Abstract
Two-dimensional (2D) and three-dimensional (3D) perovskite heterostructures have played a key role in advancing the performance of perovskite solar cells1,2. However, the migration of cations between 2D and 3D layers results in the disruption of octahedral networks, leading to degradation in performance over time3,4. We hypothesized that perovskitoids, with robust organic–inorganic networks enabled by edge- and face-sharing, could impede ion migration. We explored a set of perovskitoids of varying dimensionality and found that cation migration within perovskitoid–perovskite heterostructures was suppressed compared with the 2D–3D perovskite case. Increasing the dimensionality of perovskitoids improves charge transport when they are interfaced with 3D perovskite surfaces—this is the result of enhanced octahedral connectivity and out-of-plane orientation. The 2D perovskitoid (A6BfP)8Pb7I22 (A6BfP: N-aminohexyl-benz[f]-phthalimide) provides efficient passivation of perovskite surfaces and enables uniform large-area perovskite films. Devices based on perovskitoid–perovskite heterostructures achieve a certified quasi-steady-state power conversion efficiency of 24.6% for centimetre-area perovskite solar cells. We removed the fragile hole transport layers and showed stable operation of the underlying perovskitoid–perovskite heterostructure at 85 °C for 1,250 h for encapsulated large-area devices in ambient air.
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Data availability
The data supporting the findings of this study are available from the corresponding authors upon request. All the crystal structure files generated in this study have been deposited at the Cambridge Crystallographic Data Centre under the accession numbers 2362695, 2362696, 2362697, 2362698, 2362699, 2362700, 2362701 and 2362702.
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Acknowledgements
This work is partially supported by award 70NANB19H005 from the US Department of Commerce, National Institute of Standards and Technology as part of the Center for Hierarchical Materials Design (CHiMaD). M.G.K. was supported by DOE BES grant no. DE-SC0024422 (fundamental studies on metal halides) and T.J.M. by ONR award no. N00014-20-1-2116. This work made use of the SPID, EPIC, Keck-II and NUFAB facilities of Northwestern University’s NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-2025633), the International Institute of Nanotechnology, Northwestern University and Northwestern’s MRSEC programs (NSF DMR-1720139, NSF DMR-2308691). A.S.R.B. acknowledges support from King Abdullah University of Science and Technology (KAUST) through the Ibn Rushd Postdoctoral Fellowship Award.
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C.L., Y.Y. and D.Z. conceived the idea and proposed the experimental design. C.L. and Y.Y. conducted the characterization. C.L., Y.Y. and H.C. performed the device fabrication. I.S. performed single-crystal synthesis, characterization and structure analysis. C.L. and A.S.R.B. wrote the first draft of the manuscript. A.S.R.B. performed the SEM and XRD measurements. J.C. synthesized organic halides. B.V. and S.D.W. conducted the TEM measurements. I.W.G., R.P.R., T.E.W. and J.F. helped with the single-crystal synthesis and structure analysis. C.H. and Y.L. helped with photoluminesence measurements. A.M., Z.W., B.C. and L.X.C. helped revise the manuscript. D.Z., T.J.M., A.F., E.H.S. and M.G.K. supervised the project. All the authors contributed to comments on and revision of the manuscript.
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C.L., Y.Y., I.S., B.C., D.Z., A.F., T.J.M., E.H.S. and M.G.K. are filing a patent based on this work. The other authors declare no competing interests.
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Liu, C., Yang, Y., Chen, H. et al. Two-dimensional perovskitoids enhance stability in perovskite solar cells. Nature 633, 359–364 (2024). https://doi.org/10.1038/s41586-024-07764-8
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DOI: https://doi.org/10.1038/s41586-024-07764-8
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