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CsPbI3 inorganic perovskites have attracted significant attention due to their desirable bandgap for tandem solar cells and excellent thermal stability. However, CsPbI3 perovskite solar cells (PSCs) still exhibit low efficiency and high energy loss due to nonradiative recombination. Herein, functionalized Ti3C2Fx quantum dots (QDs) are prepared and selected as interface passivators to enhance the performance of CsPbI3 PSCs. The systematic experimental results reveal that Ti3C2Fx QDs serve as effective passivators mainly in three aspects: 1) p‐type Ti3C2Fx QDs can tune the energy level of perovskite films and provide an efficient pathway for hole transfer; 2) Ti3C2Fx QDs can effectively passivate defects and reduce interfacial nonradiative recombination, and 3) Ti3C2Fx QDs form a barrier layer to prevent water invasion and improve the stability of CsPbI3 PSCs. Consequently, the champion CsPbI3 PSC with Ti3C2Fx QDs treatment exhibits an excellent efficiency of 20.44% with a high open‐circuit voltage of 1.22 V. Meanwhile, the corresponding device without encapsulation retained 93% of its initial efficiency after 600 h of storage in ambient air. [ABSTRACT FROM AUTHOR]

CsPbI2Br perovskite is known for its advantages over its organic‐inorganic hybrid counterpart including better thermal stability and appropriate bandgap for the front sub‐cell of tandem solar cell. However, its lower‐than‐satisfactory efficiency, problematic phase stability and sensitivity to moisture hinder its further advancement. Here, three kinds of glycine halides (Gly‐X: X = Cl, Br, and I) are strategically deigned to improve the performance of CsPbI2Br perovskite solar cells (PSCs). Systematic experimental and calculated results prove that a 2D/3D hybrid structure is formed, wherein the Gly‐X‐based 2D perovskite is mainly located at the CsPbI2Br grain boundaries, and the A‐sites of the 2D perovskite form strong bonds with the 3D perovskite to suppress ion migration by increasing its activation energy. As a result, a power conversion efficiency (PCE) of 17.26% was obtained with an open‐circuit voltage (VOC) of 1.33 V, which is among the best PCE values for the CsPbI2Br PSCs. In addition, the efficiency of encapsulated device decrease only by 14.1% after 340 h continuous illumination in ambient conditions, representing one of the most‐stable inorganic PSCs reported so far. This work provides important insights into designing passivating agents to address the issue of phase segregation for the development of highly stable perovskite optoelectronic devices. [ABSTRACT FROM AUTHOR]