Abstract
Although ionic liquids (ILs) have been widely employed to heal the defects in perovskite solar cells (PSCs), the corresponding defect passivation mechanisms are not thoroughly understood up to now. Herein, we first reveal an abnormal buried interface anion defect passivation mechanism depending on cation-induced steric hindrance. The IL molecules containing the same anion ([BF4]-) and different sizes of imidazolium cations induced by substituent size are used to manipulate buried interface. It was revealed what passivated interfacial defects is mainly anions instead of cations. Theoretical and experimental results demonstrate that the large-sized cations can weaken the ionic bond strength between anions and cations, and facilitate the interaction between anions and SnO2 as well as perovskites, which is conducive to interfacial defect passivation and ameliorating interfacial contact. It can be concluded that interfacial chemical interaction strength and defect passivation effect are positively correlated with the size of cations. The discovery breaks conventional thinking that large-sized modification molecules would weaken their chemical interaction with perovskite. Compared with the control device (21.54%), the device based on 1,3-Bis(1-adamantyl)-imidazolium tetrafluoroborate (BAIMBF4) with maximum size cations achieves a significantly enhanced efficiency of 23.61% along with much increased moisture, thermal and light stabilities.
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