钙钛矿太阳电池的高可重现性与大面积制备技术研究

发布时间：2018-07-03 19:46

本文选题：钙钛矿 + 太阳电池　；参考：《华北电力大学(北京)》2017年博士论文

【摘要】：近年来,基于无机-有机杂化钙钛矿光伏材料的钙钛矿太阳电池因其因其制备成本低、光电转换效率提升快而倍受关注。而真正实现钙钛矿太阳电池的实际应用,仍有诸多问题需进一步地探索,如大面积制备及其工艺的稳定性等。针对于此,本论文从溶液制备法的工艺优化到器件性能的进一步提升,以及大面积制备工艺的开发等方面开展了研究,具体内容包括:(1)在分步液浸法及两步旋涂法的基础上,提出以多步旋涂法沉积钙钛矿薄膜,实现了钙钛矿太阳电池高可重现性的制备。一方面,以定量旋涂异丙醇的方式对PbI2薄膜进行预润湿,并采用旋涂冲洗的后处理工艺改善了钙钛矿薄膜的成膜质量;另一方面,利用异丙醇和环己烷的混合体作为溶剂配制CH3NH3I前驱体溶液,优化了PbI2到钙钛矿的转化反应。利用上述方法制备的CH3NH3PbI3薄膜晶粒尺寸分布集中,薄膜覆盖率高、均匀性好,不但有效避免原料试剂的浪费、增强了过程可操作性,而且实现了各项实验参数的量化控制。利用该方法制备的钙钛矿薄膜使器件光电转换的标准偏差不超过±0.52,器件的可重现性得以显著增强。(2)通过溶剂工程与氯添加剂的优选组合,实现了钙钛矿薄膜质量的提升,获得了较高效率的钙钛矿电池。研究表明,在DMSO溶剂体系下,PbCl2的介入可显著提升钙钛矿薄膜的成膜质量,并增强了活性层的光吸收能力;当掺入PbCl2的摩尔百分比为30%时,所得薄膜的形貌、结晶特性达到相对最优状态,并表现出了较强的光收集能力。在此条件下制备的钙钛矿太阳电池光电转换效率达到14.42%,较无PbCl2添加剂调控时的效率值提高了36.3%。(3)提出了基于磁控溅射技术的钙钛矿薄膜沉积方法。首先,使用高纯金属铅(Pb)靶,以高纯Ar、O2分别作为工作气体和反应气体,在衬底上溅射PbO薄膜;其次,使PbO薄膜与CH3NH3I前驱体溶液进行反应,实现了从PbO到CH3NH3PbI3的转化。经工艺参数的优化,获得了质量和性能均较优的钙钛矿薄膜;在此基础上,进一步制备了介孔结构的钙钛矿太阳电池,实现了13.8%的光电转换效率。(4)探索研究面向规模化量产的大面积钙钛矿太阳电池的制备工艺技术,利用磁控溅射技术沉积钙钛矿薄膜,在有效面积超过1 cm2的平面结构太阳电池上实现了10.7%的光电转换效率;通过不同面积的器件光伏性能对比分析,可以看出,该项技术是实现大面积钙钛矿电池制备的有效方法之一。
[Abstract]:In recent years, perovskite solar cells based on inorganic and organic hybrid perovskite photovoltaic materials have attracted much attention due to their low preparation cost and rapid improvement of photoelectric conversion efficiency. In order to realize the practical application of perovskite solar cells, there are still many problems that need to be further explored, such as the preparation of large area and the stability of the process. In this paper, the process optimization of the solution preparation method, the further improvement of the device performance and the development of the large area preparation process are studied. The specific contents include: (1) on the basis of the two-step liquid leaching method and the two-step spin coating method, The high reproducibility of perovskite solar cells was achieved by multi-step spin coating method. On the one hand, the prewetting of PBI2 thin film is carried out by the way of quantitative spin-coating isopropanol, and the film forming quality of perovskite film is improved by the post-treatment process of spin-coating and washing, on the other hand, The mixture of isopropanol and cyclohexane was used as solvent to prepare Ch _ 3NH _ 3i precursor solution and the conversion reaction from PBI2 to perovskite was optimized. The Ch _ 3NH _ 3PbI _ 3 thin film prepared by the above method has the advantages of concentrated grain size distribution, high film coverage and good uniformity. It not only effectively avoids the waste of the raw material reagent, enhances the operation of the process, but also realizes the quantitative control of the experimental parameters. The perovskite film prepared by this method can make the standard deviation of photovoltaic conversion less than 卤0.52, and the reproducibility of the device can be significantly enhanced. (2) the quality of perovskite film can be improved by the combination of solvent engineering and chlorine additive. A high efficiency perovskite battery was obtained. The results show that the quality of perovskite films and the photoabsorption of the active layer can be significantly enhanced by PbCl _ 2 in DMSO solvent system, and the morphology of the films can be obtained when the mole percentage of PbCl _ 2 is 30%. The crystallization characteristic reaches the relative optimum state, and shows the strong light collection ability. Under these conditions, the photovoltaic conversion efficiency of the prepared perovskite solar cells is 14.42, which is 36.3% higher than that without PbCl2 additive. (3) the method of perovskite thin film deposition based on magnetron sputtering is proposed. Firstly, PBO thin films were deposited on substrates using high purity lead (Pb) target as working gas and reaction gas, respectively. Secondly, PBO thin films were transformed from PBO to CH3NH3PbI3 by reaction with Ch _ 3NH _ 3i precursor solution. The perovskite thin films with better quality and performance were obtained by optimizing the process parameters, and the mesoporous perovskite solar cells were further prepared. The optoelectronic conversion efficiency of 13.8% has been achieved. (4) the fabrication technology of large-area perovskite solar cells for large-scale production has been studied and the magnetron sputtering technique has been used to deposit perovskite thin films. The photovoltaic conversion efficiency of 10.7% is realized on the solar cells with an effective area of more than 1 cm2. This technique is one of the effective methods to fabricate large-area perovskite batteries.
【学位授予单位】：华北电力大学(北京)
【学位级别】：博士
【学位授予年份】：2017
【分类号】：TM914.4

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