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Strong and recyclable bio-derived poly(ester amide) hot-melt adhesive

Abstract

Bio-based adhesives offer inherent advantages over conventional petrochemical-derived systems, including renewable sourcing, reduced environmental impact and potential degradability. However, most bio-based adhesives suffer from poor adhesion strength, limited substrate compatibility and a lack of chemical recyclability. Here we present a bio-derived multiblock poly(ester amide) adhesive that leverages microphase segregation between different segments to reconcile mechanical robustness with strong interfacial bonding. Notably, this multiblock architecture is accessed through a one-pot, selective acceptorless dehydrogenative polymerization, obviating the need for multistep synthesis. The materials exhibit excellent adhesion across a range of substrates including metals, glass and wet wood surpassing commercial benchmarks, while also demonstrating thermal stability, tunable mechanical properties and closed-loop chemical recyclability even in the presence of other commodity plastics. Furthermore, the adhesive strength of these materials could be tuned for various potential applications through control over the chemical composition of the polymer. By integrating renewable feedstocks, high-performance functionality and efficient chemical circularity within a single platform, this work provides a viable pathway toward more sustainable adhesive technologies and contributes to advancing circular materials manufacturing.

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Fig. 1: Synthetic overview of recyclable and bio-based multiblock PEA materials.
Fig. 2: Comprehensive property evaluation of the PEA materials.
Fig. 3: Evaluation of adhesion strength of PEA materials.
Fig. 4: Recycling of PEA materials.

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Full experimental details and the data supporting the findings of this study are available within the article and its Supplementary Information. Source data are provided with this paper.

References

  1. Cui, C. & Liu, W. Recent advances in wet adhesives: adhesion mechanism, design principle and applications. Prog. Polym. Sci. 116, 101388 (2021).

    Article  CAS  Google Scholar 

  2. Imam, S. H., Bilbao-Sainz, C., Chiou, B., Glenn, G. M. & Orts, W. J. Biobased adhesives, gums, emulsions, and binders: current trends and future prospects. J. Adhes. Sci. Technol. 27, 1972–1997 (2013).

    Article  CAS  Google Scholar 

  3. Petrie, E. M. Handbook of Adhesive and Sealants 2nd edn (McGraw-Hill, 2007).

  4. Heinrich, L. A. Future opportunities for bio-based adhesives – advantages beyond renewability. Green Chem. 21, 1866–1888 (2019).

    Article  CAS  Google Scholar 

  5. Adhesives and Sealants Market Size, Share & Trends Analysis Report, 2024–2030 (Grand View Research, accessed 17 June 2025); https://www.grandviewresearch.com/industry-analysis/adhesives-and-sealants-market

  6. Pocius, A. V. Adhesion and Adhesives Technology: An Introduction (Carl Hanser Verlag, 2021).

  7. Engels, T. in Thermosets (ed Guo, Q.) Ch. 8 (Woodhead, 2012).

  8. Pethrick, R. A. Design and ageing of adhesives for structural adhesive bonding - a review. Proc. Inst. Mech. Eng. L 229, 349–379 (2015).

    CAS  Google Scholar 

  9. Ma, Y. et al. Research advances in bio-based adhesives. Int. J. Adhes. Adhes. 126, 103444 (2023).

    Article  CAS  Google Scholar 

  10. Pereira, J. R. et al. Demonstration of the adhesive properties of the medium-chain-length polyhydroxyalkanoate produced by Pseudomonas chlororaphis subsp. aurantiaca from glycerol. Int. J. Biol. Macromol. 122, 1144–1151 (2019).

    Article  CAS  Google Scholar 

  11. Yang, G., Gong, Z., Luo, X., Chen, L. & Shuai, L. Bonding wood with uncondensed lignins as adhesives. Nature 621, 511–515 (2023).

    Article  CAS  Google Scholar 

  12. Lv, Z. et al. Bio-based hot-melt adhesive from xylan. Nat. Sustain. 8, 827–836 (2025).

    Article  Google Scholar 

  13. Zhou, Y. et al. High strength and flame retardant soybean polysaccharide-based wood adhesive produced by borate chemistry and crosslinking strategy. Eur. Polym. J. 164, 110973 (2022).

    Article  CAS  Google Scholar 

  14. Zhang, Z. et al. Stereomicrostructure-regulated biodegradable adhesives. Science 387, 297–303 (2025).

    Article  CAS  Google Scholar 

  15. Westerman, C. R., McGill, B. C. & Wilker, J. J. Sustainably sourced components to generate high-strength adhesives. Nature 621, 306–311 (2023).

    Article  CAS  Google Scholar 

  16. Zhao, Y. et al. Chemically recyclable polyolefin-like multiblock polymers. Science 382, 310–314 (2023).

    Article  CAS  Google Scholar 

  17. Liu, X. et al. Catalytic closed-loop recycling of polyethylene-like materials produced by acceptorless dehydrogenative polymerization of bio-derived diols. Nat. Chem. 17, 500–506 (2025).

    Article  Google Scholar 

  18. Zhao, Y. et al. Tailoring the properties of chemically recyclable polyethylene-like multiblock polymers by modulating the branch structure. Angew. Chem. Int. Ed. 137, e202415707 (2025).

