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All‐inorganic CsPbI3 perovskite presents preeminent chemical stability and a desirable band gap as the front absorber for perovskite/silicon tandem solar cells. Unfortunately, CsPbI3 perovskite solar cells (PSCs) still show low efficiency due to high density of defects in solution‐prepared CsPbI3 films. Herein, three kinds of hydrazide derivatives (benzoyl hydrazine (BH), formohydrazide (FH) and benzamide (BA)) are designed to reduce the defect density and stabilize the phase of CsPbI3. Calculation and characterization results corroborate that the carboxyl and hydrazine groups in BH form strong chemical bonds with Pb2+ ions, resulting in synergetic double coordination. In addition, the hydrazine group in the BH also forms a hydrogen bond with iodine to assist the coordination. Consequently, a high efficiency of 20.47 % is achieved, which is the highest PCE among all pure CsPbI3‐based PSCs reported to date. In addition, an unencapsulated device showed excellent stability 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]

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]

Formamidinium methylammonium lead iodide (FAMAPbI3) perovskite has been intensively investigated as a potential photovoltaic material because it has higher phase stability than its pure FAPbI3 perovskite counterpart. However, its power conversion efficiency (PCE) is significantly inferior due to its high density of surface detects and mismatched energy level with electrodes. Herein, a bifunctional passivator, methyl haloacetate (methyl chloroacetate, (MClA), methyl bromoacetate (MBrA)), is designed to reduce defect density, to tune the energy levels and to improve interfacial charge extraction in the FAMAPbI3 perovskite cell by synergistic passivation of both CO groups and halogen anions. As predicted by modeling undercoordinated Pb2+, the MBrA shows a very strong interaction with Pb2+ by forming a dimer complex ([C6H10Br2O4Pb]2+), which effectively reduces the defect density of the perovskite and suppresses non‐radiative recombination. Meanwhile, the Br− in MBrA passivates iodine‐deficient defects. Consequently, the MBrA‐modified device presents an excellent PCE of 24.29%, an open‐circuit voltage (Voc) of 1.18 V (Voc loss ≈ 0.38 V), which is one of the highest PCEs among all FAMAPbI3‐based perovskite solar cells reported to date. Furthermore, the MBrA‐modified devices without any encapsulation exhibit remarkable long‐term stability with only 9% of PCE loss after exposure to ambient air for 1440 h. [ABSTRACT FROM AUTHOR]

Inorganic CsPbI2Br perovskite is promising for solar cell applications due to its excellent thermal stability and optoelectronic characteristics. Unfortunately, the current high‐efficiency CsPbI2Br perovskite solar cells (PSCs) are mostly fabricated in an inert atmosphere due to their instability to moisture. Herein, a low‐dimensional intermediate‐assisted growth (LDIAG) method is reported for the deposition of CsPbI2Br film in ambient atmosphere by introducing imidazole halide (IMX: IMI and IMBr) into the precursor solution to control both nucleation and growth kinetics. The IMX first combines with PbI2 in the precursor film to form a 2D intermediate which then gradually releases PbI2 to slowly form high‐quality CsPbI2Br film during annealing. It is found that the LDIAG method produces a uniform, highly crystalline, pinhole‐free, and stable CsPbI2Br film with low defect density. Consequently, the solar cell efficiency is increased to as high as 17.26%, one of the highest for this type of device. Furthermore, the bare device without any encapsulation shows excellent long‐term stability with ≈86% of its initial efficiency retained after being exposed to the ambient environment for 1000 h. This work provides a perspective to tune the intermediate phases and crystallization pathway for high‐performance inorganic PSCs formed under ambient conditions. [ABSTRACT FROM AUTHOR]

Highlights: A series of 10 imidazolium-based ionic liquids (IILs) with different cations and anions have applied to unravel the passivation mechanism of the IILs on CsPbI2Br inorganic perovskites. It is found that anions of IILs play a more important role in passivation of lead- and cesium-related defects in inorganic perovskite compared with imidazole cations because they can form strong ionic interactions (Pb-F, Cs-F). A high-power conversion efficiency of 17.02% is obtained, which is among the highest values of CsPbI2Br-based perovskite solar cells. The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells (PSCs). However, the detailed mechanisms behind the improvement remain mysterious. Herein, a series of imidazolium-based ionic liquids (IILs) with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites. It is found that IILs display the following advantages: (1) They form ionic bonds with Cs+ and Pb2+ cations on the surface and at the grain boundaries of perovskite films, which could effectively heal/reduce the Cs+/I− vacancies and Pb-related defects; (2) They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer; and (3) They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI2Br PSCs. The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI2Br PSCs and an impressive power conversion efficiency of 17.02%. Additionally, the CsPbI2Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability. Our results provide guidance for an in-depth understanding of the passivation mechanism of IILs in inorganic perovskites. [ABSTRACT FROM AUTHOR]

