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Comprehensive Summary: Formamidinium (FA)‐based Sn‐Pb perovskite solar cells (FAPb0.5Sn0.5I3 PSCs) with ideal bandgap and impressive thermal stability have caught enormous attention recently. However, it still suffers from the challenge of realizing high efficiency due to the surface imperfections of the transport materials and the energy‐level mismatch between functional contacts. Herein, it is demonstrated that the modification on buried interface with alkali metal salts is a viable strategy to alleviate these issues. We systematically investigate the role of three alkali metal bromide salts (NaBr, KBr, CsBr) by burying them between the NiOx hole transport layer (HTL) and the perovskite light‐absorbing layer, which can effectively passivate interface defects, improve energy‐level matching and release the internal residual strain in perovskite layers. The device with CsBr buffer layer exhibits the best power conversion efficiency (PCE) approaching 20%, which is one of the highest efficiencies for FA‐based Sn‐Pb PSCs employing NiOx HTLs. Impressively, the long‐term storage stability of the unencapsulated device is also greatly boosted. Our work provides an efficient strategy to prepare desired FA‐based ideal‐bandgap Sn‐Pb PSCs which could be applied in tandem solar cells. [ABSTRACT FROM AUTHOR]

We report a solution-processing method to prepare an inorganic LaNiO3 (LNO) hole-transport layer (HTL) under low temperature (<150 °C) for the first time. The inverted PSCs prepared with LNO exhibit high UV-stability and promising efficiency (17.15%). Our preliminary results show great potential for LNO HTL in the fabrication of efficient and photostable inverted perovskite solar cells (PSCs). [ABSTRACT FROM AUTHOR]

Zinc oxide (ZnO) is an appealing electron transport layer for inorganic perovskite solar cells (IPSCs). However, attempts to achieve high device performance have been undermined by the imperfections at the ZnO/perovskite interface, including the intrinsic defects of ZnO and the nonideal contact between ZnO and perovskite films, which can cause severe interfacial recombination losses. With the purpose of resolving these problems, cesium salts with functional anions of acetate (Ac−), fluoride (F−) and trifluoroacetate (TFA−) are explored to modulate the deposition of ZnO films. It is evidenced that these functional anions can coordinate with both Zn2+ and Pb2+ ions, causing defect passivation of the ZnO and the top perovskite films to different extents. Meanwhile, the Cs+ ions can reduce the hydroxyl defects and form an interfacial dipole on the surface of ZnO via Zn–O–Cs bonds. Therefore, more stable and efficient interfacial electron transport can be established. Accordingly, we obtained a maximum power conversion efficiency (PCE) of 14.25% in low-temperature carbon-based IPSCs (C-IPSCs) using a CsPbI2Br light absorber. This PCE is the highest value among all the ZnO-based C-IPSCs reported to date. Moreover, the corresponding devices without encapsulation demonstrate improved long-term stability in ambient air. [ABSTRACT FROM AUTHOR]

Carbon-based CsPbI2Br perovskite solar cells (PSCs) have attracted widespread attention due to their low cost and superior thermal stability. Unfortunately, the bulk defects and interfacial energy level mismatch limit the improvement of device performance. To solve the above issues, we introduce aromatic phenylethylammonium halides (PEAI and PEABr) and their fluorinated derivatives of 4-fluorophenylethylammonium halides (P-F-PEAI and P-F-PEABr) as a passivation layer to post-treat low-temperature CsPbI2Br films. Benefiting from reduced perovskite defects and better energy level alignments, the charge non-radiative recombination is effectively suppressed, and the hole extraction is promoted. Compared with the reference PSCs, the optimized devices achieve a maximum power conversion efficiency (PCE) of 13.97%. To the best of our knowledge, it should be one of the highest PCEs reported among those of low-temperature carbon-based CsPbI2Br PSCs. In addition, nonencapsulated devices exhibit improved moisture and thermal stability in ambient air. [ABSTRACT FROM AUTHOR]

