本文選題：太陽電池　切入點(diǎn)：鈣鈦礦　出處：《中國科學(xué)技術(shù)大學(xué)》2017年博士論文　論文類型：學(xué)位論文

【摘要】：鈣鈦礦太陽電池作為一種新型太陽電池,具有生產(chǎn)成本低、制備工藝簡單、電遷移率高、吸光系數(shù)大等優(yōu)點(diǎn)。自誕生以來,就以驚人的速度刷新著效率記錄,是太陽能技術(shù)的一個重大革新。受帶隙寬度的限制,常規(guī)鈣鈦礦太陽電池只能吸收占太陽總輻射光譜44%左右的可見光,這導(dǎo)致電池吸收帶隙與入射太陽光譜不匹配,造成能量損失,限制了效率的提升。此外,具有較高能量的紫外光,會造成電池結(jié)構(gòu)一定程度的破壞,導(dǎo)致電池光電性能下降。采用紫外慮光膜雖然避免了紫外光對電池的損害,提高了電池的穩(wěn)定性,但也使電池?zé)o法有效利用紫外光,減小了電池的光采集效率。本論文從拓寬電池光譜響應(yīng)范圍提高效率及穩(wěn)定性的角度出發(fā),采用稀土下轉(zhuǎn)換材料將高能量紫外光轉(zhuǎn)換成低能量可見光,使其與電池的吸收光譜更加匹配,實(shí)現(xiàn)電池對入射太陽光的有效利用,同時減小紫外光誘導(dǎo)降解對電池性能的影響。稀土配合物作為一種優(yōu)良的發(fā)光材料,具有發(fā)光效率高、吸收范圍廣、熒光壽命長等優(yōu)點(diǎn)。在提高電池光利用率及性能方面,具有很好的應(yīng)用前景。本文對提高配合物發(fā)光性能、拓寬吸收范圍進(jìn)行了研究,并擇優(yōu)選取配合物應(yīng)用于鈣鈦礦太陽電池中,系統(tǒng)研究了配合物下轉(zhuǎn)換發(fā)光與電池性能之間的關(guān)系。此外,將易激發(fā)、量子效率高的Eu3+離子與介孔Ti02結(jié)合,進(jìn)一步降低電池內(nèi)部紫外光誘導(dǎo)降解,提高電池光采集效率。為提高稀土配合物的發(fā)光性能,在Phen-Eu(III)體系中引入乙二胺,調(diào)控發(fā)光中心(Eu3+離子)周圍微化學(xué)環(huán)境。通過分析配合物的光學(xué)性能發(fā)現(xiàn),乙二胺的添加含量小于或者等于0.2 mmol時,配合物的熒光強(qiáng)度明顯提高。但是過量的乙二胺與發(fā)光中心配位,會使發(fā)光中心趨于配位飽和,導(dǎo)致配體與發(fā)光中心之間的配位變困難,阻礙了配體向發(fā)光中心的有效能量傳遞,引起配合物的熒光性能下降。通過在配體(1,10-鄰菲羅啉)上引入不同特性取代基(5-硝基、5-甲基、4,7-二甲基、4,7-甲氧基和4,7-二苯基)改變配體結(jié)構(gòu),研究不同結(jié)構(gòu)下配合物的發(fā)光性能。結(jié)果表明,供電子基團(tuán)及共軛基團(tuán)能夠提高配合物電子云密度,使電子躍遷能級降低,增大配合物的紫外吸收系數(shù)。此外,這種取代基效應(yīng)及共軛效應(yīng)有助于提高配體與發(fā)光中心間的能級匹配程度,有效提升銪配合物分子內(nèi)的能量傳遞效率,從而增強(qiáng)了配合物的發(fā)光性能。選取紫外吸收能力強(qiáng)、發(fā)光強(qiáng)度大的配合物(銪-4,7-苯基-1,10-鄰菲羅啉)制成透明光轉(zhuǎn)換薄膜,采用下轉(zhuǎn)換層前置模型應(yīng)用在電池上,提高了電池的光采集效率,獲得了 11.8%的電流增益,光電轉(zhuǎn)換效率達(dá)到15.44%。紫外光照10 h后,仍保持了初始效率的74%,穩(wěn)定性明顯提高。為提高電池紫外光利用率,進(jìn)一步降低內(nèi)部紫外光誘導(dǎo)降解,將Eu引入介孔TiO2半導(dǎo)體制備TiO2:Eu3+下轉(zhuǎn)換發(fā)光材料,作為骨架層應(yīng)用到鈣鈦礦太陽電池中。采用SEM、XRD、XPS和熒光光譜等表征手段深入研究了 TiO2:Eu3+下轉(zhuǎn)換發(fā)光材料的晶體結(jié)構(gòu)和發(fā)光性能。發(fā)現(xiàn)Eu3+離子沒能摻雜到TiO2晶格中,而是附著在TiO2晶面上。同時TiO2能夠誘導(dǎo)Eu3+離子發(fā)光,實(shí)現(xiàn)電池對紫外光的有效利用。電池的光伏數(shù)據(jù)分析表明,Eu摻雜TiO2可以增強(qiáng)電池的紫外光捕獲效率,降低電池中TiO2產(chǎn)生的電子-空穴對對鈣鈦礦材料的氧化還原作用,同時抑制電子-空穴復(fù)合,提高電池開路電壓,從而使電池獲得更高的光電轉(zhuǎn)換效率及紫外穩(wěn)定性。然而過量摻雜Eu會使TiO2的晶界缺陷增加,TiO2中電子與CH3NH3PbI3中空穴復(fù)合的幾率變大,不利于TiO2中的電子傳輸。
[Abstract]:Perovskite solar battery is a new type of solar cell, has the advantages of low production cost, simple preparation, high mobility, absorption coefficient and other advantages of light. Since its birth, at an alarming rate refresh efficiency record, is a major innovation in solar technology. The band gap width limit, only routine perovskite solar absorption accounted for about 44% of the total solar radiation spectrum of visible light, which leads to cell absorption band gap and incident solar spectrum do not match, resulting in energy loss, limiting the efficiency. In addition, ultraviolet light has high energy, will cause the battery structure to a certain degree of damage, resulting in a decline in the photovoltaic performance by UV. Consider light film while avoiding the damage of UV on the battery, improves the stability of the battery, but also make the battery can not effectively use ultraviolet light, reduce the light collection efficiency of the battery. In this thesis, broaden the power The spectral response range of pool to improve the efficiency and stability of the perspective of using rare earth conversion materials will be converted into low energy high energy ultraviolet visible light, and the absorption spectrum of the battery more matching, to achieve efficient use of battery incident solar light, reduce the effect of UV induced degradation of cell performance. At the same time as rare earth complexes a kind of excellent luminescent materials, high luminous efficiency, wide range of absorption, fluorescence has the advantages of long service life. In the aspect of improving the battery light utilization rate and performance, has good application prospects. This paper to improve the