Upscaling efficient and stable perovskite layers is one of the most challenging issues in the commercialization of perovskite solar cells. Here, a lead halide–templated crystallization strategy is developed for printing formamidinium (FA)–cesium (Cs) lead triiodide perovskite films. High-quality large-area films are achieved through controlled nucleation and growth of a lead halide•N-methyl-2-pyrrolidone adduct that can react in situ with embedded FAI/CsI to directly form α-phase perovskite, sidestepping the phase transformation from δ-phase. A nonencapsulated device with 23% efficiency and excellent long-term thermal stability (at 85°C) in ambient air (~80% efficiency retention after 500 hours) is achieved with further addition of potassium hexafluorophosphate. The slot die–printed minimodules achieve champion efficiencies of 20.42% (certified efficiency 19.3%) and 19.54% with an active area of 17.1 and 65.0 square centimeters, respectively.
Among all inorganic halide perovskite photovoltaic materials, CsPbIBr2 exhibits the most balanced features in terms of bandgap and stability. However, the poor quality of solution‐processed CsPbIBr2 films impedes further optimization of cells performance. Herein, a facile intermolecular exchange strategy for CsPbIBr2 film is demonstrated, wherein an optimized methanol solution of CsI is spin‐coated on CsPbIBr2 precursor film in conventional one‐step solution route. It surprisingly produces full‐coverage and pure‐phase CsPbIBr2 films featured with average grain size of ≈0.65 µm, few grain boundaries, high crystallinity, preferable (100) orientation, stoichiometric composition along with favorable electronic structures for effective dissociation and transfer of carriers. Hence, the cost‐effective, carbon‐based all‐inorganic planar perovskite solar cells based on them, yield an optimized efficiency of 9.16% with a stabilized value of 8.46% in ambient air conditions that highlight a particularly superb open‐circuit voltage of 1.245 V, all of which represent the highest values reported in pure CsPbIBr2 based cells so far. Moreover, the optimized cell without encapsulation shows excellent long‐term stability because it can retain 90% over 60 days and 97% over 7 days of its initial efficiency, when is stored controllably in ≈45% relative humidity at 25 or 85 °C at zero humidity, respectively.
NiOx hole transporting layer has been extensively studied in optoelectronic devices. In this paper, the low temperature, solution–combustion‐based method is employed to prepare the NiOx hole transporting layer. The resulting NiOx thin films show better quality and preferable energy alignment with perovskite thin film compared to high temperature sol–gel‐processed NiOx. With this, high‐performance perovskite solar cells are fabricated successfully with power conversion efficiency exceeding 20% using a modified two‐step prepared MA1−yFAyPbI3−xClx perovskite. This efficiency value is among the highest values for NiOx‐based devices. Various characterizations and analyses provide evidence of better film quality, enhanced charge transport and extraction, and suppressed charge recombination. Meanwhile, the device exhibits much better device stability compared to sol–gel‐processed NiOx and poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate)‐based devices.
Recent research shows that the interface state in perovskite solar cells is the main factor which affects the stability and performance of the device, and interface engineering including strain engineering is an effective method to solve this issue. In this work, a CsBr buffer layer is inserted between NiOx hole transport layer and perovskite layer to relieve the lattice mismatch induced interface stress and induce more ordered crystal growth. The experimental and theoretical results show that the addition of the CsBr buffer layer optimizes the interface between the perovskite absorber layer and the NiOx hole transport layer, reduces interface defects and traps, and enhances the hole extraction/transfer. The experimental results show that the power conversion efficiency of optimal device reaches up to 19.7% which is significantly higher than the efficiency of the device without the CsBr buffer layer. Meanwhile, the device stability is also improved. This work provides a deep understanding of the NiOx/perovskite interface and provides a new strategy for interface optimization.
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