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Grain Boundary Defects Passivated with tert-Butyl Methacrylate for High-Efficiency Perovskite Solar Cells
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-09-20 , DOI: 10.1021/acsaem.1c02125 Min Zhao 1, 2, 3 , Jin Yan 2, 4 , Gang Yu 2, 3 , Weichuang Yang 2, 5 , Jiarui Wu 2 , Yongqiang Zhang 2 , Jiang Sheng 2 , Jingsong Sun 1, 2 , Chunhui Shou 1 , Baojie Yan 2 , Zhengping Fu 6 , Jichun Ye 2
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2021-09-20 , DOI: 10.1021/acsaem.1c02125 Min Zhao 1, 2, 3 , Jin Yan 2, 4 , Gang Yu 2, 3 , Weichuang Yang 2, 5 , Jiarui Wu 2 , Yongqiang Zhang 2 , Jiang Sheng 2 , Jingsong Sun 1, 2 , Chunhui Shou 1 , Baojie Yan 2 , Zhengping Fu 6 , Jichun Ye 2
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A high-quality perovskite film is critical to realize high-efficiency and hysteresis-less perovskite solar cells (PSCs). However, a solution-processed perovskite layer presents many ionic vacancies on grain boundaries, which serve as nonradiative recombination centers that cause a loss of photocurrent. Herein, a trace amount of Lewis base tert-butyl acrylate (TBA) with both effective C═O and C═C functional groups is introduced to synergistically control the crystallization process and saturate surface dangling bonds. The C═O groups of TBA strongly bond to the uncoordinated Pb2+ to be a more stable TBA-PbI2 Lewis adduct, slowing down the perovskite crystallization to form a high-crystalline quality film and suppressing the formation of nonradiative recombination defects at perovskite boundaries. In addition, the π–σ and π–π conjugated bonds of C═C and −C═O in TBA show a strong delocalized electron-rich structure, promoting the photogenerated charge carrier diffusion in the perovskite layer. As a consequence, the open-circuit voltage of a TBA-PSC is significantly increased from 1.07 to 1.12 V and the fill factor is improved from 78.20 to 81.56%. Thus, the TBA-PSC achieves a high power conversion efficiency of 22.82% with negligible hysteresis. Therefore, the TBA additive is a feasible and efficient method to improve the perovskite crystalline quality for high-performance PSCs.
中文翻译：
用于高效钙钛矿太阳能电池的甲基丙烯酸叔丁酯钝化晶界缺陷
高质量的钙钛矿薄膜对于实现高效且无滞后的钙钛矿太阳能电池 (PSC) 至关重要。然而，溶液处理的钙钛矿层在晶界上存在许多离子空位，这些空位作为非辐射复合中心，导致光电流损失。在本文中，引入了具有有效 C=O 和 C=C 官能团的痕量路易斯碱丙烯酸叔丁酯 (TBA) 以协同控制结晶过程并使表面悬键饱和。TBA 的 C=O 基团与未配位的 Pb 2+强键合，形成更稳定的 TBA-PbI 2Lewis 加合物，减缓钙钛矿结晶以形成高结晶质量的薄膜，并抑制钙钛矿边界处非辐射复合缺陷的形成。此外，TBA中C=C和-C=O的π-σ和π-π共轭键显示出很强的离域富电子结构，促进了钙钛矿层中的光生电荷载流子扩散。因此，TBA-PSC 的开路电压从 1.07 V 显着增加到 1.12 V，填充因子从 78.20 提高到 81.56%。因此，TBA-PSC 实现了 22.82% 的高功率转换效率，滞后可忽略不计。因此，TBA添加剂是提高高性能PSCs钙钛矿晶体质量的一种可行且有效的方法。
更新日期：2021-10-25
中文翻译：
用于高效钙钛矿太阳能电池的甲基丙烯酸叔丁酯钝化晶界缺陷
高质量的钙钛矿薄膜对于实现高效且无滞后的钙钛矿太阳能电池 (PSC) 至关重要。然而，溶液处理的钙钛矿层在晶界上存在许多离子空位，这些空位作为非辐射复合中心，导致光电流损失。在本文中，引入了具有有效 C=O 和 C=C 官能团的痕量路易斯碱丙烯酸叔丁酯 (TBA) 以协同控制结晶过程并使表面悬键饱和。TBA 的 C=O 基团与未配位的 Pb 2+强键合，形成更稳定的 TBA-PbI 2Lewis 加合物，减缓钙钛矿结晶以形成高结晶质量的薄膜，并抑制钙钛矿边界处非辐射复合缺陷的形成。此外，TBA中C=C和-C=O的π-σ和π-π共轭键显示出很强的离域富电子结构，促进了钙钛矿层中的光生电荷载流子扩散。因此，TBA-PSC 的开路电压从 1.07 V 显着增加到 1.12 V，填充因子从 78.20 提高到 81.56%。因此，TBA-PSC 实现了 22.82% 的高功率转换效率，滞后可忽略不计。因此，TBA添加剂是提高高性能PSCs钙钛矿晶体质量的一种可行且有效的方法。
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