSC提供新的高效电解质材料。
3.以1-丁基-3-甲基咪唑碘(BMⅡ)为电荷传输介质和碘源,双三氟甲磺酰亚胺锂(LiTFSI)为电荷传输助剂,采用低粘度的离子液体1-丁基-3-甲基咪唑硫氰酸盐(BMISCN)调节其流变性制备了二元离子液体电解质。由BMⅡ组装的DSSC能在不含12的情况下正常工作但仅获得了2.66%的效率,添加低粘度的BMISCN可降低电解质的粘度并提高电解质中的电荷交换反应,由其组装的DSSC获得了更高效率(4.33%)。LiTFSI不仅能提高电解质的离子电导率,还能改善DSSC中电荷载流子的传输并抑制电荷复合,从而获得了5.55%的效率(与未掺杂相比提高了28%)。这种二元离子液体电解质具有流变性好、无挥发和腐蚀性等特点,为离子液体电解质的研发与应用提供了新思路。
4.为克服离子液体电解质的流动性问题,以丁二腈作为固态溶剂和基质,离子液体BMⅡ和1-丙基-3-甲基咪唑碘(PMⅡ)为电荷传输介质和碘源制备了新型塑晶离子液体电解质。掺杂5wt%LiClO4到塑晶电解质中时,Li+与丁二腈能通过配位作用将结晶性基质转化为无定形含盐基质,改善了电解质的离子电导率,还能通过静电作用力吸引-和形成的13-以促进其电荷交换反应,进而将DSSC的效率提高到5.50%(与未掺杂相比提高了157%)。这种不含12的塑晶离子液体电解质具有机械性能好、便于封装以及无挥发和腐蚀性等特点,在柔性或固态DSSC的规模化生产方面具有较好的应用前景。
5.为验证不含I2的离子液体凝胶电解质在染料共敏化DSSC中应用的可行性,采用分步共敏化方法将光谱响应范围互补的有机染料OD-8与D149或SQ2联合对Ti02光阳极进行共敏化并组装成准固态DSSC,利用OD-8和D149或SQ2的吸收光谱匹配互补的特性提高电池的光捕获效率。OD-8/D149(6.21%)或OD-8/SQ2(6.10%)共敏化DSSC的效率均远高于OD-8(4.53%),D149(5.46%)和SQ2(2.86%)单一染料敏化的DSSC此外,不含I2的离子液体凝胶电解质在共敏化DSSC中能成功发挥电解质的功能,且表现出比传统有机液态电解质组装的共敏化DSSC更高的短路电流、开路电压和电池效率,表明不含I2的离子液体凝胶电解质在共敏化DSSC中具有显著的应用前景,也为替代价格昂贵的钌联毗啶类染料和发展宽光谱响应、高效环保的DSSCs提供了一些新的思路。
Due to its low-cost and high efficiency, dye-sensitized solar cells (DSSCs) have been the most promising candidate for traditional silicon solar cells since it was first invented in1991. However, traditional organic liquid electrolytes composed of I-/I3-redox couple are volatile, poisonous, corrosive and with optical absorption, which hurdles the encapsulation of DSSC and limits its industrialization. Thus, we carried out iodine free quasi solid-state electrolytes based on different matrix, and broadened spectral response of photoanodes. The main contents and conclusions are as follows:
1. CuI gel electrolyte is prepared by employing CuI as hole transport material, PEO as gelator and LiC104as dopant. It is concluded that PEO can inhibit the crystallization of Cul, promoting well interfacial contact between TiO2/CuI. Cul gel electrolyte doped with3wt%LiClO4achieves the highest ionic conductivity of8.7×10-3S cm-1. With LiClO4doped, PEO can be transformed to highly amorphous matrix. In addition, Li+absorbed on TiO2would enhance the electron injection efficiency. With PEO and LiC104participated Cul electrolyte, DSSC achieves an overall efficiency of2.81%, showing a96-116%improvement. The above Cul gel electrolyte is proved to be low cost, simple and eco-friendly, which offers us novel hole transport material for solid-state DSSC.
