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The performance of large‐area perovskite solar cells (PSCs) has been assessed for typical compositions, such as methylammonium lead iodide (MAPbI₃), using a blade coater, slot‐die coater, solution shearing, ink‐jet printing, and thermal evaporation. However, the fabrication of large‐area all‐inorganic perovskite films is not well developed. This study develops, for the first time, an eco‐friendly solvent engineered all‐inorganic perovskite ink of dimethyl sulfoxide (DMSO) as a main solvent with the addition of acetonitrile (ACN), 2‐methoxyethanol (2‐ME), or a mixture of ACN and 2‐ME to fabricate large‐area CsPbI_2.77Br_0.23films with slot‐die coater at low temperatures (40–50 °C). The perovskite phase, morphology, defect density, and optoelectrical properties of prepared with different solvent ratios are thoroughly examined and they are correlated with their respective colloidal size distribution and solar cell performance. The optimized slot‐die‐coated CsPbI_2.77Br_0.23perovskite film, which is prepared from the eco‐friendly binary solvents dimethyl sulfoxide:acetonitrile (0.8:0.2 v/v), demonstrates an impressive power conversion efficiency (PCE) of 19.05%. Moreover, the device maintains ≈91% of its original PCE after 1 month at 20% relative humidity in the dark. It is believed that this study will accelerate the reliable manufacturing of perovskite devices.

Poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is a popular hole transport material in perovskite solar cells (PSCs). However, the devices with PEDOT:PSS exhibit large open‐circuit voltage (V_oc) loss and low efficiency, which is attributed to mismatched energy level alignment and the poor interface of PEDOT:PSS and perovskite. Here, three polymer analogues to polyaniline (PANI), PANI–carbazole (P1), PANI–phenoxazine (P2), and PANI–phenothiazine (P3) are designed with different energy levels to modify the interface between PEDOT:PSS and the perovskite layer and improve the device performance. The effects of the polymers on the device performance are demonstrated by evaluating the work function adjustment, perovskite growth control, and interface modification in MAPbI₃‐based PSCs. Low bandgap Sn–Pb‐based PSCs are also fabricated to confirm the effects of the polymers. Three effects are evaluated through the comparison study of PEDOT:PSS‐based organic solar cells and MAPbI₃ PSCs based on the PEDOT:PSS modified by P1, P2, and P3. The order of contribution for the three effects is work function adjustment > surface modification > perovskite growth control. MAPbI₃ PSCs modified with P2 exhibit a highV_ocof 1.13 V and a high‐power conversion efficiency of 21.06%. This work provides the fundamental understanding of the interface passivation effects for PEDOT:PSS‐based optoelectronic devices.