Abstract
Self-healing polymer materials, capable of autonomously repairing physical damage, have been broadly applied in modern technologies. In various self-healing systems, metal–ligand coordination bonds have been extensively utilized for their advantages of rich metal–ligand species and functionalities. However, common metal-ligand coordination either has excessively stable bond strengths or is too weak to construct self-healing materials. This work introduces coordination metals into liquid metals (LMs) to form multi-component LMs (mLMs), which creatively leverage the inherent fluidity of mLMs to convert common metal-ligand coordination (e.g., silver-sulfur and zinc/copper-imidazole systems) into reversible interfacial coordination. Such dynamic coordination successfully offers the fantastic self-healing efficiency over 90% for general polymers. Considering the ultra-high thermal conductivity of mLMs, self-healable thermal interface materials (TIMs) are obtained, which successfully address the long-standing challenge of the irreversible damage in long-term used TIMs. The self-healable TIMs can lower the peak temperature of the central processing unit (CPU) by 20 oC under extreme conditions for long time (accumulated 16 hours thermal shock, −10 oC to 100 oC). This work provides a universal strategy for self-healing materials and greatly broadens the investigations of self-healing, coordination chemistry, liquid metal science, soft electronics, and thermal management materials.
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References
Wang, S. & Urban, M. W. Self-healing polymers. Nat. Rev. Mater. 5, 562–583 (2020).
Zhou, Y. et al. Self-healing polymers for electronics and energy devices. Chem. Rev. 123, 558–612 (2023).
Cornellà, A. C., Furia, F., Van Assche, G. & Brancart, J. Controlling the relaxation dynamics of polymer networks by combining associative and dissociative dynamic covalent bonds. Adv. Mater. 36, e2407663 (2024).
Jung, J. et al. Self-healing electronic skin with high fracture strength and toughness. Nat. Commun. 15, 9763 (2024).
Choi, C. et al. Light-mediated synthesis and reprocessing of dynamic bottlebrush elastomers under ambient conditions. J. Am. Chem. Soc. 143, 9866–9871 (2021).
Yanagisawa, Y., Nan, Y., Okuro, K. & Aida, T. Mechanically robust, readily repairable polymers via tailored noncovalent cross-linking. Science 359, 72–76 (2018).
Chen, Y., Kushner, A. M., Williams, G. A. & Guan, Z. Multiphase design of autonomic self-healing thermoplastic elastomers. Nat. Chem. 4, 467–472 (2012).
Sun, J.-Y. et al. Highly stretchable and tough hydrogels. Nature 489, 133–136 (2012).
Wang, M. et al. Glassy gels toughened by solvent. Nature 631, 313–318 (2024).
Nakahata, M., Takashima, Y., Yamaguchi, H. & Harada, A. Redox-responsive self-healing materials formed from host–guest polymers. Nat. Commun. 2, 511 (2011).
Nitta, N., Takatsuka, M., Kihara, S., Hirao, T. & Haino, T. Self-healing supramolecular materials constructed by copolymerization via molecular recognition of cavitand-based coordination capsules. Angew. Chem. Int. Ed. 59, 16690–16697 (2020).
Li, C.-H. et al. A highly stretchable autonomous self-healing elastomer. Nat. Chem. 8, 618–624 (2016).
Mozhdehi, D., Ayala, S., Cromwell, O. R. & Guan, Z. Self-healing multiphase polymers via dynamic metal–ligand interactions. J. Am. Chem. Soc. 136, 16128–16131 (2014).
Burnworth, M. et al. Optically healable supramolecular polymers. Nature 472, 334–337 (2011).
Sato, K. et al. Phase-separation-induced anomalous stiffening, toughening, and self-healing of polyacrylamide gels. Adv. Mater. 27, 6990–6998 (2015).
Bonardd, S. et al. Self-healing polymeric soft actuators. Chem. Rev. 123, 736–810 (2023).
Lee, S. et al. A shape-morphing cortex-adhesive sensor for closed-loop transcranial ultrasound neurostimulation. Nat. Electron. 7, 800–814 (2024).
Sproncken, C. C. M. et al. Large-area, self-healing block copolymer membranes for energy conversion. Nature 630, 866–871 (2024).
Pena-Francesch, A., Jung, H., Demirel, M. C. & Sitti, M. Biosynthetic self-healing materials for soft machines. Nat. Mater. 19, 1230–1235 (2020).
Li, B., Cao, P.-F., Saito, T. & Sokolov, A. P. Intrinsically self-healing polymers: from mechanistic insight to current challenges. Chem. Rev. 123, 701–735 (2023).
Khare, E., Holten-Andersen, N. & Buehler, M. J. Transition-metal coordinate bonds for bioinspired macromolecules with tunable mechanical properties. Nat. Rev. Mater. 6, 421–436 (2021).
Gohy, J.-F. Metallo-supramolecular block copolymer micelles. Coord. Chem. Rev. 253, 2214–2225 (2009).
Li, C. & Zuo, J. Self-healing polymers based on coordination bonds. Adv. Mater. 32, e1903762 (2020).