2. Ionic liquid gel electrolyte is prepared by employing1,2-dimethyl-3-propyl imidazolium iodide (DMPII) as charge transfer intermediate, PEO as gelator and KI as charge transfer enhancer. With KI participation, ionic conductivity goes up to16.32×10-3S cm-1. The existance of K+in electrolyte can inhibit the crystallization of PEO, and promote electron transfer between TiO2/dye/electrolyte. Compared to the DSSC based on ionic liquid electrolyte without KI (4.05%),5wt%KI doped electrolyte based DSSC obtains an improvement of45%, with Jsc of14.11mA cm-2, Voc of0.71∨and η of5.87%, respectively. Due to the advantages of simple, highly efficient and eco-friendly, the above ionic liquid gel electrolyte provides reference for the development of quasi solid-state DSSCs.
3. To improve the rheological behavior of ionic liquid electrolyte, binary ionic liquid electrolyte is prepared by employing BMII as charge transfer intermediate, LiTFSI as charge transfer enhancer and BMISCN with low viscosity as dopant. Ionic liquid BMII based DSSC without I2can work well and obtain a low efficiency of2.66%, addition of BMISCN can decrease the viscosity of electrolyte and improve the charge exchange reaction, leading to a higher efficiency of4.33%. LiTFSI doped with electrolyte could not only increase its ionic conductivity, but also improve the transportation of charge carrier and inhibit charge recombination in DSSC, finally yields the highest efficiency of5.55%, with an increasement of28%. I2is demonstrated to be unnecessary in the binary ionic liquid electrolyte. Since the bove binary ionic liquid electrolyte is proved to be simple, non-volatile and eco-friendly, it offers us novel suggestion for development of ionic liquid electrolytes.
4. In order to overcome the flowability of ionic liquid electrolyte, plastic crystal ionic liquid electrolyte is prepared by employing BMII and PMII as charge transfer intermediate, succinonitrile as solid solvent. It is concluded that5wt%LiClO4doped in plastic crystal ionic liquid electrolyte could transform succinonitrile matrix into amorphous matrix, increase the ionic conductivity of electrolyte and promote the charge exchange reaction between I-and I3-through electrostatic attraction, therefore improves the efficiency of DSSC up to5.50%, revealing an improvement of157%compared to that of without LiC104doped. Attributing to its flexible, non volatile and eco-friendly, the above plastic crystal ionic liquid electrolyte is beneficial for the industrialization development of flexible and solid-state DSSCs.
5. To demonstrate that iodine-free ionic liquid gel electrolyte is workable in cosensitized DSSC, we combined organic dye OD-8and D149or SQ2with complementary spectral response for stepwise cosensitization of photoanode, and assembled the quasi solid state DSSCs. It is hopeful to take advantage of OD-8and D149or SQ2's complementary spectral response to increase the light harvesting efficiency of DSSC. The overall efficiencies of OD-8/D149(6.21%) and OD-8/SQ2(6.10%) cosensitized DSSCs are superior to that of OD-8(4.53%), D149(5.46%) and SQ2(2.86%) sensitized DSSCs. In addition, iodine-free ionic liquid gel electrolyte can operate successfully in cosensitized DSSC, and achieves higher Jsc, Voc and r(than that of organic liquid electrolyte based DSSC, suggesting that iodine-free ionic liquid gel electrolyte is promising in cosensitized DSSC and provides us novel method for preparation of DSSCs with broad spectra response and eco-friendly.