luminous properties of complexes were studied, to broaden the range of absorption and ativity complexes used in perovskite in the solar cell system, studies the relationship between the complexes of conversion and cell performance. In addition, the easy to stimulate, Eu3+ ion and mesoporous Ti02 with high quantum efficiency, further reduced The internal battery UV induced degradation, improve the battery light collection efficiency. In order to improve the luminescence properties of rare earth complexes, Phen-Eu (III) into the ethylenediamine system, regulation of the luminescent center (Eu3+ ion) around the micro chemical environment. Through the analysis of the optical properties with the discovery, the content of ethylenediamine is less than or equal to 0.2 mmol, with the the fluorescence intensity increased significantly. But excessive ethylenediamine and luminescence center coordination, the coordination center of light tends to be saturated, causes between the ligand and the luminescent center coordination becomes difficult, hampered the effective energy transfer from ligand light center, decrease the fluorescence properties of the complexes. The ligand (1,10- o phenanthroline) on the introduction of different characteristics of substituents (5- nitro, 5- methyl 4,7-, methyl two, 4,7- two and 4,7- methoxy phenyl) change the ligand structure, luminescent properties of complexes of different structure. The results show that the electron donating group and conjugated complexes can improve the electron density, the electron transition energy level decreases and the UV absorption coefficient increase complexes. In addition, the substituent effect and conjugated effect is helpful to improve the level of luminescence center between the ligand and the matching degree, effectively improve the transfer efficiency of molecules within the EU the energy cooperation, so as to enhance the luminescence properties of the complexes. The selection of UV absorption ability, the luminescence intensity of complexes (europium -4,7- phenyl -1,10- phenanthroline) made of transparent light conversion film, pre conversion layer model is used in the battery use, improve the light collection efficiency of the battery, the current gain 11.8%, the photoelectric conversion efficiency reached 15.44%. after 10 h of UV light, still maintain the initial efficiency of 74%, significantly improve the stability. In order to improve the utilization of the battery to further reduce internal UV light, UV light induced reduction Solution, luminescent materials Eu into mesoporous TiO2 semiconductor fabrication of TiO2:Eu3+ conversion, as the skeleton layer applied to the perovskite solar cell. By using SEM, XRD, XPS and fluorescence spectra research TiO2:Eu3+ down conversion crystal structure and luminescence properties of luminescent materials. We can't Eu3+ ion doped into the TiO2 lattice but, attached to the TiO2 surface. At the same time, TiO2 can induce luminescence of Eu3+ ions, realize the effective utilization of the battery to ultraviolet. The photovoltaic battery data analysis shows that Eu doped TiO2 can enhance cell UV capture efficiency, reduce the oxidative electron hole cell TiO2 on the perovskite material reduction, and suppression the electron hole recombination, improve the open circuit voltage of the cell, so that the battery photoelectric conversion efficiency and UV stability higher. However, excessive Eu doping makes grain boundary defects increase of TiO2, TiO The probability of cavity recombination between 2 and 2 electrons in CH3NH3PbI3 becomes larger and is not conducive to electronic transmission in TiO2.

【學(xué)位授予單位】：中國科學(xué)技術(shù)大學(xué)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：O641.4;TM914.4

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