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中国物理学会期刊

离子液体辅助的结晶调控与界面修饰以提升全无机钙钛矿电池的光伏性能

Ionic Liquid-Assisted Crystallization Regulation and Interface Modification for Enhancing Photovoltaic Performance of All-Inorganic Perovskite Solar Cells

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  • 全无机钙钛矿可用于研发钙钛矿叠层或半透明电池,具有良好的发展潜力. 但全无机钙钛矿存在结晶质量差、多体相缺陷和界面缺陷等问题,严重制约了太阳能电池光伏性能的提升. 针对这一问题,本文将离子液体1-乙基-3-甲基咪唑乙酸盐(1-ethyl-3-methylimidazolium acetate, EMIMAc)加入到CsPbI1.5Br1.5钙钛矿前驱体溶液中以调控其结晶速率,成功获得了高质量的薄膜. 钙钛矿结晶后,EMIMAc在其表面、体相和TiO2/钙钛矿埋底界面均有分布. 在表面和体相,EMIMAc钝化了Pb2+缺陷和卤素缺陷;在埋底界面,EMIMAc不仅钝化了TiO2的氧空位缺陷还优化了其能级匹配. 虽然该离子液体兼具缺陷钝化与界面优化的双重功能,但电荷传输动力学分析证实,体相缺陷钝化是器件光伏性能提升的主导因素,界面优化则起辅助作用. 经EMIMAc优化,碳基无空穴传输层钙钛矿电池的光电转换效率达到了13.38%, 远高于对照组电池(11.44%). 此外,EMIMAc的引入显著提高了电池的长期稳定性. 在空气环境中贮存65天后,未封装的电池保持了初始效率的95%;在100 mW/cm2持续光照且最大功率点跟踪测试120 h后,封装的电池仍保持了初始效率的93%,其稳定性明显优于对照组.

     

    All-inorganic perovskites hold promise for tandem or semi-transparent photovoltaics. However, they often suffer from poor crystallization quality and high densities of bulk and interfacial defects, severely limiting device performance. To address these issues, an ionic liquid 1-ethyl-3-methylimidazolium acetate (EMIMAc) is incorporated into the CsPbI1.5Br1.5 perovskite precursor to modulate the crystallization rate, thus successfully obtaining high-quality films. After perovskite crystallization, EMIMAc distributes across its surface, bulk, and the buried TiO2/perovskite interface. At the surface and in the bulk, it passivates Pb2+-related and halogen defects; at the buried interface, it passivates oxygen vacancies on TiO2 and optimizes the energy-level alignment. Thus, EMIMAc serves as a dual-functional agent for defect passivation and interface modification. Notably, charge transport dynamics confirms that bulk defect passivation dominates the performance enhancement, with interface optimization playing a subsidiary role. The resultant carbon-based hole-transport-layer-free CsPbI1.5Br1.5 perovskite solar cell achieves a power conversion efficiency of 13.38%, substantially higher than that of the control device (11.44%). Moreover, EMIMAc incorporation significantly improves the device stability. After storage in ambient air for 65 days, the unencapsulated device retains 95% of its initial efficiency; after 120 h of continuous maximum power point tracking under 100 mW/cm2 illumination, the encapsulated device maintains 93% of its initial efficiency, demonstrating superior stability compared to the control device.

     

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