1.采用聚氧化乙烯(PEO)为胶凝剂,CuI为p-型空穴传输材料,LiC104为电荷传输助剂制备了CuI凝胶电解质。该电解质中的PEO能有效地抑制CuI的快速结晶,促进TiO2/CuI电解质形成良好的界面接触；而LiC104能将PEO转化为无定形基质以利于电荷传输。在含20wt%PEO的CuI凝胶电解质中掺杂3wt%LiClO4时获得了最高的离子电导率(8.7×10-3S cm-1),且吸附在Ti02表面的Li+能改善电子从激发态染料到Ti02的注入效率,极大地提高了DSSC的效率(2.81%)。与未加PEO(1.46%)或LiClO4(1.30%)的CuI电解质组装的DSSC相比,效率提高了96-116%。这种CuI凝胶电解质具有成本低、操作简便、环保高效等特点,为固态空穴传输材料在DSSC中的应用开辟了新的途径。
2.采用PEO为胶凝剂,离子液体1,2-二甲基-3-丙基咪唑碘(DMPⅡ)为电荷传输介质和碘源制备了离子液体凝胶电解质。由含20wt%PEO的离子液体凝胶电解质组装的DSSC能在不含12的情况下正常工作,并达到4.05%的效率,表明在电解质中去除12以规避其对DSSC困扰的思路是可行的。掺杂5wt%KI可极大地提高电解质的离子电导率(1.63×10-2S cm-1),且K+能抑制PEO的结晶、促进电子在TiO2/染料/电解质界面的迁移,从而将电池的效率提高到5.87%,效率改善了45%。这种离子液体凝胶电解质具有成分简单、操作简便和无毒不泄漏等特点,可为准固态DSSC提供新的高效电解质材料。
3.以1-丁基-3-甲基咪唑碘(BMⅡ)为电荷传输介质和碘源,双三氟甲磺酰亚胺锂(LiTFSI)为电荷传输助剂,采用低粘度的离子液体1-丁基-3-甲基咪唑硫氰酸盐(BMISCN)调节其流变性制备了二元离子液体电解质。由BMⅡ组装的DSSC能在不含12的情况下正常工作但仅获得了2.66%的效率,添加低粘度的BMISCN可降低电解质的粘度并提高电解质中的电荷交换反应,由其组装的DSSC获得了更高效率(4.33%)。LiTFSI不仅能提高电解质的离子电导率,还能改善DSSC中电荷载流子的传输并抑制电荷复合,从而获得了5.55%的效率(与未掺杂相比提高了28%)。这种二元离子液体电解质具有流变性好、无挥发和腐蚀性等特点,为离子液体电解质的研发与应用提供了新思路。
4.为克服离子液体电解质的流动性问题,以丁二腈作为固态溶剂和基质,离子液体BMⅡ和1-丙基-3-甲基咪唑碘(PMⅡ)为电荷传输介质和碘源制备了新型塑晶离子液体电解质。掺杂5wt%LiClO4到塑晶电解质中时,Li+与丁二腈能通过配位作用将结晶性基质转化为无定形含盐基质,改善了电解质的离子电导率,还能通过静电作用力吸引-和形成的13-以促进其电荷交换反应,进而将DSSC的效率提高到5.50%(与未掺杂相比提高了157%)。这种不含12的塑晶离子液体电解质具有机械性能好、便于封装以及无挥发和腐蚀性等特点,在柔性或固态DSSC的规模化生产方面具有较好的应用前景。
5.为验证不含I2的离子液体凝胶电解质在染料共敏化DSSC中应用的可行性,采用分步共敏化方法将光谱响应范围互补的有机染料OD-8与D149或SQ2联合对Ti02光阳极进行共敏化并组装成准固态DSSC,利用OD-8和D149或SQ2的吸收光谱匹配互补的特性提高电池的光捕获效率。OD-8/D149(6.21%)或OD-8/SQ2(6.10%)共敏化DSSC的效率均远高于OD-8(4.53%),D149(5.46%)和SQ2(2.86%)单一染料敏化的DSSC此外,不含I2的离子液体凝胶电解质在共敏化DSSC中能成功发挥电解质的功能,且表现出比传统有机液态电解质组装的共敏化DSSC更高的短路电流、开路电压和电池效率,表明不含I2的离子液体凝胶电解质在共敏化DSSC中具有显著的应用前景,也为替代价格昂贵的钌联毗啶类染料和发展宽光谱响应、高效环保的DSSCs提供了一些新的思路。
Due to its low-cost and high efficiency, dye-sensitized solar cells (DSSCs) have been the most promising candidate for traditional silicon solar cells since it was first invented in1991. However, traditional organic liquid electrolytes composed of I-/I3-redox couple are volatile, poisonous, corrosive and with optical absorption, which hurdles the encapsulation of DSSC and limits its industrialization. Thus, we carried out iodine free quasi solid-state electrolytes based on different matrix, and broadened spectral response of photoanodes. The main contents and conclusions are as follows:
1. CuI gel electrolyte is prepared by employing CuI as hole transport material, PEO as gelator and LiC104as dopant. It is concluded that PEO can inhibit the crystallization of Cul, promoting well interfacial contact between TiO2/CuI. Cul gel electrolyte doped with3wt%LiClO4achieves the highest ionic conductivity of8.7×10-3S cm-1. With LiClO4doped, PEO can be transformed to highly amorphous matrix. In addition, Li+absorbed on TiO2would enhance the electron injection efficiency. With PEO and LiC104participated Cul electrolyte, DSSC achieves an overall efficiency of2.81%, showing a96-116%improvement. The above Cul gel electrolyte is proved to be low cost, simple and eco-friendly, which offers us novel hole transport material for solid-state DSSC.
