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Oligomeric-solvent engineering of hierarchical hydrogen-bonding networks for multifunctional glass interlayers
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  • Published: 07 March 2026

Oligomeric-solvent engineering of hierarchical hydrogen-bonding networks for multifunctional glass interlayers

  • Min Li1,
  • Longyu Hu1,
  • Menghan Pi1,
  • Xiayue Yang1,
  • Xiaoyu He1,
  • Wei Cui  ORCID: orcid.org/0000-0003-3449-85241 &
  • …
  • Rong Ran  ORCID: orcid.org/0000-0001-9904-88961 

Nature Communications , Article number:  (2026) Cite this article

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We are providing an unedited version of this manuscript to give early access to its findings. Before final publication, the manuscript will undergo further editing. Please note there may be errors present which affect the content, and all legal disclaimers apply.

Subjects

  • Gels and hydrogels
  • Glasses
  • Polymers

Abstract

The properties of polymer gels are governed not only by the crosslinked network but also by the solvent. Conventional small-molecule solvents impose trade-offs among environmental adaptability, cost, and biocompatibility. Here, we employ oligomeric polyethylene glycol as a multifunctional solvent for poly (methacrylic acid) (PMAA), converting the otherwise plastic PMAA network into a transparent, dissipative gel. The oligomeric solvent promotes a hierarchical hydrogen-bonding architecture with broadly distributed strengths, coupling elasticity and viscosity, stabilizing the network, and enabling high energy dissipation for acoustic damping and impact resistance. Meanwhile, thermally reversible hydrogen-bond dissociation provides broad endothermic heat absorption, affording thermal buffering. The gels further exhibit high transparency, robust adhesion, and self-healing. Harnessing the gel as an interlayer, we fabricate laminated glass that integrates light transmission, thermal regulation, sound attenuation, and mechanical protection. This oligomer-solvent strategy offers a practical route to multifunctional, energy-efficient, safer building glazing applications in real-world architecture settings.

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Data availability

The data supporting the findings of this study are available within the Article and its Supplementary Information. All raw data are available from the corresponding author on request. Source data are provided with this paper.

References

  1. Li, X. & Gong, J. P. Design principles for strong and tough hydrogels. Nat. Rev. Mater. 9, 380–398 (2024).

    Google Scholar 

  2. Zhang, Y. S. & Khademhosseini, A. Advances in engineering hydrogels. Science 356, eaaf3627 (2017).

    Google Scholar 

  3. Feng, W. & Wang, Z. Tailoring the swelling-shrinkable behavior of hydrogels for biomedical applications. Adv. Sci. 10, 2303326 (2023).

    Google Scholar 

  4. Liu, X. et al. Recent advances in stimuli-responsive shape-morphing hydrogels. Adv. Funct. Mater. 32, 2203323 (2022).

    Google Scholar 

  5. Li, M. et al. Regulable mixed-solvent-induced phase separation in hydrogels for information encryption. Small 18, 2205359 (2022).

    Google Scholar 

  6. Sato, K. et al. Phase-separation-induced anomalous stiffening, toughening, and self-healing of polyacrylamide gels. Adv. Mater. 27, 6990–6998 (2015).

    Google Scholar 

  7. Wang, M. et al. Glassy gels toughened by solvent. Nature 631, 313–318 (2024).

    Google Scholar 

  8. Li, J. & Mooney, D. J. Designing hydrogels for controlled drug delivery. Nat. Rev. Mater. 1, 16071 (2016).

    Google Scholar 

  9. Huang, Y. et al. Strong tough polyampholyte hydrogels via the synergistic effect of ionic and metal–ligand bonds. Adv. Funct. Mater. 31, 2103917 (2021).

    Google Scholar 

  10. Gong, J. P., Katsuyama, Y., Kurokawa, T. & Osada, Y. Double-network hydrogels with extremely high mechanical strength. Adv. Mater. 15, 1155–1158 (2003).

    Google Scholar 

  11. He, X. et al. A compartmentalized nanoreactor formed by interfacial hydrogelation for cascade enzyme catalytic therapy. Angew. Chem. Int. Ed. 62, e202218766 (2023).

    Google Scholar 

  12. Kuzina, M. A., Kartsev, D. D., Stratonovich, A. V. & Levkin, P. A. Organogels versus hydrogels: advantages, challenges, and applications. Adv. Funct. Mater. 33, 2301421 (2023).

    Google Scholar 

  13. Li, M. et al. Water-induced phase separation for anti-swelling hydrogel adhesives in underwater soft electronics. Adv. Sci. 10, 2304780 (2023).

    Google Scholar 

  14. Zhang, X. et al. Intrinsic anti-freezing, tough, and transparent hydrogels for smart optical and multi-modal sensing applications. Adv. Mater. 37, 2413856 (2025).

    Google Scholar 

  15. Song, J. et al. Mechanically and electronically robust transparent organohydrogel fibers. Adv. Mater. 32, 1906994 (2020).

