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Aromatic cation−π-dominated pathway control in living supramolecular polymerization

Nature Synthesis volume 5, pages 139–150 (2026)Cite this article

Abstract

Living supramolecular polymerization (LSP) has attracted widespread attention as a synthetic method for precisely controlling the supramolecular polymerization process and structure. However, effectively coupling the kinetic and thermodynamic energy landscape in LSP to achieve precise control of the polymerization process remains challenging due to the complexity of the multiple energy landscapes involved in the kinetic supramolecular polymerization process. Here we propose a cation−π-dominated pathway regulation strategy that establishes an integrated energy landscape between kinetic traps and thermodynamic polymerization processes by dynamically switching various aromatic cation−π bonding modes, complemented by the photoregulated conformational transformation of azobenzene. By controlling the folding of the azobenzene core conformation under light irradiation, metastable dormant monomers stabilized by individual intramolecular cation−π bonding are competitively formed, which spontaneously transform into thermodynamically favourable ordered two-dimensional nanosheets upon conformational unfolding through alternating intermolecular cation−π interactions. This coupled transition from the kinetic to the thermodynamic pathway can be accelerated by seeds addition, enabling controllable LSP.

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Fig. 1: Energy landscapes of supramolecular polymerization and chemical structures of monomers.
Fig. 2: Studies of the metastable supramolecular polymerization and the pathway complexity of M1.
Fig. 3: Characterization of the morphological evolution of M1.
Fig. 4: Molecular stacking mode confirmation of dormant monomer cis-M1 and thermodynamically stable 2DSP-1.
Fig. 5: Experimental and theoretical confirmation of the cation–π interactions in cis-M1 and 2DSP-1.
Fig. 6: Confirmation of LSP.
Fig. 7: Electrocatalytic HER performance during LSP.

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Data availability

All data that support the findings of this study are available in the Article and its Supplementary Information. Crystallographic data for the structures reported in this Article have been deposited at the Cambridge Crystallographic Data Centre, under deposition numbers CCDC 2393096 (M1), 2393089 (M2), 2393090 (D3) and 2393091 (D4). Copies of the data can be obtained free of charge via https://www.ccdc.cam.ac.uk/structures/.Source data are provided with this paper.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (22471219, W.T. and 22071197, W.T.), the Innovation Capability Support Program of Shaanxi (2025RS-CXTD-022, W.T.), the Shaanxi Fundamental Science Research Project for Chemistry & Biology (23JHZ002, W.T.), the Fundamental Research Funds for the Central Universities (G2025KY06148, W.T.) and the the Open Foundation Project of Henan University (DCSHENU2420, S.Q.). We thank the Analytical & Testing Center of Northwestern Polytechnical University for TEM, AFM and SEM measurements.

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Author notes

  1. These authors contributed equally: Zhelin Zhang, Junlong Su.

Authors and Affiliations

  1. Shaanxi Key Laboratory of Macromolecular Science and Technology, Xi’an Key Laboratory of Hybrid Luminescent Materials and Photonic Device, MOE Key Laboratory of Material Physics and Chemistry under Extraordinary Conditions, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an, P. R. China

    Zhelin Zhang, Junlong Su, Xuxu Xie, Xiaotian Li & Wei Tian

  2. Institute of Nanoscience and Engineering, Henan University, Kaifeng, P. R. China

    Shuai Qiu

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  1. Zhelin Zhang
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Contributions

W.T. conceived the idea for this project. Z.Z. and J.S. performed the primary experiments, interpreted the results and assisted with the paper. X.X. contributed to the investigation of supramolecular polymerization. X.L. contributed to the electrocatalytic experiments. S.Q. performed the theoretical calculation and data interpretation. All authors contributed to the manuscript preparation.

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Correspondence to Wei Tian.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–93, Discussion and Tables 1–6.

Supplementary Data 1

Crystallographic data for M1, CCDC 2393096.

Supplementary Data 2

Crystallographic data for M2, CCDC 2393089.

Supplementary Data 3

Crystallographic data for D3, CCDC 2393090.

Supplementary Data 4

Crystallographic data for D4, CCDC 2393091.

Source data

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Source Data Fig. 4

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Source Data Fig. 5

Source data for Fig. 5.

Source Data Fig. 6

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Source Data Fig. 7

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Zhang, Z., Su, J., Xie, X. et al. Aromatic cation−π-dominated pathway control in living supramolecular polymerization. Nat. Synth 5, 139–150 (2026). https://doi.org/10.1038/s44160-025-00912-6

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