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Abstract The optimal selection of alkyl chains and halogen ions in ammonium salts for addressing specific defect types in perovskite films remains unclear, although ammonium salts emerged as a promising strategy to enhance the performance of perovskite solar cells (PSCs). Herein, four ammonium salts are introduced with different alkyl chain types and halogen ions to passivate perovskite films. Branched‐alkyl chain ammonium salts exhibited superior passivation effects compared to linear‐alkyl chain salts, with the alkyl chain structure having a more significant impact on device performance than the halogen ion component. In addition, DFT calculations are performed to investigate which defect types in perovskite films are most effectively passivated by different alkyl chain types and halogen ions in ammonium salts. Branched‐alkyl chain ammonium salts demonstrated superior passivation effects on V_Pband V_FAdefects in perovskite films compared to linear‐alkyl chain salts, while exhibiting similar passivation effects for V_Idefects. PSCs passivated with tert‐OAI achieved an impressive efficiency of 25.49%, with a V_ocof 1.19 V, a J_scof 25.40 mA cm⁻², and an FF of 84.34%. This work highlights a targeted ammonium salt passivation strategy tailored to address different defect types in perovskite films, accounting for variations in perovskite composition and fabrication environments. 

Abstract Dimethylammonium lead iodide (DMAPbI_x) has the potential to address the phase stability issue of inorganic perovskite solar cells (PSCs). In this study, the crystallinity, phase structure, defect states, and crystal growth habits of DMAPbI_xare controlled by adjusting thexvalue during synthesis, where N,N‐dimethylacetamide (DMAC) is used as the solvent to regulate perovskite film growth. Furthermore, large‐area CsPbI_2.85Br_0.15perovskite films with preferred oriented growth are achieved using the optimizedxvalue in DMAPbI_xthrough the slot‐die coating method. The inorganic PSCs, with a n‐i‐p structure and the active area of 0.04 cm², achieve a champion power conversion efficiency (PCE) of 19.82%, with an open‐circuit voltage (V_oc) of 1.16 V based on perovskite films formed by slot‐die coating. This work provides important insights into the DMAPbI_x‐based method for fabricating high‐quality inorganic perovskite films, and paves the way for large‐area inorganic PSCs fabrication for practical applications. 

Abstract 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.