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Efficient tin-based perovskite solar cells with trans-isomeric fulleropyrrolidine additives

Abstract

Tin-based perovskite solar cells (TPSCs) are among the best candidates for lead-free photovoltaic technology owing to their low toxicity and high theoretical efficiency. However, the efficiency and stability of TPSCs lag far behind their lead counterparts because of the poor controllability of perovskite film growth and the intrinsically easy oxidation of Sn2+. Here we synthesize two pyridyl-substituted fulleropyrrolidines (PPF) with cis (CPPF) and trans (TPPF) configurations and use them as precursor additives. The spatial configurations of the CPPF and TPPF greatly affect their electron density distributions and interactions with perovskite components. Compared with the CPPF, the TPPF has spatially separated pyridine groups that can catch more perovskite colloids through coordination bonds, thus slowing the perovskite crystallization process. The resultant perovskite film displayed better crystal orientation and compactness. The TPPF also remains located at the grain boundaries, improves the interface energy level alignment and suppresses Sn2+ oxidation. As a result, the TPPF-based TPSCs exhibit a high power conversion efficiency of 15.38% (certified 15.14%) and excellent stability, maintaining 99% and 93% of their initial efficiencies after 3,000 h of storage and 500 h of continuous illumination, respectively. This work highlights the importance of regulating coordination in the precursor solution in preparing high-quality tin-based perovskite films, paving the way to more efficient and stable TPSCs.

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Fig. 1: Optoelectronic performance of the devices.
Fig. 2: Regulatory mechanism of the crystallization process of perovskite film.
Fig. 3: Defect density and energy level alignment.
Fig. 4: Antioxidant and operational stability of the devices.

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Data availability

The data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. The data are available via Figshare at https://doi.org/10.6084/m9.figshare.24669252. Source data are provided with this paper.

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Acknowledgements

Z.W. and C.T. acknowledge financial support from the National Natural Science Foundation of China (grant numbers U21A2078 and 22179042), the Natural Science Foundation of Fujian Province (grant numbers 2020J01064 and 2020J06021), the Scientific Research Funds of Huaqiao University and the Promotion Program for Young and Middle-aged Teacher in Science and Technology Research of Huaqiao University (grant numbers ZQN-806 and ZQN-PY607). We thank the Instrumental Analysis Center of Huaqiao University for assistance with the device characterizations.

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Contributions

C.T. and Z.W. conceived the idea and supervised the project. J.C. carried out device and film fabrication and characterizations, analysed the data and wrote the manuscript. J.L. synthesized the fulleropyrrolidines. J.L. and S.C. contributed to NMR characterization and mass spectrometry. E.H. assisted with data collection from the devices, including the stability tests, EQE measurements, electrochemical impedance spectroscopy and so on. P.S. helped to analyse the grazing incidence wide-angle X-ray scattering data. Y.L. and W.F. contributed to the steady-state photoluminescence measurements of the perovskite films. L.X. contributed to the Discussion. C.S. and H.Z. contributed to the exploration of basic processes of the devices.

Corresponding authors

Correspondence to Chengbo Tian or Zhanhua Wei.

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Nature Photonics thanks Liyuan Han, Shuzi Hayase and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Figs. 1–25 and Tables 1–8.

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Chen, J., Luo, J., Hou, E. et al. Efficient tin-based perovskite solar cells with trans-isomeric fulleropyrrolidine additives. Nat. Photon. (2024). https://doi.org/10.1038/s41566-024-01381-7

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