As perovskite solar cells (PSCs) are highly efficient, demonstration of high‐performance printed devices becomes important. 2D/3D heterostructures have recently emerged as an attractive way to relieving the film inhomogeneity and instability in perovskite devices. In this work, a 2D/3D ensemble with 2D perovskites self‐assembled atop 3D methylammonium lead triiodide (MAPbI3) via a one‐step printing process is shown. A clean and flat interface is observed in the 2D/3D bilayer heterostructure for the first time. The 2D perovskite capping layer significantly suppresses nonradiative charge recombination, resulting in a marked increase in open‐circuit voltage (VOC) of the devices by up to 100 mV. An ultrahigh VOC of 1.20 V is achieved for MAPbI3 PSCs, corresponding to 91% of the Shockley–Queisser limit. Moreover, notable enhancement in light, thermal, and moisture stability is obtained as a result of the protective barrier of the 2D perovskites. These results suggest a viable approach for scalable fabrication of highly efficient perovskite solar cells with enhanced environmental stability.
As perovskite solar cells are highly efficient and already meet the efficiency requirement for renewable power generation, more attention is given to the technological barriers such as scalability and stability....
Halide perovskites are one of the ideal photovoltaic materials for constructing flexible solar devices due to relatively high efficiencies for low‐temperature solution‐processed devices. However, the overwhelming majority of flexible perovskite solar cells are produced using spin coating, which represents a major hurdle for upscaling. Here, a scalable approach is reported to fabricate efficient and robust flexible perovskite solar cells on a polymer substrate. Thiourea is introduced into perovskite precursor solution to modulate the crystal growth, resulting in dense and uniform perovskite thin films on rough surfaces. As a decisive step, a cascade energy alignment is realized for the hole extraction layer by rationally designing a bilayer interface comprised of PEDOT:PSS/PTAA with a distinct offset in the highest occupied molecular orbital levels, enabling markedly enhanced charge extraction and spectral response. An efficiency as high as 19.41% and a record fill factor up to 81% are achieved for flexible perovskite devices processed by a scalable printing method. Equally important, the bilayer interface reinforces the bendability of the indium tin oxide substrate, leading to enhanced mechanical robustness of the flexible devices. These results underpin the importance of morphology control and interface design in constructing high‐performance flexible perovskite solar cells.
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