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Redox mediator-stabilized wide-bandgap perovskites for monolithic perovskite-organic tandem solar cells

Nature Energy volume 9, pages 411–421 (2024)Cite this article

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Abstract

Halide segregation critically limits the stability of mixed-halide perovskite solar cells under device operational conditions. There is a strong indication that halide oxidation is the primary driving force behind halide de-mixing. To alleviate this problem, we develop a series of multifunctional redox mediators based on anthraquinone that selectively reduce iodine and oxidize metallic Pb0, while simultaneously passivating defects through tailored cationic substitution. These effects enable wide-bandgap perovskite solar cells to achieve a power conversion efficiency of 19.58% and a high open-circuit voltage of 1.35 V for 1.81-eV PSCs. The device retains 95% of its initial efficiency after operating at its maximum power point for 500 h. Most notably, by integrating the perovskite device into the monolithic perovskite-organic tandem solar cell as a wide-bandgap subcell, we report an efficiency of 25.22% (certified 24.27%) with impressive long-term operational stability (T90 > 500 h).

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Fig. 1: Electron shuttling enabled by AQS-based redox mediators.
Fig. 2: Effect of redox mediators on the phase stability of I/Br mixed perovskites.
Fig. 3: DFT calculations based on the redox mediator/perovskite interfacial models.
Fig. 4: Photovoltaic performance of single-junction PSCs.
Fig. 5: Photovoltaic performance of monolithic PO-TSCs.

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All data generated or analysed during this study are included in the published Article and its Supplementary Information and Source Data files. Source data are provided with this paper.

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Acknowledgements

We thank Y. An and H.-L. Yip from City University of Hong Kong for conducting the optical simulation, and Nano-X from Suzhou Institute of Nano-Tech and Nano-Bionics, Chinese Academy of Sciences (SINANO) for technical support. A.K.-Y.J. is thankful for the sponsorship of the Lee Shau-Kee Chair Professor (Materials Science) and support from APRC grants from the City University of Hong Kong (9380086, 9610419, 9610492 and 9610508), a TCFS grant (GHP/018/20SZ), an MRP grant (MRP/040/21X) from the Innovation and Technology Commission of Hong Kong, the Green Tech Fund (202020164) from the Environment and Ecology Bureau of Hong Kong, GRF grants (11307621 and 11316422) from the Research Grants Council of Hong Kong, Shenzhen Science and Technology Program (SGDX20201103095412040), Guangdong Major Project of Basic and Applied Basic Research (2019B030302007), Guangdong-Hong Kong-Macao Joint Laboratory of Optoelectronic and Magnetic Functional Materials (2019B121205002), Guangzhou Huangpu Technology Bureau (2022GH02) and a CRF grant (C6023-19GF) from the Research Grants Council of Hong Kong. J.Y. acknowledges support from the Hong Kong Polytechnic University (grant no. P0042930). The work described in this paper was partially supported by a fellowship award from the Research Grants Council of the Hong Kong Special Administrative Region, China (project no. CityU PDFS2223-1S08).

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Author notes

  1. These authors contributed equally: Shengfan Wu, Yichao Yan, Jun Yin.

Authors and Affiliations

  1. Department of Materials Science and Engineering, City University of Hong Kong, Kowloon, Hong Kong

    Shengfan Wu, Fengzhu Li, Zixin Zeng, Sai-Wing Tsang & Alex K.-Y. Jen

  2. Hong Kong Institute for Clean Energy, City University of Hong Kong, Kowloon, Hong Kong

    Shengfan Wu, Yichao Yan, Kui Jiang, Fengzhu Li & Alex K.-Y. Jen

  3. Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong

    Yichao Yan, Kui Jiang & Alex K.-Y. Jen

  4. Department of Applied Physics, The Hong Kong Polytechnic University, Kowloon, Hong Kong

    Jun Yin

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Contributions

S.W. and Y.Y. conceived the idea. S.W. designed the project, fabricated single-junction and tandem solar cells and conducted the relevant characterizations. Y.Y. synthesized the organic redox mediators and helped to analyse the data. J.Y. performed the DFT calculations. K.J. and F.L. helped optimize single-junction organic and perovskite solar cells. Z.Z. and S.-W.T. contributed to time-dependent PL measurements. A.K.-Y.J. supervised the project. S.W. drafted the original manuscript. S.W. and A.K.-Y.J. finalized the manuscript. All authors contributed to data interpretation.

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Correspondence to Alex K.-Y. Jen.

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Nature Energy thanks Zhubing He and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–45, Notes 1–4, Tables 1–7 and references 1–7.

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Wu, S., Yan, Y., Yin, J. et al. Redox mediator-stabilized wide-bandgap perovskites for monolithic perovskite-organic tandem solar cells. Nat Energy 9, 411–421 (2024). https://doi.org/10.1038/s41560-024-01451-8

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