The lead-free inorganic perovskite CsSnI3 is considered as one of the best candidates for emerging photovoltaics. Nevertheless, CsSnI3-based perovskite solar cells experience a significant drop in performance due to the nonradiative recombination facilitated by trapping. Here, we show an electron donor passivation method to regulate deep-level defects for CsSnI3 perovskite with electron donor pyrrole. Experimental observations combined with theoretical simulations verify that the saturation of Tin dangling bonds with pyrrole on the CsSnI3 surface via a Lewis acid-base addition reaction can significantly reduce the density of deep-level defects. Consequently, the printable mesoporous perovskite solar cells with an FTO/compact-TiO2/mesoporous-TiO2/Al2O3/NiO/carbon framework device structure penetrated with CsSnI3 achieve a power conversion efficiency of up to 10.11%. To our knowledge, this represents the highest efficiency reported to date for lead-free perovskite-based printable mesoporous solar cells. Furthermore, the unencapsulated devices demonstrated remarkable long-term stability, retaining 92% of their initial efficiency even after 2400 h of aging in a nitrogen atmosphere.
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