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Durable all-inorganic perovskite tandem photovoltaics

Nature volume 637, pages 1111–1117 (2025)Cite this article

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Abstract

All-inorganic perovskites prepared by substituting the organic cations (for example, methylammonium and formamidinium) with inorganic cations (for example, Cs+) are effective concepts to enhance the long-term photostability and thermal stability of perovskite solar cells (PSCs)1,2. Hence, inorganic perovskite tandem solar cells (IPTSCs) are promising candidates for breaking the efficiency bottleneck and addressing the stability issue, too3,4. However, challenges remain in fabricating two-terminal (2T) IPTSCs due to the inferior film formation and deep trap states induced by tin cations5,6,7. Here a ligand evolution (LE) strategy with p-toluenesulfonyl hydrazide (PTSH) is used to regulate film formation and eliminate deep traps in inorganic narrow-bandgap (NBG) perovskites, enabling the successful development of 2T IPTSCs. Accordingly, the 1.31 eV CsPb0.4Sn0.6I3:LE device delivers a record efficiency of 17.41%. Combined with the 1.92 eV CsPbI2Br top cell, 2T IPTSCs exhibit a champion efficiency of 22.57% (certified, 21.92%). Moreover, IPTSCs are engineered to deliver remarkable durability under maximum power point (MPP) tracking, maintaining 80% of their initial efficiency at 65 °C for 1,510 h and at 85 °C for 800 h. We elucidate that LE deliberately leverages multiple roles for inorganic NBG perovskite growth and anticipate that our study provides an insightful guideline for developing high-efficiency and stable IPTSCs.

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Fig. 1: LE improved the performance of inorganic NBG PSCs.
Fig. 2: LE-improved perovskite crystallization and microstructure.
Fig. 3: Monitoring the interaction mechanism of LE.
Fig. 4: Photovoltaic and stability performance of optimized 2T IPTSC.

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The data that support the findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was supported in part by funds from the National Natural Science Foundation of China (U2001217), Guangdong Science and Technology Program (2019ZT08L075, 2019QN01L118 and 2024A1515011154), National Key Research and Development Program of China (2022YFB3803300), the International Training Program for Young Talents of Guangdong Province and Guangzhou Science and Technology Planning Project (2023A04J1697) and Zhejiang Jusheng Solar S&T (2023440002001153).

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Authors and Affiliations

  1. School of Environment and Energy, State Key Laboratory of Luminescent Materials and Devices, Guangdong Provincial Key Laboratory of Solid Wastes Pollution Control and Recycling, South China University of Technology, Guangzhou, People’s Republic of China

    Chenghao Duan, Feilin Zou, Jiong Li, Zheng Zhang, Chang Chen, Qiliang Zhu, Ning Li & Keyou Yan

  2. Department of Physics, The Chinese University of Hong Kong, Hong Kong, People’s Republic of China

    Chenghao Duan, Shiang Li & Xinhui Lu

  3. Institute of Materials for Electronics and Energy Technology (i-MEET), Department of Materials Science and Engineering, Friedrich-Alexander University Erlangen-Nürnberg, Erlangen, Germany

    Kaicheng Zhang, Zijian Peng & Christoph J. Brabec

  4. Department of Physics, Chemistry and Biology (IFM), Linköping University, Linköping, Sweden

    Feng Wang & Feng Gao

  5. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, People’s Republic of China

    Jianhang Qiu

  6. Center of Excellence in Nanoscience (CAS), Key Laboratory of Nanosystem and Hierarchical Fabrication, National Center for Nanoscience and Technology, Beijing, People’s Republic of China

    Liming Ding

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Contributions

K.Y. conceived the idea and directed the overall project. C.J.B., F.G., F.W., X.L. and N.L. supervised the research. K.Z., Z.P. and L.D. revised the manuscript. C.D. performed the main experiments and drafted the manuscript. S.L. and X.L. carried out the GIWAXS measurement and analysis. J.Q. carried out the TOF-SIMS measurement. F.Z. and Q.Z. fabricated the NBG perovskite films. C.C. prepared the WBG perovskite films. J.L. carried out the SEM and X-ray diffraction characterizations. Z.Z. performed the photoluminescence and time-resolved photoluminescence analysis of perovskite films.

Corresponding author

Correspondence to Keyou Yan.

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Nature thanks Michael Saliba, Qingwen Tian and Yiqiang Zhang for their contribution to the peer review of this work. Peer reviewer reports are available.

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Extended data figures and tables

Extended Data Fig. 1 In situ characterization for film growth.

2D contour maps of in-situ UV-vis spectra of (a) CsPb0.4Sn0.6I3 and (b) CsPb0.4Sn0.6I3:PTSH perovskite film during the annealing process at 70 °C. 2D contour maps of in-situ XRD spectra of (c) CsPb0.4Sn0.6I3 and (d) CsPb0.4Sn0.6I3:PTSH perovskite film during the annealing process at 70 °C.

Extended Data Fig. 2 DFT simulation on the coordination.

The binding energies (BE) between DMSO or PTSH molecules and PbI2 or SnI2, respectively. Where white, brown, light blue, red, yellow, ice blue, and black balls are H, C, N, O, S, Sn, and Pb atoms. The BE of PTSH molecules with Sn2+ for SnI2 and Pb2+ for PbI2 are −2.112 eV and −1.817 eV, respectively, which are higher than the binding energies of DMSO molecules with Sn2+ for SnI2 (−1.613 eV) and Pb2+ for PbI2 (−1.434 eV).

Extended Data Fig. 3 Identification of gas products of LE.

(a) Diagram of the gas collection process. (b) Photographs of CuSO4 powder color change. (c) Photographs of the color change of purple litmus reagent in bottle 1, and the color change of H2O2 solution and starch solution in bottle 1 successively. (d) Photographs of Mg burning in bottle 2, and the color change of litmus paper caused by the gas produced after adding hot water.

Extended Data Fig. 4 ToF-SIMS measurements.

ToF-SIMS of depth profiles of anion distribution in inorganic (a) CsPb0.4Sn0.6I3, (b) CsPb0.4Sn0.6I3:LE and (c) CsPb0.4Sn0.6I3:LE based on ALD-SnO2 PSCs with continuous illumination at 85 °C for 10 days in N2 glovebox.

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Supplementary Information

Supplementary Notes 1–3, Figs. 1–60, Tables 1–9, Schemes 1 and 2 and references.

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Duan, C., Zhang, K., Peng, Z. et al. Durable all-inorganic perovskite tandem photovoltaics. Nature 637, 1111–1117 (2025). https://doi.org/10.1038/s41586-024-08432-7

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