本文選題：鈣鈦礦太陽能電池　切入點：電子傳輸層　出處：《中國科學(xué)院大學(xué)(中國科學(xué)院物理研究所)》2017年博士論文

【摘要】：鈣鈦礦太陽能電池因其優(yōu)秀的吸光能力、簡單的制備工藝、高的能量轉(zhuǎn)化效率成為具有商業(yè)化應(yīng)用前景的下一代太陽能電池之一。在鈣鈦礦電池中,電子傳輸材料和異質(zhì)結(jié)界面與載流子的傳輸、復(fù)合過程緊密聯(lián)系,嚴(yán)重影響著電池的性能。本論文的工作圍繞鈣鈦礦太陽能電池的電子傳輸層以及界面展開,主要涉及了鈣鈦礦電池的準(zhǔn)確性測量,新型電子傳輸層結(jié)構(gòu)的的制備,鈣鈦礦電池中電子傳輸層異質(zhì)結(jié)界面原子結(jié)構(gòu)的研究,以及制備電子傳輸層的原子層沉積系統(tǒng)的設(shè)計、集成與搭建等,取得了以下成果:一、詳細(xì)分析了鈣鈦礦太陽能電池中,測量蒙版(mask)的大小和實際電池的活性面積之間的比例對電池性能的準(zhǔn)確評估的影響。研究了不同大小的蒙版面積(mask aperture)下鈣鈦礦太陽能電池的J-V特性,指出不同大小的非光照暗態(tài)面積會顯著影響電池的開路電壓。首次提出了一種雙二極管的模型來模擬暗態(tài)電池和光照電池同時存在時對整體器件J-V測量結(jié)果的影響,利用阻抗譜和瞬態(tài)光電壓衰減的手段證明如果mask小于電池活性面積會導(dǎo)致器件中增加的電荷復(fù)合途徑,將會低估實際器件的開路電壓(減少約10%)。最終的研究結(jié)果指明了一種準(zhǔn)確評價鈣鈦礦性能的方法。二、首次提出制備了一種TiO_2/ZnO雙層電子傳輸層的結(jié)構(gòu),這種雙層結(jié)構(gòu)結(jié)合了高的電子抽取性能和低的界面復(fù)合特點。在平面結(jié)構(gòu)的鈣鈦礦太陽能電池中,由于使用了這種雙層電子傳輸層,前表面復(fù)合過程得到了有效的抑制,獲得了超過17%的光電轉(zhuǎn)化效率,其中短路電流超過21mA/cm~2,開路電壓1084 mV,填充因子0.75。該工作提供了一種簡單的界面層處理方法用來獲得高效率的鈣鈦礦電池。三、與中科院物理所谷林研究員合作,利用球差矯正電子顯微鏡研究了鈣鈦礦電池中TiO_2/MAPbI_3異質(zhì)結(jié)界面,發(fā)現(xiàn)這個界面存在一個單原子層厚度的重原子層,是由于界面甲胺基團(tuán)空位的存在所導(dǎo)致。配合第一性原理計算,表明這個異質(zhì)結(jié)界面的MA基團(tuán)缺失可以導(dǎo)致TiO_2和MAPbI_3之間更強原子間結(jié)合力,從而增強界面的穩(wěn)定性。這個研究結(jié)果能夠幫助進(jìn)一步理解鈣鈦礦電池中的異質(zhì)結(jié)界面原子排布與相互作用,為今后的界面處理提供理論指導(dǎo)。四、自主設(shè)計研制了實驗室第一臺原子層沉積設(shè)備,包括真空腔體、氣路、電氣控制的設(shè)計與控制軟件的編寫,具有單次反應(yīng)時間小于50 ms,單次循環(huán)時間小于20s的快速響應(yīng)特點。研制的原子層沉積設(shè)備被用于氧化物薄膜的制備和太陽能電池的界面處理。利用該設(shè)備,低溫制備了ZnO、TiO_2電子傳輸層并應(yīng)用于鈣鈦礦太陽能電池,獲得了超過18%的光電轉(zhuǎn)化效率。自主搭建的系統(tǒng)有效降低了成本,并投入到實驗室的使用,成為一種薄膜制備的有效手段。
[Abstract]:Perovskite solar cells have become one of the next generation solar cells with commercial applications due to their excellent absorptivity, simple preparation process and high energy conversion efficiency.In perovskite batteries, the transport of electron transport materials and heterojunction surfaces with carriers is closely related to the recombination process, which seriously affects the performance of the battery.This paper focuses on the electron transport layer and interface of the perovskite solar cell. It mainly involves the measurement of the accuracy of the perovskite cell and the preparation of the new structure of the electron transport layer.The research on atomic structure of electron transport layer heterojunction surface in perovskite battery and the design, integration and construction of atomic layer deposition system for preparing electron transport layer have obtained the following achievements: first, the detailed analysis of perovskite solar cell,The effect of the ratio between the size of the mask and the active area of the actual battery on the accurate evaluation of the battery performance is measured.The J-V characteristics of perovskite solar cells under mask aperture with different sizes are studied. It is pointed out that the open circuit voltage is significantly affected by different sizes of non-illumination dark areas.A two-diode model is proposed for the first time to simulate the effect of the existence of both dark and light cells on the J-V measurement results of the whole device.By means of impedance spectroscopy and transient photovoltage attenuation, it is proved that if the mask is smaller than the active area of the cell, it will lead to the increase of the charge recombination path in the device, and the open circuit voltage of the actual device will be underestimated (about 10% reduction).The final results indicate an accurate method for evaluating perovskite properties.Secondly, a structure of TiO_2/ZnO double-layer electron transport layer is proposed for the first time, which combines the characteristics of high electron extraction performance and low interface recombination.In a planar perovskite solar cell, the composite process of the front surface is effectively suppressed by the use of this double-layer electron transport layer, and over 17% of the photoelectric conversion efficiency is obtained.The short circuit current exceeds 21 Ma / cm ~ 2, the open circuit voltage is 1084 MV, and the filling factor is 0.75.This work provides a simple interface layer processing method for high efficiency perovskite cells.Third, in cooperation with Gulin, a researcher at the Institute of Physics of the Chinese Academy of Sciences, the TiO_2/MAPbI_3 heterojunction interface in perovskite batteries has been studied using spherical aberration electron microscopy. It has been found that there is a heavy atomic layer with a single atomic layer thickness at the interface.This is due to the existence of interfacial methylamine group vacancies.The results of first-principles calculation show that the absence of MA group in the heterojunction interface can lead to a stronger interatomic bonding force between TiO_2 and MAPbI_3, thus enhancing the stability of the interface.The results of this study can help to further understand the arrangement and interaction of heterojunction atoms in perovskite cells and provide theoretical guidance for the interface treatment in the future.Fourth, the first atomic layer deposition equipment in the laboratory has been independently designed and developed, including the design and control software for vacuum chamber, gas path and electrical control.The reaction time is less than 50 Ms and the single cycle time is less than 20 s.The atomic layer deposition equipment has been developed for the preparation of oxide films and the interface treatment of solar cells.Using this equipment, ZnO- TiO2 electronic transport layer was prepared at low temperature and applied to perovskite solar cells. The photovoltaic conversion efficiency of more than 18% was obtained.The self-built system can effectively reduce the cost and be used in the laboratory. It has become an effective method for the preparation of thin films.
【學(xué)位授予單位】：中國科學(xué)院大學(xué)(中國科學(xué)院物理研究所)
【學(xué)位級別】：博士
【學(xué)位授予年份】：2017
【分類號】：TM914.4

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