    Google Scholar 

  16. Fan, X. et al. Ionogels: recent advances in design, material properties and emerging biomedical applications. Chem. Soc. Rev. 52, 2497–2527 (2023).

    Google Scholar 

  17. Li, M. et al. Superstretchable, yet stiff, fatigue-resistant ligament-like elastomers. Nat. Commun. 13, 2279 (2022).

    Google Scholar 

  18. Lyu, X. et al. Multi-modal sensing ionogels with tunable mechanical properties and environmental stability for aquatic and atmospheric environments. Adv. Mater. 36, 2410572 (2024).

    Google Scholar 

  19. Shao, Y. et al. Polyfunctional eutectogels with multiple hydrogen-bond-shielded amorphous networks for soft ionotronics. Matter 7, 4076–4098 (2024).

    Google Scholar 

  20. Zhang, Y., Wang, Y., Guan, Y. & Zhang, Y. Peptide-enhanced tough, resilient and adhesive eutectogels for highly reliable strain/pressure sensing under extreme conditions. Nat. Commun. 13, 6671 (2022).

    Google Scholar 

  21. Huang, J. et al. Ultrahigh energy-dissipation elastomers by precisely tailoring the relaxation of confined polymer fluids. Nat. Commun. 12, 3610 (2021).

    Google Scholar 

  22. Chen, G. et al. Armored polymer-fluid gels with integrated damping and impact protection across broad temperatures. Sci. Adv. 11, eadv5292 (2025).

    Google Scholar 

  23. Wang, Z. et al. Tough, Transparent, 3D-Printable, and Self-Healing Poly(ethylene glycol)-Gel (PEGgel). Adv. Mater. 34, 2107791 (2022).

    Google Scholar 

  24. Wang, Z., Heck, M., Yang, W., Wilhelm, M. & Levkin, P. A. Tough PEGgels by in situ phase separation for 4D printing. Adv. Funct. Mater. 34, 2300947 (2024).

    Google Scholar 

  25. Dong, J., Ozaki, Y. & Nakashima, K. Infrared, Raman, and near-infrared spectroscopic evidence for the coexistence of various hydrogen-bond forms in poly(acrylic acid). Macromolecules 30, 1111–1117 (1997).

    Google Scholar 

  26. Zhang, X. et al. Non-monotonic information and shape evolution of polymers enabled by spatially programmed crystallization and melting. Chem. Bio Eng. 1, 790–797 (2024).

    Google Scholar 

  27. Zhou, Y. et al. Ultrasensitive ionic conductors with tunable resistance switching temperature enabled by phase transformation of polymer cocrystals. Adv. Mater. 36, 2309568 (2024).

    Google Scholar 

  28. Schmidt, R. F., Lutzki, J., Dalgliesh, R., Prévost, S. & Gradzielski, M. pH-responsive rheology and structure of poly(ethylene oxide)–poly(methacrylic acid) interpolymer complexes. Macromolecules 58, 321–333 (2025).

    Google Scholar 

  29. Tajiri, T., Morita, S. & Ozaki, Y. Hydration mechanism on a poly(methacrylic acid) film studied by in situ attenuated total reflection infrared spectroscopy. Polymer 50, 5765–5770 (2009).

    Google Scholar 

  30. Lin, X. et al. A viscoelastic adhesive epicardial patch for treating myocardial infarction. Nat. Biomed. Eng. 3, 632–643 (2019).

    Google Scholar 

  31. Wang, Y.-J. et al. Polymer pressure-sensitive adhesive with a temperature-insensitive loss factor operating under water and oil. Adv. Funct. Mater. 31, 2104296 (2021).

    Google Scholar 

  32. Pasek-Allen, J. L., Wilharm, R. K., Bischof, J. C. & Pierre, V. C. NMR Characterization of Polyethylene Glycol Conjugates for Nanoparticle Functionalization. ACS Omega 8, 4331–4336 (2023).

    Google Scholar 

  33. Pranjali, P. et al. Physicochemical and antibacterial properties of pegylated zinc oxide nanoparticles dispersed in peritoneal dialysis fluid. ACS Omega 4, 19255–19264 (2019).

    Google Scholar 

  34. Xie, J., Xu, C., Kohler, N., Hou, Y. & Sun, S. Controlled PEGylation of Monodisperse Fe3O4 nanoparticles for reduced non-specific uptake by macrophage cells. Adv. Mater. 19, 3163–3166 (2007).

    Google Scholar 

  35. Yu, S., An, S. J., Kim, K. J., Lee, J. H. & Chi, W. S. High-Loading Poly(ethylene glycol)-Blended Poly(acrylic acid) Membranes for CO2 Separation. ACS Omega 8, 2119–2127 (2023).

