Solution-processed transition metal oxides (TMOs) prepared from complex ion precursors are developed as promising scalable interfacial layers for non-fullerene organic photovoltaics (OPVs); however, challenges remain in achieving defect-free and highly oriented metal-oxygen networks without post-deposition treatments due to the presence of residual organic metalbinding ligands in films. Herein, the novel strategy that the problematic organic metal-binding ligands in TMO precursors can be successfully eliminated by an anion-induced catalytic reaction (ACR) at room temperature is demonstrated, in which the low-level anions induce electron redistribution and instability of TMO precursors, expediting binding ligand removal during the hydrolysis reaction. The subsequent condensation process facilitates a dimensionally confined and continuous metal-oxygen network with a 20-fold increase in electrical conductivity (from 8.4 × 10 −4 to 1.8 × 10 −2 S m −1 ) and superior work function tunability (from 5.1 to 5.3 eV) compared to the pristine film. The ACR-derived TMO thin film on top of a ternary PBDB-TF:Y6:PC 71 BM photoactive layer enables an inverted device configuration with improved efficiency of 17.6%, as well as enhanced stability over 70% of the initial efficiency for up to 100 h AM 1.5G illumination.

Solar cells (PSCs) with quasi‐2D Ruddlesden–Popper perovskites (RPP) exhibit greater environmental stability than 3D perovskites; however, the low power conversion efficiency (PCE) caused by anisotropic crystal orientations and defect sites in the bulk RPP materials limit future commercialization. Herein, a simple post–treatment is reported for the top surfaces of RPP thin films (RPP composition of PEA2MA4Pb5I16 = 5) in which zwitterionic n‐tert‐butyl‐α‐phenylnitrone (PBN) is used as the passivation material. The PBN molecules passivate the surface and grain boundary defects in the RPP and simultaneously induce vertical direction crystal orientations of the RPPs, which lead to efficient charge transport in the RPP photoactive materials. With this surface engineering methodology, the optimized devices exhibit a remarkably enhanced PCE of 20.05% as compared with the devices without PBN (≈17.53%) and excellent long‐term operational stability with 88% retention of the initial PCE under continuous 1‐sun irradiation for over 1000 h. The proposed passivation strategy provides new insights into the development of efficient and stable RPP‐based PSCs.

Photoelectrochemical (PEC) water splitting based on organic semiconductors (OSs) is a promising way to enable sustainable hydrogen production because of its high photovoltaic performance and mass productivity by low-cost printing....

Solution-processed bathocuproine (BCP) has been widely used in fullerene (FA)-based organic solar cells (OSCs) for decades as an electron transport layer (ETL).

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