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Stabilization of 3D/2D perovskite heterostructures via inhibition of ion diffusion by cross-linked polymers for solar cells with improved performance

Abstract

Two-dimensional (2D) and quasi-2D modifications of three-dimensional (3D) perovskite active layers have contributed to advances in the performance of perovskite solar cells (PSCs). However, the ionic diffusion between the surface 2D and bulk 3D perovskites leads to the degradation of the 3D/2D perovskite heterostructures and limits the long-term stability of PSCs. Here we incorporate a cross-linked polymer (CLP) on the top of a 3D perovskite layer and then deposit a 2D perovskite layer via a vapour-assisted two-step process to form a 3D/CLP/2D perovskite heterostructure. Photoluminescence spectra and thickness-profiled elemental analysis indicate that the CLP stabilizes the heterostructure by inhibiting the diffusion of cations (formamidinium, FA+ and 4-fluorophenylethylammonium, 4F-PEA+) between the 2D and 3D perovskites. For devices based on carbon electrodes, we report small-area devices with an efficiency of 21.2% and mini-modules with an efficiency of 19.6%. Devices retain 90% of initial performance after 4,390 hours operation under maximum power point tracking and one-sun illumination at elevated temperatures.

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Fig. 1: Preparation of the 3D/CLP/2D perovskite heterostructure and selection of CLP.
Fig. 2: Stabilization effect of the CLP on perovskite heterostructures.
Fig. 3: Charge carrier dynamics and device performance.
Fig. 4: Long-term stability test.

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Data availability

All the data supporting the findings of this study are available within this article and its Supplementary Information. Any additional information can be obtained from corresponding authors upon request. Source data are provided with this paper.

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Acknowledgements

This work was financially supported by National Key Research and Development Program of China (2020YFA0715000, L.M.; 2022YFB4200305, X.L. and Y.R.); National Natural Science Foundation of China (21875081, X.L.; 22279039, X.L.; 52172200, Y.R. and 52127816, L.M.); the Chinese National 1000-Talent-Plan programme (X.L.); the Science and Technology Department of Hubei Province (2021CFB315, Y.R.); the Innovation Project of Optics Valley Laboratory OVL2021BG008 (X.L.); the foundation of State Key Laboratory of New Textile Materials and Advanced Processing Technologies (grant number FZ2021011, X.L.), the Foundation of State Key Laboratory of Coal Conversion (grant number J18-19-913, X.L.). We thank the Analytical and Testing Center from HUST and the Center for Nanoscale Characterization and Devices (CNCD) from WNLO (HUST) for the facility support of sample measurements. We would like to thank Suzhou Institute of Nano-Tech and Nano-Bionics for performing TOF-SIMS. Z.W. acknowledges the Banting Postdoctoral Fellowships Program of Canada.

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Contributions

X.L. directed and supervised the project. L. Luo, Z.W. and Y.R. designed the experiments. L. Luo fabricated the perovskite devices. H.Z. synthesized polymer materials. L. Luo, M.L. and S.Y. contributed to the certification of mini-modules. Q.A. and L.C., conducted XRD and XPS measurements. W. Li and L. Luo carried out SEM and PL measurements. D.L. and J.H. conducted UPS and XPS measurements. L. Luo and H.Z. conducted FTIR measurements. L. Li conducted AFM-IR measurement. R.G. conducted the stability tests on the devices. R.H. conducted TOF-SIMS measurement. X.C. and W. Liang conducted TA measurements. L. Luo wrote the first draft of the manuscript. X.L, E.H.S., Y.R., L.M., Z.W., B.C., A.M. and H.Z. revised the manuscript. All authors analysed the data and reviewed the manuscript.

Corresponding authors

Correspondence to Liqiang Mai, Yaoguang Rong, Edward H. Sargent or Xiong Li.

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Supplementary Notes 1–4, Figs. 1–22, Tables 1–6 and References.

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Supplementary Video 1

This video shows the insolubility of CLP in H2O, IPA and DMF.

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Luo, L., Zeng, H., Wang, Z. et al. Stabilization of 3D/2D perovskite heterostructures via inhibition of ion diffusion by cross-linked polymers for solar cells with improved performance. Nat Energy 8, 294–303 (2023). https://doi.org/10.1038/s41560-023-01205-y

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