In perovskite solar cells (PSCs), a defective perovskite (PVK) surface and cliff‐like energy offset at the interface always slow down the charge extraction; meanwhile, interface ion diffusion causes oxidation of the metal electrode, inducing device instability. Here, the in situ grown 2D‐(CH3NH2)3Sb2I9 (MA3Sb2I9) on the back surface of MAPbI3 results in a more robust interface. MA3Sb2I9 changes the MAPbI3 surface to p‐type and thus acts like a back surface field to drive charge extraction and suppress recombination, resulting in an obviously higher fill factor (FF) = 0.8 and power conversion efficiency (PCE) = 20.4% of SnO2/MAPbI3/MA3Sb2I9/Spiro‐OMeTAD (2,2′,7,7′‐Tetrakis[N,N‐di(4‐methoxyphenyl)amino]‐9,9′‐spirobifluorene) PSC than the pure MAPbI3 device. More importantly, strong chemical bonding of SbI prohibits ion diffusion, largely enhancing the thermal stability and longtime stability. Here, special 2D‐MA3Sb2I9 constructs' robust band alignment and chemical environment at the interface are highlighted for efficient and stable PSCs. [ABSTRACT FROM AUTHOR]

Comprehensive Summary: Formamidinium (FA)‐based Sn‐Pb perovskite solar cells (FAPb0.5Sn0.5I3 PSCs) with ideal bandgap and impressive thermal stability have caught enormous attention recently. However, it still suffers from the challenge of realizing high efficiency due to the surface imperfections of the transport materials and the energy‐level mismatch between functional contacts. Herein, it is demonstrated that the modification on buried interface with alkali metal salts is a viable strategy to alleviate these issues. We systematically investigate the role of three alkali metal bromide salts (NaBr, KBr, CsBr) by burying them between the NiOx hole transport layer (HTL) and the perovskite light‐absorbing layer, which can effectively passivate interface defects, improve energy‐level matching and release the internal residual strain in perovskite layers. The device with CsBr buffer layer exhibits the best power conversion efficiency (PCE) approaching 20%, which is one of the highest efficiencies for FA‐based Sn‐Pb PSCs employing NiOx HTLs. Impressively, the long‐term storage stability of the unencapsulated device is also greatly boosted. Our work provides an efficient strategy to prepare desired FA‐based ideal‐bandgap Sn‐Pb PSCs which could be applied in tandem solar cells. [ABSTRACT FROM AUTHOR]

The power conversion efficiency (PCE) of perovskite solar cells (PSCs) is approaching their Shockley‐Queisser (S‐Q) limit through numerous efforts in key parameters improvement. To further approaching the limit, it is important to facilitate the fill factor (FF), a parameter closely related to carrier transport and nonradiative recombination. Herein, an interfacial bridging strategy is proposed to improve FF, which utilizes functional graphene quantum dots at the tin oxide (SnO2)/perovskite buried interface. As a result, synergistic effects of enhanced conductivity of SnO2, preferable energy alignment at the buried interface and improved perovskite crystal orientation are realized. The champion FF reaches 85.24% in formamidinium lead iodide (FAPbI3) based PSCs, which ranks among the highest in the n‐i‐p structure. Such strategy is also proven successful in other perovskite systems, where the champion PCE reaches 24.86% in the formamidinium‐cesium (FACs)‐based devices and 24.44% in the flexible devices. Therefore, this work provides a practical design rule for pursuing high FF of PSCs with carbon materials. [ABSTRACT FROM AUTHOR]

We report a solution-processing method to prepare an inorganic LaNiO 3 (LNO) hole-transport layer (HTL) under low temperature (<150 °C) for the first time. The inverted PSCs prepared with LNO exhibit high UV-stability and promising efficiency (17.15%). Our preliminary results show great potential for LNO HTL in the fabrication of efficient and photostable inverted perovskite solar cells (PSCs).

