Novel C₃N₄-Assisted Bilateral Interface Engineering for Efficient and Stable Perovskite Solar Cells

g-C3N4-assisted interface engineering has been developed as an effective method to improve the efficiency and stability of perovskite solar cells (PSCs). However, most of the reported works used g-C3N4-induced single-interface modification, which is difficult to passivate the bilateral interfaces of the perovskite layer at the same time. In this paper, we fabricated two kinds of C3N4 materials simultaneously (w-CN and y-CN) after the twice calcination of melamine and used them in the bilateral interface modification toward all-inorganic PSCs. The two kinds of C3N4 play different roles in different interface engineering. On the front interface, w-CN could optimize band level arrangement and improve the perovskite film quality, which contributes to the efficiency of the device. On the back interface, y-CN could also improve the film quality of the perovskite layer, accelerating the extraction of charge carriers. The champion efficiency of the CsPbIBr2-based device treated by the bilateral interface is significantly enhanced from 7.8 to 10.1%. Moreover, the modified perovskite film exhibits negligible degradation after 40 min of exposure in the ambient environment with a relative humidity of 70%, while the pristine perovskite film has a rapid degradation within 20 min.