Dion-Jacobson (DJ) phase and Ruddlesden-Popper phase 2D perovskites have been, individually, demonstrated to be more stable than 3D counterparts for perovskite solar cells (PSCs). In order to further improve the efficiency and stability of 2D PSCs, we herein report merging them to construct a DJ:RP double-phase perovskite (DPP) structure for the first time. With the DJ 2D perovskite composed of diammonium as the matrix, a monoammonium with a larger size than the diammonium is incorporated to form an independent RP phase 2D perovskite coexisting with the DJ one (DJ:RP DPP structure), which facilitates crystal growth, suppresses charge recombination, and improves charge transport. As a comparison, introduction of a smaller monoammonium than the diammonium leads to its insertion between inorganic slabs, yielding a distorted DJ 2D perovskite structure, which induces lattice relaxation/distortion and thus lowered charge transportation. Consequently, 2D PSCs based on the DJ:RP DPP afford an impressive efficiency of 13.8% with excellent thermal stability at 85 °C in damp air. This work demonstrates a new and promising strategy of developing the DJ:RP DPP for highly efficient and robust 2D PSCs.

Dion-Jacobson (DJ) 相和 Ruddlesden-Popper 相 2D 钙钛矿已单独证明比钙钛矿太阳能电池 (PSC) 的 3D 对应物更稳定。为了进一步提高二维 PSC 的效率和稳定性，我们在此首次报告将它们合并以构建 DJ:RP 双相钙钛矿 (DPP) 结构。以二铵组成的DJ 2D钙钛矿为基体，掺入比二铵大的单铵，形成独立的RP相二维钙钛矿与DJ一共存（DJ:RP DPP结构），促进晶体生长，抑制电荷重组，改善电荷传输。作为比较，引入比二铵更小的单铵导致其插入无机板之间，产生扭曲的 DJ 2D 钙钛矿结构，这会导致晶格弛豫/畸变，从而降低电荷传输。因此，基于 DJ:RP DPP 的 2D PSC 提供了令人印象深刻的 13.8% 的效率，并在潮湿空气中在 85°C 下具有出色的热稳定性。这项工作展示了一种新的、有前途的策略，即为高效和强大的 2D PSC 开发 DJ:RP DPP。