Inorganic CsPbI2Br perovskite solar cells (PSCs) have gained enormous research interest due to their excellent thermal and light stabilities. However, their unsatisfactory power‐conversion efficiency and poor intrinsic phase stability remain roadblocks to their further development. Herein, Cs2PbI2Cl2 nanosheets (NSs) with the Ruddlesden–Popper (RP) structure are synthesized, and an NSs/CsPbI2Br/NSs heterostructure is employed to enhance both the stability and efficiency of CsPbI2Br solar cells. The novel Cs2PbI2Cl2 NSs can not only passivate the top and bottom surfaces of the perovskite film and top surface of the TiO2 film but also enhance the stability of the perovskite film. Based on the heterostructured NSs/CsPbI2Br/NSs inorganic perovskite film, the efficiency of the CsPbI2Br PSCs is improved from 15.02% to 16.65%. Moreover, the unencapsulated CsPbI2Br devices with the NSs/CsPbI2Br/NSs heterostructure sustain over 90% of their original efficiencies after being exposed to ambient conditions (≈25 °C and ≈35% RH) for 648 h. Both the UV‐light‐soaking stability (100 mW cm−1 365 nm UV light) and thermal stability (T = 85 °C) of the optimized devices are dramatically improved in comparison with their counterparts with only a 3D active layer. Therefore, this work promotes the application of RP inorganic perovskite nanocrystals in a range of perovskite optoelectronic devices. [ABSTRACT FROM AUTHOR]

Cesium lead triiodide (CsPbI 3 ) is a promising light-absorbing material for constructing perovskite solar cells (PSCs) owing to its favorable bandgap and thermal tolerance. However, the high density of defects in the CsPbI 3 film not only act as recombination centers, but also facilitate ion migration, leading to lower PCE and inferior stability compared with the state-of-the-art organic-inorganic hybrid PSC counterpart. Theoretical analyses suggest that the effective suppression of defects in CsPbI 3 film is helpful for improving the device performance. Herein, the stable and efficient γ -CsPbI 3 PSCs are demonstrated by developing an acyloin ligand (1,2-di(thiophen-2-yl)ethane-1,2-dione (DED)) as a phase stabilizer and defect passivator. The experiment and calculation results confirm that carbonyl and thienyl in DED can synergistically interact with CsPbI 3 by forming a chelate to effectively passivate Pb-related defects and further suppress ion migration. Consequently, DED-treated CsPbI 3 PSCs yield a champion PCE of 21.15%, which is one of the highest PCE among all the reported CsPbI 3 PSCs to date. In addition, the unencapsulated DED-CsPbI 3 PSC can retain 94.9% of itsinitial PCE when stored under ambient conditions for 1000 h and 92.8% of its initial PCE under constant illumination for 250 h., (© 2023 Wiley-VCH GmbH.)

The application of ionic liquids in perovskite has attracted wide-spread attention for its astounding performance improvement of perovskite solar cells (PSCs). However, the detailed mechanisms behind the improvement remain mysterious. Herein, a series of imidazolium-based ionic liquids (IILs) with different cations and anions is systematically investigated to elucidate the passivation mechanism of IILs on inorganic perovskites. It is found that IILs display the following advantages: (1) They form ionic bonds with Cs + and Pb 2+ cations on the surface and at the grain boundaries of perovskite films, which could effectively heal/reduce the Cs + /I - vacancies and Pb-related defects; (2) They serve as a bridge between the perovskite and the hole-transport-layer for effective charge extraction and transfer; and (3) They increase the hydrophobicity of the perovskite surface to further improve the stability of the CsPbI 2 Br PSCs. The combination of the above effects results in suppressed non-radiative recombination loss in CsPbI 2 Br PSCs and an impressive power conversion efficiency of 17.02%. Additionally, the CsPbI 2 Br PSCs with IILs surface modification exhibited improved ambient and light illumination stability. Our results provide guidance for an in-depth understanding of the passivation mechanism of IILs in inorganic perovskites., (© 2021. The Author(s).)