2. Ionic liquid gel electrolyte is prepared by employing1,2-dimethyl-3-propyl imidazolium iodide (DMPII) as charge transfer intermediate, PEO as gelator and KI as charge transfer enhancer. With KI participation, ionic conductivity goes up to16.32×10-3S cm-1. The existance of K+in electrolyte can inhibit the crystallization of PEO, and promote electron transfer between TiO2/dye/electrolyte. Compared to the DSSC based on ionic liquid electrolyte without KI (4.05%),5wt%KI doped electrolyte based DSSC obtains an improvement of45%, with Jsc of14.11mA cm-2, Voc of0.71∨and η of5.87%, respectively. Due to the advantages of simple, highly efficient and eco-friendly, the above ionic liquid gel electrolyte provides reference for the development of quasi solid-state DSSCs.
3. To improve the rheological behavior of ionic liquid electrolyte, binary ionic liquid electrolyte is prepared by employing BMII as charge transfer intermediate, LiTFSI as charge transfer enhancer and BMISCN with low viscosity as dopant. Ionic liquid BMII based DSSC without I2can work well and obtain a low efficiency of2.66%, addition of BMISCN can decrease the viscosity of electrolyte and improve the charge exchange reaction, leading to a higher efficiency of4.33%. LiTFSI doped with electrolyte could not only increase its ionic conductivity, but also improve the transportation of charge carrier and inhibit charge recombination in DSSC, finally yields the highest efficiency of5.55%, with an increasement of28%. I2is demonstrated to be unnecessary in the binary ionic liquid electrolyte. Since the bove binary ionic liquid electrolyte is proved to be simple, non-volatile and eco-friendly, it offers us novel suggestion for development of ionic liquid electrolytes.
4. In order to overcome the flowability of ionic liquid electrolyte, plastic crystal ionic liquid electrolyte is prepared by employing BMII and PMII as charge transfer intermediate, succinonitrile as solid solvent. It is concluded that5wt%LiClO4doped in plastic crystal ionic liquid electrolyte could transform succinonitrile matrix into amorphous matrix, increase the ionic conductivity of electrolyte and promote the charge exchange reaction between I-and I3-through electrostatic attraction, therefore improves the efficiency of DSSC up to5.50%, revealing an improvement of157%compared to that of without LiC104doped. Attributing to its flexible, non volatile and eco-friendly, the above plastic crystal ionic liquid electrolyte is beneficial for the industrialization development of flexible and solid-state DSSCs.
5. To demonstrate that iodine-free ionic liquid gel electrolyte is workable in cosensitized DSSC, we combined organic dye OD-8and D149or SQ2with complementary spectral response for stepwise cosensitization of photoanode, and assembled the quasi solid state DSSCs. It is hopeful to take advantage of OD-8and D149or SQ2's complementary spectral response to increase the light harvesting efficiency of DSSC. The overall efficiencies of OD-8/D149(6.21%) and OD-8/SQ2(6.10%) cosensitized DSSCs are superior to that of OD-8(4.53%), D149(5.46%) and SQ2(2.86%) sensitized DSSCs. In addition, iodine-free ionic liquid gel electrolyte can operate successfully in cosensitized DSSC, and achieves higher Jsc, Voc and r(than that of organic liquid electrolyte based DSSC, suggesting that iodine-free ionic liquid gel electrolyte is promising in cosensitized DSSC and provides us novel method for preparation of DSSCs with broad spectra response and eco-friendly.
引文
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