Efficient and stable Ruddlesden–Popper perovskite solar cell with tailored interlayer molecular interaction

Abstract

Two-dimensional Ruddlesden–Popper phase (2DRP) perovskites are known to exhibit improved photostability and environmental stability compared with their three-dimensional (3D) counterparts. However, fundamental questions remain over the interaction between the bulky alkylammoniums and the 2DRP perovskite framework. Here, we unambiguously demonstrate that a sulfur–sulfur interaction is present for a new bulky alkylammonium, 2-(methylthio)ethylamine hydrochloride (MTEACl). In addition to a weaker van der Waals interaction, the interaction between sulfur atoms in two MTEA molecules enables a (MTEA)2(MA)4Pb5I16 (n = 5) perovskite framework with enhanced charge transport and stabilization. The result is 2DRP perovskite solar cells with significantly improved efficiency and stability. Cells with a power conversion efficiency as high as 18.06% (17.8% certified) are achieved, along with moisture tolerance for up to 1,512 h (under 70% humidity conditions), thermal stability for 375 h (at 85 °C) and stability under continuous light stress (85% of the initial efficiency retained over 1,000 h of operation at the maximum power point).

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Fig. 1: Crystal structures and DFT calculations for the 2DRP perovskites.
Fig. 2: GIWAXS patterns for the 3D and 2DRP perovskite films.
Fig. 3: Charge transfer dynamics and charge transport characteristics.
Fig. 4: 2DRP PSCs architecture and characterization.
Fig. 5: Stability of (MTEA)2(MA)4Pb5I16 and (BA)2(MA)4Pb5I16 2DRP thin films and PSCs.

Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request

Change history

  • 22 January 2020

    In the version of the Supplementary Information originally published online with this Article, Supplementary Fig. 12 was missing; the figure has now been added.

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Acknowledgements

This work was financially supported by the National Basic Research Program of China, Fundamental Studies of Perovskite Solar Cells (grant no. 2015CB932200), Natural Science Foundation of China (grants nos. 51602149, 61705102, 61722403 and 11674121), National Key Research and Development Program of China (grants nos. 2017YFA0403403 and 2016YFB0201204), Natural Science Foundation of Jiangsu Province, China (grants nos. BK20161011, BK20161010 and BK20150064), the Young 1000 Talents Global Recruitment Program of China, the Jiangsu Specially Appointed Professor Program, the ‘Six talent peaks’ Project in Jiangsu Province, China and the Program for JLU Science and Technology Innovative Research Team. Calculations were performed in part at the High Performance Computing Centre of Jilin University.

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Y.C. and W.H. conceived and designed the experiments. Y.C. and W.H. supervised the experimental work. L.Z. supervised the theoretical part. H.R. and L.C. carried out the device fabrication and characterizations. Y.Y. and H.D. carried out GIWAXS measurements and analyses. S.Y., Y.S. and L.Z. carried out calculations. S.Z., F.L. and J.Z. carried out XANES measurements. Y.C., H.R., L.Z., S.Y. and Y.X. wrote the first draft of the manuscript. X.G., H.J., J.W. and W.H. participated in data analysis and provided major revisions. All authors discussed the results and commented on the manuscript.

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Correspondence to Lijun Zhang or Yonghua Chen or Wei Huang.

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Supplementary Figs. 1–18 and Tables 1–4.

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Ren, H., Yu, S., Chao, L. et al. Efficient and stable Ruddlesden–Popper perovskite solar cell with tailored interlayer molecular interaction. Nat. Photonics 14, 154–163 (2020). https://doi.org/10.1038/s41566-019-0572-6

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