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Electron-withdrawing organic ligand for high-efficiency all-perovskite tandem solar cells

Nature Energy volume 9, pages 298–307 (2024)Cite this article

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Abstract

Tin–lead mixed perovskite-based tandem solar cells show promise. However, the inherent oxidation of tin remains a challenge for achieving high power conversion efficiency and device stability. In this study, we present an approach to address this challenge by developing an electron-withdrawing chloromethyl phosphonic acid ligand based on the substituent effect, designed to mitigate tin oxidation in tin–lead mixed perovskite materials. The introduction of this electron-withdrawing ligand improves the redox potential of the tin adduct. Furthermore, it leads to a substantial increase in the ionization potential of the perovskite structure. Through comparative analysis with conventional coordinating molecules, we reveal that the electron-withdrawing ligand is more effective in suppressing tin oxidation and reducing the defect density within the tin-based perovskite film. Using our approach, we demonstrate certified efficiency of 26.96% for all-perovskite tandem solar cells.

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Fig. 1: Antioxidant behaviour of phosphonic acids on SnI2.
Fig. 2: Analysis for the antioxidants in perovskite films.
Fig. 3: Analysis of defects in perovskite films.
Fig. 4: Characterization of carrier transport and JV performance.
Fig. 5: Characterization of 2-T tandem PSCs.

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The datasets generated during and/or analysed during the current study are included in the published article and its supplementary information and source data provided with this paper.

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Acknowledgements

We gratefully acknowledge financial support from the National Natural Science Foundation of China (grant nos. 61935016, 92056119, 22175118), National Key Research and Development Programme of China (under grant no. 2021YFA0715502), the Double First-Class Initiative Fund of ShanghaiTech University and the Science and Technology Commission of Shanghai Municipality (grant nos. 20XD1402500, 20JC1415800 and 21ZR1442100). We appreciate the Instrument Analysis Center and Centre for High resolution Electron Microscopy (CħEM) of ShanghaiTech University. We thank W. Liu and Y. Huang for helping with the cyclic voltammetry measurement and analysis. The computational support is provided by the high performance computing facility in ShanghaiTech University.

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  1. These authors contributed equally: Danni Yu, Mengling Pan, Gaoqi Liu.

Authors and Affiliations

  1. School of Physical Science and Technology, ShanghaiTech University, Shanghai, China

    Danni Yu, Mengling Pan, Gaoqi Liu, Xianyuan Jiang, Xin Wen, Wenzhuo Li, Shaojie Chen, Wenjia Zhou, Hao Wang, Yue Lu, Mingyu Ma, Zihao Zang, Peihong Cheng, Qingqing Ji, Fan Zheng & Zhijun Ning

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Contributions

Z.N. and D.Y. conceived the idea and designed the experiment. D.Y. and M.P. conducted the tandem solar cell fabrication. D.Y., G.L. and W.L. fabricated and characterized perovskite films and devices. X.W. and F.Z. conducted the theoretical simulation. S.C. assisted with the cyclic voltammetry measurement. W.Z. performed the TPC testing of the perovskite devices. H.W. performed the electroluminescence testing of the perovskite devices. Y.L. and Q.J. performed the field-effect transistor measurement. P.C. guided the UPS measurements. D.Y. and Z.N. wrote the manuscript. All authors discussed the results and contributed to the revision of the manuscript. Z.N. supervised the project.

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Correspondence to Zhijun Ning.

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Nature Energy thanks Kenneth Graham, Feng Yan and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Extended data

Extended Data Fig. 1 Characterization of perovskite cross-section SEM.

SEM cross-sectional images of (a) the control film, (b) the film with MP and (c) the film with CMP (Scale bar 200 nm).

Extended Data Fig. 2 Infrared characterization of coordination molecules.

IR spectra of (a) perovskite film with MP, (b) MP powder, (c) perovskite film with CMP, and (d) CMP powder.

Extended Data Fig. 3 Theoretical calculation of perovskite ionization potential.

Ionization potential (IP) of the control, MP-coordinated, and CMP-coordinated FASnI3 at FAI terminals calculated by DFT.

Supplementary information

Supplementary Information

Supplementary Figs. 1–20 and Tables 1–4.

Reporting Summary

Source data

Source Data Fig. 4d

The efficiency data of solar cell devices in Fig. 4d.

Source Data Fig. 5b

The efficiency data of solar cell devices in Fig. 5b.

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Yu, D., Pan, M., Liu, G. et al. Electron-withdrawing organic ligand for high-efficiency all-perovskite tandem solar cells. Nat Energy 9, 298–307 (2024). https://doi.org/10.1038/s41560-023-01441-2

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