Abstract
Although being highly demanded in organic electronics, functional conjugated polymers face challenges on scalable synthesis with batch uniformities. Here a reactivity-regulated sequent cross-coupling carbon–nitrogen polycondensation method is developed to enable the precise synthesis of functional polyarylamines with excellent batch-to-batch uniformity. It is revealed that the stepwise regulation of intermediate reactivities is key to accomplish controllable polycondensation via two sequent palladium-promoted carbon–nitrogen coupling cycles, which is distinct to the unicyclic carbon–carbon coupling. A variety of polyarylamines are prepared to improve the material functionalities, where a ternary polymer consisting of polar substituents is shown to optimize the interfacial and bulk properties of perovskite layers fabricated on top. The corresponding inverted perovskite solar cells achieved remarkable power conversion efficiencies of 25.2% (active area, 5.97 mm2) and 23.2% (active area, 128 mm2), along with decent operational stabilities. Overall, this work provides an effective polymerization method for advanced conjugated polymers to enable high-performance optoelectronics.
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Acknowledgements
This research was funded by the National Natural Science Foundation of China (no. 22125901), the National Key Research and Development Program of China (no. 2019YFA0705900), the Fundamental Research Funds for the Central Universities (no. 226-2024-00005) and the Scientific Research Project of China Three Gorges Corporation (no. 202303014). We thank P. Qian and B. Shi from the Department of Chemistry, Zhejiang University, for technical support on scale synthesis.
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C.-Z.L. and Z.S. developed the concept. C.-Z.L., Z.S., Y.H. and K.Y. designed the experiments. C.-Z.L. and H.C. supervised the project. Z.S. conducted the synthesis experiments. Y.H. and Z.S. performed the PSC fabrication and characterization. Y.H., Z.S., Y.D. and K.Y. carried out the film measurements and analysis. Z.S., Y.H. and C.-Z.L. prepared the manuscript. All authors provided feedback and commented on the manuscript.
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Nature Materials thanks Mohammad Khaja Nazeeruddin, Yanlin Song and Atsushi Wakamiya for their contribution to the peer review of this work.
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Shen, Z., Huang, Y., Dong, Y. et al. Precise synthesis of advanced polyarylamines for efficient perovskite solar cells. Nat. Mater. (2025). https://doi.org/10.1038/s41563-025-02199-6
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DOI: https://doi.org/10.1038/s41563-025-02199-6
