Reducing Photovoltaic Property Loss of Organic Solar Cells in Blade‐Coating by Optimizing Micro‐Nanomorphology via Nonhalogenated Solvent

Blade‐coating which is compatible with roll‐to‐roll (R2R) fabrication has been considered a promising technology for the large‐scale production of organic solar cells (OSCs). Despite the rapid increase in power conversion efficiency (PCE) of the devices, most processing solvents are still halogenated, which is a key issue that needs to be addressed urgently in commercialized manufacturing. In this work, targeted strategies are explored for the preparation of efficient OSCs via combining the nonhalogenated solvent toluene (TL) with blade‐coating. Based on the in situ UV–vis absorption, grazing‐incidence wide‐angle X‐ray scattering, and device performance measurements, the subtle relationship between processing solvents, film morphology, and properties is successfully established. The PM6:BTP‐eC9 blend film prepared by this strategy demonstrates higher crystallinity and smaller phase separation morphology, resulting in an outstanding PCE of 16.58% with low energy loss and high fill factor, which is higher than the CF‐based device (15.08%). Finally, the 1.00 cm2 device exhibits a high PCE of 14.82%, which is one of the highest values for OSCs prepared by blade‐coating based on TL solvent. This specific strategy combines blade‐coating with nonhalogenated solvent processing shows outstanding synergy in optimization of morphology, demonstrating excellent potential for the preparation of highly efficient large area OSCs. A targeted strategy for the preparation of large‐area films is proposed by combining blade‐coating technology with a green solvent. Because of suitable crystallization kinetics and phase separation morphology of the films, high power conversion efficiencies are achieved with 16.58% for 0.04 cm2 and 14.82% for 1.00 cm2, which are the leading results of organic solar cells based on blade‐coating.