    Google Scholar 

  36. Park, J. et al. Biodegradable block copolymer–tannic acid glue. JACS Au 2, 1978–1988 (2022).

    Google Scholar 

  37. Xie, X. et al. A solvent-free processed low-temperature tolerant adhesive. Nat. Commun. 15, 5017 (2024).

    Google Scholar 

  38. Guo, R. et al. Extremely strong and tough biodegradable poly(urethane) elastomers with unprecedented crack tolerance via hierarchical hydrogen-bonding interactions. Adv. Mater. 35, 2212130 (2023).

    Google Scholar 

  39. Kim, M. J., Cho, S. H., Oh, S. J. & Kim, S. W. Ultrastretchable, fatigue-resistant eutectogel with hierarchical bonding for advanced wearable monitoring. Adv. Compos. Hybrid Mater. 8, 323 (2025).

    Google Scholar 

  40. Peng, W. et al. A strong and tough ion-gel enabled by hierarchical meshing and ion hybridizations collaboration. Adv. Funct. Mater. 35, 2414682 (2025).

    Google Scholar 

  41. Sun, T. L. et al. Molecular structure of self-healing polyampholyte hydrogels analyzed from tensile behaviors. Soft Matter 11, 9355–9366 (2015).

    Google Scholar 

  42. Webber, R. E., Creton, C., Brown, H. R. & Gong, J. P. Large strain hysteresis and mullins effect of tough double-network hydrogels. Macromolecules 40, 2919–2927 (2007).

    Google Scholar 

  43. Cui, K. et al. Stretching-induced ion complexation in physical polyampholyte hydrogels. Soft Matter 12, 8833–8840 (2016).

    Google Scholar 

  44. Rubinstein, M. & Panyukov, S. Elasticity of polymer networks. Macromolecules 35, 6670–6686 (2002).

    Google Scholar 

  45. Wang, Z. et al. Hydrogen bonds-pinned entanglement blunting the interfacial crack of hydrogel–elastomer hybrids. Adv. Mater. 36, 2313177 (2024).

    Google Scholar 

  46. Ye, H., Wu, B., Sun, S. & Wu, P. Self-compliant ionic skin by leveraging hierarchical hydrogen bond association. Nat. Commun. 15, 885 (2024).

    Google Scholar 

  47. Ge, S., Tsao, Y.-H. & Evans, C. M. Polymer architecture dictates multiple relaxation processes in soft networks with two orthogonal dynamic bonds. Nat. Commun. 14, 7244 (2023).

    Google Scholar 

  48. Lewis, C. L., Stewart, K. & Anthamatten, M. The influence of hydrogen bonding side-groups on viscoelastic behavior of linear and network polymers. Macromolecules 47, 729–740 (2014).

    Google Scholar 

  49. Ewoldt, R. H., Winter, P., Maxey, J. & McKinley, G. H. Large amplitude oscillatory shear of pseudoplastic and elastoviscoplastic materials. Rheol. Acta 49, 191–212 (2010).

    Google Scholar 

  50. Cheng, J. et al. Sterically Hindered Organogels with Self-Healing, Impact Response, and High Damping Properties. Adv. Mater. 36, 2411700 (2024).

    Google Scholar 

  51. Yi, B. et al. Surface hydrophobization of hydrogels via interface dynamics-induced network reconfiguration. Nat. Commun. 15, 239 (2024).

    Google Scholar 

  52. Long, R. & Hui, C.-Y. Fracture toughness of hydrogels: measurement and interpretation. Soft Matter 12, 8069–8086 (2016).

    Google Scholar 

Download references

Acknowledgements

This work was supported mainly by the National Natural Science Foundation of China (52473238 (W.C.), 52203027 (W.C.), 52573231 (R.R.)), the Sichuan Science and Technology Program (2024NSFSC0245 (W.C.), 2025ZNSFSC0340 (R.R.)), the State Key Laboratory of Polymer Materials Engineering (sklpme-2024-01-04 (R.R.)), and the State Key Laboratory of Advanced Polymer Materials (sklamp2025-2-04 (W.C.)). The authors also gratefully acknowledge the support from the Sichuan Province Advanced Building Materials Production-Education Integration Innovation Demonstration Platform.

Author information

Authors and Affiliations

  1. College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, China

    Min Li, Longyu Hu, Menghan Pi, Xiayue Yang, Xiaoyu He, Wei Cui & Rong Ran

Authors
  1. Min Li
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  2. Longyu Hu
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Contributions

R.R. and W.C. conceived and supervised the project and designed the experiments. M.L. performed the majority of the experiments. L.H., X.Y., and X.H. assisting in sample synthesis and M.P. supporting the Molecular Dynamics simulations. M.L., R.R., and W.C. co-wrote and revised the paper. All authors discussed the results and commented on the manuscript.

Corresponding authors

Correspondence to Wei Cui or Rong Ran.

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Li, M., Hu, L., Pi, M. et al. Oligomeric-solvent engineering of hierarchical hydrogen-bonding networks for multifunctional glass interlayers. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70223-7

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  • Received: 16 September 2025

  • Accepted: 23 February 2026

  • Published: 07 March 2026

  • DOI: https://doi.org/10.1038/s41467-026-70223-7

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