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Surface passivation by constructing a 2D/3D structure is considered to be an effective strategy for suppressing non-radiative recombination and improving the device efficiency and stability. Herein, the 2D perovskite is formed in situ on the surface of a 3D perovskite via chemical interactions between diethylammonium iodide (DAI) and Pb–I octahedra, which greatly reduces the deep level defects and non-radiative recombination. Moreover, the 2D/3D structure can regulate the energy level alignment, enhance the charge extraction, and improve the open-circuit voltage. Finally, compared with the control device, the power conversion efficiency (PCE) of the DAI-treated device increases from 21.58 to 23.50%. The unencapsulated devices stored in air for more than 500 hours can still retain 97% of their initial PCE, revealing good long-term placement stability. This work provides a promising strategy to fabricate efficient PSCs through the in situ construction of 2D/3D perovskite heterojunctions. [ABSTRACT FROM AUTHOR]

The industrialization of perovskite solar cells (PSCs) is based on the development of efficiency and stability. Here, a composite film of a polyethylenimine ethoxylated (PEIE) and tellurophene-based two-dimensional metal–organic framework (2D MOF) was introduced to realize the nondestructive passivation of TiO2. This interfacial layer can not only realize the effective passivation of TiO2, but can also further improve the morphology of the perovskite film. After the modification of the PEIE-2D MOF composite film, the morphology and crystallinity of the perovskite film are greatly optimized, the trap states in the TiO2 layer are reduced, and the electron transport in the device is enhanced, thus finally achieving highly efficient and stable FA0.25MA0.75PbI3 PSCs with a maximum efficiency of 22.22%. It was demonstrated that the reduced trap states and the smooth surface of the TiO2 electron transport layer are the reasons for the high performance of modified PSCs. This method provides a new way for improving the interface state to achieve highly efficient and stable PSCs. [ABSTRACT FROM AUTHOR]