Liang, C. et al. Stiff and self-healing hydrogels by polymer entanglements in co-planar nanoconfinement. Nat. Mater. 24, 599–606 (2025).
Shi, Y., Wu, B., Sun, S. & Wu, P. Aqueous spinning of robust, self-healable, and crack-resistant hydrogel microfibers enabled by hydrogen bond nanoconfinement. Nat. Commun. 14, 1370 (2023).
Zhang, L., Bailey, J. B., Subramanian, R. H., Groisman, A. & Tezcan, F. A. Hyperexpandable, self-healing macromolecular crystals with integrated polymer networks. Nature 557, 86–91 (2018).
Kang, J. et al. Tough and water-insensitive self-healing elastomer for robust electronic skin. Adv. Mater. 30, e1706846 (2018).
Chen, J. et al. Ladderphane copolymers for high-temperature capacitive energy storage. Nature 615, 62–66 (2023).
Liu, S., Shah, D. S. & Kramer-Bottiglio, R. Highly stretchable multilayer electronic circuits using biphasic gallium-indium. Nat. Mater. 20, 851–858 (2021).
Zhao, Y. et al. A self-healing electrically conductive organogel composite. Nat. Electron. 6, 206–215 (2023).
Ni, X. et al. Soft shape-programmable surfaces by fast electromagnetic actuation of liquid metal networks. Nat. Commun. 13, 5576 (2022).
Liu, H. et al. Stimuli-driven insulator–conductor transition in a flexible polymer composite enabled by biphasic liquid metal. Adv. Mater. 33, e2104634 (2021).
Idrus-Saidi, S. A. et al. Liquid metal synthesis solvents for metallic crystals. Science 378, 1118–1124 (2022).
Duan, L. et al. Colourful liquid metals. Nat. Rev. Mater. 7, 929–931 (2022).
Daeneke, T. et al. Liquid metals: fundamentals and applications in chemistry. Chem. Soc. Rev. 47, 4073–4111 (2018).
Tang, J. et al. Dynamic configurations of metallic atoms in the liquid state for selective propylene synthesis. Nat. Nanotechnol. 19, 306–310 (2024).
Xiang, W. et al. Liquid-metal-based magnetic fluids. Nat. Rev. Mater. 9, 433–449 (2024).
Wang, H., Peng, Y., Peng, H. & Zhang, J. Fluidic phase–change materials with continuous latent heat from theoretically tunable ternary metals for efficient thermal management. Proc. Natl. Acad. Sci. USA 119, e2200223119 (2022).
Yan, J. et al. Solution processable liquid metal nanodroplets by surface-initiated atom transfer radical polymerization. Nat. Nanotechnol. 14, 684–690 (2019).
Xu, J. et al. Room-temperature self-healing soft composite network with unprecedented crack propagation resistance enabled by a supramolecular assembled lamellar structure. Adv. Mater. 35, e2300937 (2023).
Lei, Y. et al. Increased silver activity for direct propylene epoxidation via subnanometer size effects. Science 328, 224–228 (2010).
Liu, P., Qin, R., Fu, G. & Zheng, N. Surface coordination chemistry of metal nanomaterials. J. Am. Chem. Soc. 139, 2122–2131 (2017).
Yang, C. et al. Cation insertion to break the activity/stability relationship for highly active oxygen evolution reaction catalyst. Nat. Commun. 11, 1378 (2020).
Tong, X. C. Advanced Materials for Thermal Management of Electronic Packaging (Springer, 2011).
Burger, N. et al. Review of thermal conductivity in composites: Mechanisms, parameters and theory. Prog. Polym. Sci. 61, 1–28 (2016).
Kim, G.-H. et al. High thermal conductivity in amorphous polymer blends by engineered interchain interactions. Nat. Mater. 14, 295–300 (2015).
Acknowledgements
The work was supported by National Key Research and Development Program of China under Grant (grant number 2023YFB4404200, to J.Y.Z.). Basic Research Program of Jiangsu (Grant No. BK20241359, to Y.P.; BK20250075, to J.Y.Z.).
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J.Y.Z. proposed the idea and conceived the project. J.Y.Z., Z.W.L., and Y.Z. designed the experiments and performed the experiments. J.Y.Z., Z.W.L., Y.Z., S.L.L., J.Y.L., and P.Y. analyzed the results of the experiments for data. J.Y.Z., Z.W.L., and J.Y.L. wrote the manuscript. All authors commented on the manuscript.
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The patents for this strategy (NO. 2025109379401) have been submitted to the China Patent Office. The patent application (CN2025109379401) has been filed by Southeast University with inventors J.Y.Z., Z.W.L., and P.Y. The applicants for the related patents of this manuscript are author J.Y.Z., Z.W.L., and P.Y. declare that there are no other conflicts of interest related to this research. The remaining authors, Y.Z., S.L.L., and J.Y.L., who did not participate in the patent application, also declare that there are no competing interests.
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Li, Z., Zhang, Y., Liu, S. et al. A universal strategy towards self-healing materials via dynamic interfacial liquid metal coordination. Nat Commun (2026). https://doi.org/10.1038/s41467-026-69609-4
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DOI: https://doi.org/10.1038/s41467-026-69609-4
