钙钛矿型太阳能电池制备方法的研究
发布时间：2018-11-15 07:34
【摘要】：新型薄膜太阳能电池领域中,钙钛矿太阳能电池近年来发展迅速,在短短几年的时间里,最高光电转化效率从3.8%迅速提高到22.1%,超过了量子点敏化太阳能电池和有机聚合物太阳能电池,得到了越来越多的关注。钙钛矿型太阳能电池包括电极材料,电子传输层,钙钛矿吸光层,空穴传输材料等全部或部分结构,其中钙钛矿吸光层是电池性能的关键影响因素。在材料制备方面,制备方法决定结构,结构决定性质,所以钙钛矿材料的制备方法决定电池的性能。在过去的几年中,人们对钙钛矿的制备方法有了很多突出的工作,电池性能取得了巨大进步。本文围绕两步多次沉积方法制备钙钛矿吸光材料展开了研究,并且取得了以下成果:首次将多次沉积方法应用于制备纯相FAPbI_3钙钛矿太阳能电池。结果表明,用该方法制备纯相FAPbI_3钙钛矿太阳能电池,不会产生δ非钙钛矿黄相,并且制备得到的薄膜取向性良好,结晶性和稳定性也得到了很大的提高,并且薄膜晶粒出现非正常生长,晶粒尺寸达到了微米量级。通过控制沉积滴数,可以有效控制剩余碘化铅量及反应进度。较好的薄膜性质是高效率的基础,用该方法制备的纯相FAPbI_3钙钛矿电池最高效率达到17.66%。我们在制备过程中加入少量的MAI,对FAI进行替换,使得整体电压和效率得到明显提高,最优比例为摩尔比RFAI/MAI=6:4,在最优比例下,制备的电池最高效率达到19.3%。该工作为发展和制备高效FAPbI_3和混合阳离子钙钛矿电池提供了一个可靠有效的方法。首次通过研究FAI和MAI不同阳离子与PbI2反应过程中成核生长过程,对两步法中阳离子沉积过程进行调控,进而调控钙钛矿生长过程。将两步法沉积过程中第二步用纯相溶液依次沉积—原位离子交换法,并研究和表征了沉积和退火过程中的成核反应过程。结果表明,用该方法可以制备出结晶性良好,晶粒尺寸大,形貌良好的混合阳离子钙钛矿薄膜。通过对沉积和退火后薄膜性能的表征,对沉积过程和成核生长过程进行了研究,我们发现,用原位离子交换法制备薄膜可以先沉积MA+,与碘化铅反应形成致密的小晶粒层钙钛矿薄膜,后面沉积FA+,FA+与MA+相互扩散并替换,使得薄膜的成分梯度分布,FA+不容易与碘化铅反应形成钙钛矿晶粒,但是FA+相对比较容易与钙钛矿反应对MA+进行替换,从而形成较均匀且致密的薄膜。FA+后沉积过程,有利于辅助晶粒长大,晶粒尺寸达到微米量级。我们用该方法制备的最优条件下的钙钛矿太阳能电池最高效率突破20%,达到20.44%。该工作对两步法中多次沉积方法进行了改进,并研究了沉积和退火过程,对进一步改进钙钛矿材料的制备工艺具有一定的指导意义。
[Abstract]:In the field of new thin film solar cells, perovskite solar cells have developed rapidly in recent years. In just a few years, the highest photoelectric conversion efficiency has been raised rapidly from 3.8% to 22.1%. More and more attention has been paid to quantum dot-sensitized solar cells and organic polymer solar cells. Perovskite solar cells include electrode materials, electron transport layer, perovskite absorbent layer, hole transport material, etc. Among them, perovskite absorption layer is the key factor affecting the performance of the cell. In the aspect of material preparation, the preparation method determines the structure and properties, so the preparation method of perovskite material determines the performance of the battery. In the past few years, a lot of outstanding work has been done on the preparation of perovskite, and great progress has been made in the performance of the battery. In this paper, the preparation of perovskite absorbent materials by two steps multiple deposition method has been studied, and the following results have been obtained: for the first time, the multiple deposition method has been applied to the preparation of pure FAPbI_3 perovskite solar cells. The results show that the pure FAPbI_3 perovskite solar cells prepared by this method will not produce 未 -non-perovskite yellow phase, and the prepared films have good orientation, and the crystallinity and stability have been greatly improved. And the grain size of the film reaches micron order of magnitude. The amount of residual lead iodide and reaction progress can be effectively controlled by controlling the number of droplets deposited. Good film properties are the basis of high efficiency. The maximum efficiency of pure phase FAPbI_3 perovskite battery prepared by this method is 17.66. In the preparation process, a small amount of MAI, was added to replace the FAI, and the overall voltage and efficiency were improved obviously. The optimum molar ratio of RFAI/MAI=6:4, in the optimal proportion was 19.3wt%, and the maximum efficiency of the prepared battery was 19.3%. This work provides a reliable and effective method for the development and preparation of high efficiency FAPbI_3 and mixed cationic perovskite batteries. For the first time, the nucleation and growth process of different cations of FAI and MAI in reaction with PbI2 was studied, and the process of cationic deposition in the two-step process was regulated, and then the growth process of perovskite was regulated. The second step of the two-step deposition process was sequentially deposition-in-situ ion exchange method with pure phase solution, and the nucleation reaction process in the deposition and annealing process was studied and characterized. The results show that the mixed cationic perovskite thin films with good crystallinity, large grain size and good morphology can be prepared by this method. The deposition and nucleation process of the films were investigated by characterizing the properties of the films after deposition and annealing. We found that MA can be deposited first by in situ ion exchange method. A compact perovskite thin film with small grain layer was formed by reaction with lead iodide, and then FA, FA and MA were deposited to diffuse and replace each other, which resulted in the composition gradient distribution of the film, and FA could not react easily with lead iodide to form perovskite grain. However, FA is relatively easy to replace MA with perovskite to form a more uniform and compact film. The post-deposition process of FA is favorable to assist grain growth, and the grain size reaches micron order. The maximum efficiency of perovskite solar cells prepared by this method is 20.44. In this work, the method of multiple deposition in the two-step method is improved, and the deposition and annealing process are studied, which has certain guiding significance for further improving the preparation process of perovskite materials.
