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Suppression of phase segregation in wide-bandgap perovskites with thiocyanate ions for perovskite/organic tandems with 25.06% efficiency

Nature Energy (2024)Cite this article

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Abstract

Mixed halide wide-bandgap perovskites are suitable for integration in tandem photovoltaics such as perovskite/organic tandem solar cells. However, halide phase segregation originating from halogen vacancy-assisted ion migration in wide-bandgap perovskites limits the device efficiency and lifetime. Here we incorporate pseudo-halogen thiocyanate (SCN) ions in iodide/bromide mixed halide perovskites and show that they enhance crystallization and reduce grain boundaries. Trace amount of SCN ions in the bulk enter the perovskite lattice, forming an I/Br/SCN alloy, and occupy iodine vacancies, blocking halide ion migration via steric hindrance. Taken together, these effects retard halide phase segregation under operation and reduce energy loss in the wide-bandgap perovskite cells. The resulting perovskite/organic tandem solar cell achieves a power conversion efficiency of 25.82% (certified 25.06%) and an operational stability of 1,000 h.

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Fig. 1: Regulating the crystallization of perovskites.
Fig. 2: Characteristics of the pseudo-triple-halide alloyed perovskite.
Fig. 3: Ion migration behaviour and halide phase segregation.
Fig. 4: Performance of single-junction cells and TSCs.

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The authors declare that the experimental data that support the findings of this paper are available within this article and its Supplementary Information files. Other findings in this study are available from the corresponding authors on reasonable request. Source data are provided with this paper.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (grant nos. 52325307, 22075194, 52203233, 52273188 and 52102287), the National Key Research and Development Program of China (grant no. 2022YFB4200302 and 2020YFB1506400), Department of Science and Technology of Jiangsu Province (grant no. BE2022023), the National Postdoctoral Program for Innovative Talents (grant no. BX2021205), project funded by China Postdoctoral Science Foundation (grant no. 2022M710102), the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD), Collaborative Innovation Center of Suzhou Nano Science and Technology, and the Key Laboratory of Polymeric Materials Design and Synthesis for Biomedical Function, Soochow University.

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Authors and Affiliations

  1. Laboratory of Advanced Optoelectronic Materials, Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China

    Zhichao Zhang, Weijie Chen, Jianlei Cao, Haidi Yang, Haiyang Chen, Fu Yang, Yunxiu Shen, Heyi Yang, Qinrong Cheng, Xining Chen, Xiaohua Tang, Shuaiqing Kang, Xue-mei Ou, Yaowen Li & Yongfang Li

  2. Department of Applied Physics, School of Physics and Electronics, Hunan University, Changsha, China

    Xingxing Jiang

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

    Fu Yang & Christoph J. Brabec

  4. Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (HI ERN), Erlangen, Germany

    Christoph J. Brabec

  5. Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Soochow University, Suzhou, China

    Yaowen Li & Yongfang Li

  6. State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials, Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application, College of Chemistry, Chemical Engineering and Materials Science, Soochow University, Suzhou, China

    Yaowen Li

  7. Beijing National Laboratory for Molecular Sciences; CAS Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, China

    Yongfang Li

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  1. Zhichao Zhang
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Contributions

W.C., C.J.B. and Yaowen Li conceived the project. Z.Z. and J.C. made the devices and contributed to the performance improvement. X.J. conducted the DFT calculation. Y.S. conducted the GIWAXS measurement and performed the results analysis. Z.Z. and Heyi Yang analysed the MPP stability and impedance spectra. Q.C. measured the absorption spectra and performed the results analysis. Z.Z. and X.C. measured the in situ absorption spectra and PL spectra. S.K. measured the XRD spectra. X.T. encapsulated the devices for certification. H.C., F.Y., Haidi Yang and X.-m.O. participated in the characterizations of devices. Z.Z., W.C., C.J.B., Yaowen Li and Yongfang Li contributed to the results analysis. W.C. and Yaowen Li wrote the paper. W.C., C.J.B., Yaowen Li and Yongfang Li supervised the project. All authors discussed the results and commented on the final paper.

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Correspondence to Weijie Chen, Christoph J. Brabec or Yaowen Li.

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Nature Energy thanks Peter Chen, Byungha Shin and Zonglong Zhu for their contribution to the peer review of this work.

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Zhang, Z., Chen, W., Jiang, X. et al. Suppression of phase segregation in wide-bandgap perovskites with thiocyanate ions for perovskite/organic tandems with 25.06% efficiency. Nat Energy (2024). https://doi.org/10.1038/s41560-024-01491-0

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