Dion-Jacobson (DJ) phase 2D layered perovskites are developed by removing the van der Waals gap between organic layers and inorganic slabs in Ruddlesden-Popper (RP) phase counterparts. The hydrogen bonding formed at both sides of diammonium cations with perovskite layers in the DJ phase 2D perovskite endows it with extremely high structural stability, compared with that at only one side in the RP phase one. The devices exhibit a PCE of 13.3% with unprecedented stability, even when subjected to very harsh testing conditions.

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The inorganic hole transport layer of nickel oxide (NiOx) has shown highly efficient, low‐cost, and scalable in perovskite photovoltaics. However, redox reactions at the interface between NiOx and perovskites limit their commercialization. In this study, ABABr (4‐(2‐Aminoethyl) benzoic acid bromide) between the NiOx and different perovskite layers to address the issues has been introduced. How the ABABr interacts with NiOx and perovskites is experimentally and theoretically investigated. These results show that the ABABr molecule chemically reacts with the NiOx via electrostatic attraction on one side, whereas on the other side, it forms a strong hydrogen bond via the NH3+ group with perovskites layers, thus directly diminishing the redox reaction between the NiOx and perovskites layers and passivating the layer surfaces. Additionally, the ABABr interface modification leads to significant improvements in perovskite film morphology, crystallization, and band alignment. The perovskites solar cells (PSCs) based on an ABABr interface modification show power conversion efficiency (PCE) improvement by over 13% and maintain over 90% of its PCE after continuous operation at maximum power point for over 500 h. The work not only contributes to the development of novel interlayers for stable PSCs but also to the understanding of how to prevent interface redox reactions.

Developing dopant-free hole transporting materials (HTM) and passivating defects in perovskite films are two significant themes to realize efficient and stable perovskite solar cells (PSCs). Compared to various individual endeavors...