【学位授予单位】：中国科学院大学(中国科学院物理研究所)
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TM914.4
本文编号：2332584
[Abstract]:In the field of new thin film solar cells, perovskite solar cells have developed rapidly in recent years. In just a few years, the highest photoelectric conversion efficiency has been raised rapidly from 3.8% to 22.1%. More and more attention has been paid to quantum dot-sensitized solar cells and organic polymer solar cells. Perovskite solar cells include electrode materials, electron transport layer, perovskite absorbent layer, hole transport material, etc. Among them, perovskite absorption layer is the key factor affecting the performance of the cell. In the aspect of material preparation, the preparation method determines the structure and properties, so the preparation method of perovskite material determines the performance of the battery. In the past few years, a lot of outstanding work has been done on the preparation of perovskite, and great progress has been made in the performance of the battery. In this paper, the preparation of perovskite absorbent materials by two steps multiple deposition method has been studied, and the following results have been obtained: for the first time, the multiple deposition method has been applied to the preparation of pure FAPbI_3 perovskite solar cells. The results show that the pure FAPbI_3 perovskite solar cells prepared by this method will not produce 未 -non-perovskite yellow phase, and the prepared films have good orientation, and the crystallinity and stability have been greatly improved. And the grain size of the film reaches micron order of magnitude. The amount of residual lead iodide and reaction progress can be effectively controlled by controlling the number of droplets deposited. Good film properties are the basis of high efficiency. The maximum efficiency of pure phase FAPbI_3 perovskite battery prepared by this method is 17.66. In the preparation process, a small amount of MAI, was added to replace the FAI, and the overall voltage and efficiency were improved obviously. The optimum molar ratio of RFAI/MAI=6:4, in the optimal proportion was 19.3wt%, and the maximum efficiency of the prepared battery was 19.3%. This work provides a reliable and effective method for the development and preparation of high efficiency FAPbI_3 and mixed cationic perovskite batteries. For the first time, the nucleation and growth process of different cations of FAI and MAI in reaction with PbI2 was studied, and the process of cationic deposition in the two-step process was regulated, and then the growth process of perovskite was regulated. The second step of the two-step deposition process was sequentially deposition-in-situ ion exchange method with pure phase solution, and the nucleation reaction process in the deposition and annealing process was studied and characterized. The results show that the mixed cationic perovskite thin films with good crystallinity, large grain size and good morphology can be prepared by this method. The deposition and nucleation process of the films were investigated by characterizing the properties of the films after deposition and annealing. We found that MA can be deposited first by in situ ion exchange method. A compact perovskite thin film with small grain layer was formed by reaction with lead iodide, and then FA, FA and MA were deposited to diffuse and replace each other, which resulted in the composition gradient distribution of the film, and FA could not react easily with lead iodide to form perovskite grain. However, FA is relatively easy to replace MA with perovskite to form a more uniform and compact film. The post-deposition process of FA is favorable to assist grain growth, and the grain size reaches micron order. The maximum efficiency of perovskite solar cells prepared by this method is 20.44. In this work, the method of multiple deposition in the two-step method is improved, and the deposition and annealing process are studied, which has certain guiding significance for further improving the preparation process of perovskite materials.
【学位授予单位】：中国科学院大学(中国科学院物理研究所)
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：TM914.4
【参考文献】
相关期刊论文 前2条
1 Huiyin Zhang;Jiangjian Shi;Juan Dong;Xin Xu;Yanhong Luo;Dongmei Li;Qingbo Meng;;A repeated interdiffusion method for efficient planar formamidinium perovskite solar cells[J];Journal of Energy Chemistry;2015年06期
2 姚鑫;丁艳丽;张晓丹;赵颖;;钙钛矿太阳电池综述[J];物理学报;2015年03期
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