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.

Inspired by the structural feature of the classical hole-transport material (HTM), Spiro-OMeTAD, many analogues based on a highly symmetrical spiro-core were reported for perovskite solar cells (PSCs). However, these HTMs were prone to crystallize because of the high molecular symmetry, forming non-uniform films, unfavorable for the device stability and large-area processing. By lowering the symmetry of spiro-core, we report herein a novel spirobisindane-based HTM, Spiro-I, which could form amorphous films with high uniformity and morphological stability. Compared to the Spiro-OMeTAD-based PSCs, those containing Spiro-I exhibit similar efficiencies for small area but higher ones for large area (1 cm ), and especially much higher air stability (retaining 80 % of initial PCE after 2400 h storage without encapsulation). Moreover, the Spiro-I can be synthesized from a cheap starting material bisphenol A and used with a small amount for the device fabrication.

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