A Special Additive Enables All Cations and Anions Passivation for Stable Perovskite Solar Cells with Efficiency over 23%

Passivating undercoordinated ions is an effective way to reduce the defect densities at the surface and grain boundaries (GBs) of perovskite materials for enhanced photovoltaic performance and stability of perovskite solar cells (PSCs). Here, (BBF) complex is chosen as a multifunctional additive, which contains both C(7)H(9)N and BF(3) groups working as Lewis base and Lewis acid, respectively, can bond with Pb(2+)/I(−) and FA(+) on the surface and in the GBs in the perovskite film, affording passivation of both cation and anion defects. The synergistic effect of the C(7)H(9)N and BF(3) complex slows the crystallization during the perovskite film deposition to improve the crystalline quality, which reduces the trap density and the recombination in the perovskite film to suppress nonradiative recombination loss and minimizes moisture permeation to improve the stability of the perovskite material. Meanwhile, such an additive improves the energy-level alignment between the valence band of the perovskite and the highest occupied molecular orbital of the hole-transporting material, Spiro-OMeTAD. Consequently, our work achieves power conversion efficiency of 23.24%, accompanied by enhanced stability under ambient conditions and light illumination and opens a new avenue for improving the performance of PSCs through the use of a multifunctional complex. [Image: see text] SUPPLEMENTARY INFORMATION: The online version contains supplementary material available at 10.1007/s40820-021-00688-2.