Abstract

AbstractThe poor interface quality between cesium lead triiodide (CsPbI3) perovskite and the electron transport layer limits the stability and efficiency of CsPbI3 perovskite solar cells (PSCs). Herein, a 4‐amino‐2,3,5,6‐tetrafluorobenzoate cesium (ATFC) is designed as a bifacial defect passivator to tailor the perovskite/TiO2 interface. The comprehensive experiments demonstrate that ATFC can not only optimize the conductivity, electron mobility, and energy band structure of the TiO2 layer by passivation of the undercoordinated Ti4+, oxygen vacancy (VO), and free OH defects but also promote the yield of high‐quality CsPbI3 film by synergistic passivation of undercoordinated Pb2+ defects with the CO group and F atom, and limiting I− migration via F···I interaction. Benefiting from the above interactions, the ATFC‐modified CsPbI3 device yields a champion power conversion efficiency (PCE) of 21.11% and an excellent open‐circuit voltage (VOC) of 1.24 V. Meanwhile, the optimized CsPbI3 PSC maintains 92.74% of its initial efficiency after aging 800 h in air atmosphere, and has almost no efficiency attenuation after tracking at maximum power point for 350 h.

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