【作者】 唐彬；

【导师】 刘明侦；

【作者基本信息】 电子科技大学 ， 材料科学与工程， 2025， 硕士

【摘要】 有机-无机杂化钙钛矿太阳能电池（PSCs）由于其卓越的光电性能在光伏领域中受到青睐,然而其进一步发展仍受到钙钛矿薄膜结晶质量与器件稳定性的双重制约。一方面,采用低温溶液法制备的钙钛矿薄膜因快速结晶导致较差的结晶质量以及较高的缺陷密度,严重阻碍了器件光电转换效率（PCE）的提升;另一方面,钙钛矿薄膜在环境空气易发生降解,严重影响了器件稳定性。针对上述问题,本论文以提升器件PCE及稳定性为目标,系统开展了钙钛矿体相添加剂分子对薄膜结晶动力学及稳定性的影响研究。首先深入探究了添加剂分子作为体相结晶调节剂的作用机制,旨在通过优化结晶过程来提高薄膜的质量,接着基于对分子设计的深入理解,引入了多功能添加剂,通过协同调控策略,实现器件PCE与稳定性的同时增强。本文的具体研究内容如下:（1）针对溶液法快速结晶导致的结晶质量差、缺陷密度高等问题,本文创新性的引入含双羰基（C=O）基团的2,5-呋喃二羧酸（FDOA）作为结晶调节添加剂。通过C=O基团与钙钛矿前驱体中Pb²⁺之间的强配位作用,有效钝化铅相关缺陷,促使钙钛矿快速成核,使得优化后的薄膜展现出更大的晶粒尺寸和更低的Pb I₂残余量,显著提高了薄膜的结晶质量。基于此策略制备的PSCs实现了23.83%的光电转化效率,其中V_OC为1.196 V。（2）为了克服FDOA官能团功能单一性和未充分考虑器件稳定性的局限,本研究引入了一种多功能添加剂—四氟丁二酸酐（TFSA）从而实现对钙钛矿薄膜的协同调控。TFSA不仅保留了C=O基团的结晶调控及铅相关缺陷钝化作用,其分子中的氟基还可以通过N-H···F氢键锚定阳离子（FA⁺）,显著抑制阳离子空位的形成和离子迁移。同时,多氟基团提供疏水屏障,显著提高器件在环境空气中的稳定性。基于此策略,优化后的器件效率进一步提升至24.60%,其中V_OC高达1.208 V,且器件的正反扫迟滞现象显著降低,在高湿度环境（40-60%RH）下存储700小时后能保持75%初始效率,在低湿条件（5-10%RH）下效率保持率更是达到了93%。本论文提出的基于分子配位调控的钙钛矿改性策略,通过精心设计添加剂的分子结构,为实现高效稳定的PSCs提供了新的思路和方法。更多还原

【Abstract】 Organic-inorganic hybrid perovskite solar cells（PSCs）are gaining increasing attention in the photovoltaic field due to their superior optoelectronic performance.However,their further development is constrained by the dual challenges of perovskite film crystallization quality and device stability.On one hand,perovskite films fabricated via low-temperature solution methods suffer from rapid crystallization,leading to poor crystalline quality and high defect density,which severely hinder the improvement of power conversion efficiency（PCE）.On the other hand,perovskite films are prone to degradation in ambient air,significantly compromising device stability.To address these issues,this thesis aims to enhance both PCE and stability by systematically investigating the impact of bulk-phase additive molecules on perovskite film crystallization kinetics and stability.First,the mechanism of additive molecules as bulk-phase crystallization regulators is thoroughly explored to improve film quality by optimizing crystallization processes.Subsequently,leveraging insights from molecular design,multifunctional additives are introduced to synergistically enhance device PCE and stability.The specific research contributions are as follows:（1）To address poor crystallization quality and high defect density caused by rapid solution-phase crystallization,this thesis innovatively introduces 2,5-furandicarboxylic acid（FDOA）containing dicarbonyl（C=O）groups,as a crystallization-regulating additive.Through the strong coordination interaction between the C=O groups and Pb²⁺ions within the perovskite precursors,lead-related defects are effectively passivated,thereby promoting the rapid nucleation of the perovskite.This results in optimized films with larger grain sizes,reduced residual Pb I₂,and significantly improved crystallinity.PSCs fabricated using this strategy achieve a PCE of 23.83%with a high open-circuit voltage(V_OC)of 1.196 V.（2）To overcome FDOA’s limited functionality and insufficient stability considerations,a multifunctional additive,tetrafluorosuccinic anhydride（TFSA）,is introduced for synergistic regulation of perovskite films.TFSA not only retains the crystallization modulation and lead-related defect passivation functions of the C=O groups but also anchors cations（FA⁺）via N-H···F hydrogen bonds,significantly suppressing the formation of cation vacancies and ion migration.Additionally,its polyfluorinated groups create a hydrophobic barrier,markedly enhancing environmental stability.Optimized devices achieve a PCE of 24.60%with a V_OC of 1.208 V,along with significantly reduced hysteresis between forward and reverse scans.Remarkably,these devices retain 75%of their initial efficiency after 700 hours in high humidity（40–60%RH）and 93%under low humidity（5–10%RH）.The perovskite modification strategy based on molecular coordination regulation proposed in this thesis provides new ideas and methods for preparing highly efficient and stable PSCs by carefully designing the molecular structure of the additives.更多还原