Surface Reconstruction and In Situ Formation of 2D Layer for Efficient and Stable 2D/3D Perovskite Solar Cells

The 2D/3D composite structure possesses both the excellent stability of 2D perovskite and the excellent performance of 3D perovskite, which recently have attracted special attention. Different from the popular isopropanol, a novel additive solvent-polypropylene glycol bis (2-aminopropyl ether) (A-PPG) is introduced here to dissolve excess PbI₂ and perovskite, and then reconstruct and in situ form the quasi-2D perovskite layer on 3D perovskite bulk. The lone electron pairs of the ether-oxygen and amino in A-PPG can form coordination bonds with Pb²⁺ . The introduction of A-PPG tunes the energy array of functional layers, passivates defects, and mitigates carrier nonradiative recombination. Consequently, the 2D/3D perovskite device exhibits a championship efficiency of 22.24% with a distinguished open-circuit voltage of 1.21 V (the thermodynamic limit of 1.30 V). Moreover, the 2D/3D device still maintains 90% of the original efficiency in the ambient atmosphere with a relative humidity of 30 ± 10% after 50 days.