Buried interface modification is promising for preparing high-performance perovskite solar cells (PSCs) by improving the film quality and adjusting the interfacial energy level alignment. In this work, multifunctional ethylenediaminetetraacetic acid diammonium (EAD)-modulated ZnO is employed as an effective buried interface to regulate the interplay between SnO 2 and CsPbI 2 Br in carbon-based inorganic PSCs (C-IPSCs). The burying of EAD into the ZnO interlayer not only enhances the photoelectric properties of ZnO by passivating oxygen defects but also adjusts the energy level alignment of the buried interface. More importantly, the perovskite quality is optimized and the buried interface defects are passivated due to the formation of coordination and hydrogen bondings. Benefiting from such a robust and efficient charge transfer configuration, a maximum power conversion efficiency of 14.58% is achieved in the optimized device, which represents the highest performance reported among those of low-temperature CsPbI 2 Br C-IPSCs. In addition, the unencapsulated device demonstrates better long-term and thermal stability.

The charge recombination resulting from bulk defects and interfacial energy level mismatch hinders the improvement of the power conversion efficiency (PCE) and stability of carbon-based inorganic perovskite solar cells (C-IPSCs). Herein, a series of small molecules including ethylenediaminetetraacetic acid (EDTA) and its derivatives (EDTA-Na and EDTA-K) are studied to functionalize the zinc oxide (ZnO) interlayers at the SnO 2 /CsPbI 2 Br buried interface to boost the photovoltaic performance of low-temperature C-IPSCs. This strategy can simultaneously passivate defects in ZnO and perovskite films, adjust interfacial energy level alignment, and release interfacial tensile stress, thereby improving interfacial contact, inhibiting ion migration, alleviating charge recombination, and promoting electron transport. As a result, a maximum PCE of 13.94% with a negligible hysteresis effect is obtained, which is one of the best results reported for low-temperature CsPbI 2 Br C-IPSCs so far. Moreover, the optimized devices without encapsulation demonstrate greatly improved operational stability., (© 2022 Wiley-VCH GmbH.)

N-type tin oxide (SnO 2 ) films are commonly used as an electron transport layer (ETL) in perovskite solar cells (PSCs). However, SnO 2 films are of poor quality due to facile agglomeration under a low-temperature preparation method. In addition, energy level mismatch between the SnO 2 and perovskite (PVK) layer as well as interfacial charge recombination would cause open-circuit voltage loss. In this work, alkali metal oxalates (M-Oxalate, M = Li, Na, and K) are doped into the SnO 2 precursor to solve these problems. First, it is found that the hydrolyzed alkali metal cations tend to change colloid size distribution of SnO 2 , in which Na-Oxalate with suitable basicity leads to most uniform colloid size distribution and high-quality SnO 2 -Na films. Second, the electron conductivity is enhanced by slightly agglomerated SnO 2 -Na, which facilitates the transmission of electrons. Third, alkali metal cations increase the conduction band level of SnO 2 in the sequence of K + , Na + , and Li + to promote band alignment between ETLs and perovskite. Based on the optimized film quality and energy states of SnO 2 -Na, the best PSC efficiency of 20.78% is achieved with a significantly enhanced open-circuit voltage of 1.10 V. This work highlights the function of alkali metal salts on the colloid particle distribution and energy level modulation of SnO 2 .

Defective grain boundaries (GBs) and surface trap states are detrimental to the efficiency and stability of perovskite solar cells (PSCs). In this research, ionic liquid (IL) is used to control the defect states at the perovskite surface and GBs. The newly formed (EMIm) x MA 1- x Pb[(BF 4 ) x I 1- x ] 3 interlayer promotes secondary grain growth to diminish GBs; besides, EMIM + and BF 4 - fill the vacancies of MA + and I - and also passivate undercoordinated Pb 2+ trap states. The newly formed interface largely reduces the nonradiative recombination, thus enhancing the solar-cell performance to 19.0% (AM 1.5, 1 sun) with higher photovoltage and fill factor than the control device. Due to the hydrophobicity of the (EMIm) x MA 1- x Pb[(BF 4 ) x I 1- x ] 3 interlayer, the unencapsulated device stability in 30 days is much better than the control device under relative humidity (RH) = 20%. This work highlights IL-induced secondary grain growth and a defect passivation method for efficient and stable PSCs.