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With the rapid rise in perovskite solar cells (PSCs) performance, it is imperative to develop scalable fabrication techniques to accelerate potential commercialization. However, the power conversion efficiencies (PCEs) of PSCs fabricated via scalable two-step sequential deposition lag far behind the state-of-the-art spin-coated ones. Herein, the additive methylammonium chloride (MACl) is introduced to modulate the crystallization and orientation of a two-step sequential doctor-bladed perovskite film in ambient conditions. MACl can significantly improve perovskite film quality and increase grain size and crystallinity, thus decreasing trap density and suppressing nonradiative recombination. Meanwhile, MACl also promotes the preferred face-up orientation of the (100) plane of perovskite film, which is more conducive to the transport and collection of carriers, thereby significantly improving the fill factor. As a result, a champion PCE of 23.14% and excellent long-term stability are achieved for PSCs based on the structure of ITO/SnO2/FA1-xMAxPb(I1-yBry)3/Spiro-OMeTAD/Ag. The superior PCEs of 21.20% and 17.54% are achieved for 1.03 cm2 PSC and 10.93 cm2 mini-module, respectively. These results represent substantial progress in large-scale two-step sequential deposition of high-performance PSCs for practical applications.

Perovskite solar cells (PSCs) have emerged as one of the most promising and competitive photovoltaic technologies, and doctor‐blading is a facile and robust deposition technique to efficiently fabricate PSCs in large scale, especially matching with roll‐to‐roll process. Herein, it demonstrates the encouraging results of one‐step, antisolvent‐free doctor‐bladed methylammonium lead iodide (CH3NH3PbI3, MAPbI3) PSCs under a wide range of humidity from 45% to 82%. A synergy strategy of ionic‐liquid methylammonium acetate (MAAc) and molecular phenylurea additives is developed to modulate the morphology and crystallization process of MAPbI3 perovskite film, leading to high‐quality MAPbI3 perovskite film with large‐size crystal, low defect density, and ultrasmooth surface. Impressive power conversion efficiency (PCE) of 20.34% is achieved for doctor‐bladed PSCs under the humidity over 80% with a device structure of ITO/SnO2/MAPbI3/Spiro‐OMeTAD/Ag. It is the highest PCEs for one‐step solution‐processed MAPbI3 PSCs without antisolvent assistance. The research provides a facile and robust large‐scale deposition technique to fabricate highly efficient and stable PSCs under a wide range of humidity, even with the humidity over 80%.

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