    Article  Google Scholar 

  19. Han, S. & Wu, J. Recent advances of poly(ester amide)s-based biomaterials. Biomacromolecules 23, 1892–1919 (2022).

    Article  CAS  Google Scholar 

  20. Rodriguez-Galan, A., Franco, L. & Puiggali, J. Degradable poly(ester amide)s for biomedical applications. Polymers 3, 65–99 (2011).

    Article  CAS  Google Scholar 

  21. Winnacker, M. & Rieger, B. Poly(ester amide)s: recent insights into synthesis, stability and biomedical applications. Polym. Chem. 7, 7039–7046 (2016).

    Article  CAS  Google Scholar 

  22. He, J., Ding, Y., Jiang, F. & Wang, Z. Poly(ester amide)s derived from low-value plant oil as reusable low-temperature tolerant adhesive. Eur. Polym. J. 198, 112387 (2023).

    Article  CAS  Google Scholar 

  23. Yoshinaka, Y. & Miller, S. A. Bio-oil derived polyesteramides as water-degradable replacements for polyethylene. Green Chem. 27, 4152–4164 (2025).

    Article  CAS  Google Scholar 

  24. Zeng, H. & Guan, Z. Direct synthesis of polyamides via catalytic dehydrogenation of diols and diamines. J. Am. Chem. Soc. 133, 1159–1161 (2011).

    Article  CAS  Google Scholar 

  25. Filonenko, G. A., Putten, R., Hensen, E. J. M. & Pidko, E. A. Catalytic (de)hydrogenation promoted by non-precious metals – Co, Fe and Mn: recent advances in an emerging field. Chem. Soc. Rev. 47, 1459–1483 (2018).

    Article  CAS  Google Scholar 

  26. Gunanathan, C. & Milstein, D. Bond activation and catalysis by ruthenium pincer complexes. Chem. Rev. 114, 12024–12087 (2014).

    Article  CAS  Google Scholar 

  27. Li, H., Wang, X., Huang, F., Jiang, J. & Wang, Z. Computational study on the catalytic role of pincer ruthenium (II)-PNN complex in directly synthesizing amide from alcohol and amine: the origin of selectivity of amide over ester and imine. Organometallics 30, 5233–5247 (2011).

    Article  CAS  Google Scholar 

  28. Beyer, V. P., Kim, J. & Becer, C. R. Synthetic approaches for multiblock copolymers. Polym. Chem. 11, 1271–1291 (2020).

    Article  CAS  Google Scholar 

  29. Dau, H. et al. Linear block copolymer synthesis. Chem. Rev. 122, 14471–14553 (2022).

    Article  CAS  Google Scholar 

  30. Pingen, D. et al. Diamines for polymer materials via direct amination of lipid- and lignocellulose-based alcohols with NH3. ChemCatChem 10, 3027–3033 (2018).

    Article  CAS  Google Scholar 

  31. Tuominen, J. & Seppälä, J. V. Synthesis and characterization of lactic acid based poly(ester−amide). Macromolecules 33, 3530–3535 (2000).

    Article  CAS  Google Scholar 

  32. Regaño, C., Alla, A., Ilarduya, A. M. & Muñoz-Guerra, S. Poly(ester amide)s derived from L-malic acid. Macromolecules 37, 2067–2075 (2004).

    Article  Google Scholar 

  33. Mahadas, N. A. et al. High molecular weight biobased long-chain aliphatic polyesters with degradability: insights into mimicking polyethylene. Macromolecules 58, 4070–4081 (2025).

    Article  CAS  Google Scholar 

  34. Wolfgang, G. & Ruestem, D. Nylon-12-preparation, properties, and applications. Ind. Eng. Chem. 62, 16–22 (1970).

    Article  Google Scholar 

  35. Luckachan, E. G. & Pillai, C. K. S. Random multiblock poly(ester amide)s containing poly(L-lactide) and cycloaliphatic amide segments: synthesis and biodegradation studies. J. Polym. Sci. A Polym. Chem. 44, 3250–3260 (2006).

    Article  CAS  Google Scholar 

  36. Michell, R. M. et al. Effect of sequence distribution on the morphology, crystallization, melting, and biodegradation of poly(ε-caprolactone-co-ε-caprolactam) copolymers. Macromolecules 42, 6671–6681 (2009).

    Article  CAS  Google Scholar 

  37. Hamley, I. W. et al. Crystallization in poly(l-lactide)-b-poly(ε-caprolactone) double crystalline diblock copolymers: a study using X-ray scattering, differential scanning calorimetry, and polarized optical microscopy. Macromolecules 38, 463–472 (2005).

    Article  CAS  Google Scholar 

  38. Marques, E. A. S., da Silva, L. F. M., Banea, M. D. & Carbas, R. J. C. Adhesive joints for low- and high-temperature use: an overview. J. Adhes. 91, 556–585 (2015).

    Article  CAS  Google Scholar 

  39. Viana, G., Costa, M., Banea, M. D. & da silva, L. F. M. A review on the temperature and moisture degradation of adhesively bonded joints. Proc. Inst. Mech. Eng. Part L J. Mater. Des. Appl. 231, 488–501 (2017).

    Google Scholar 

  40. Ellis, L. D. et al. Chemical and biological catalysis for plastics recycling and upcycling. Nat. Catal. 4, 539–556 (2021).

    Article  CAS  Google Scholar 

  41. Khopade, K. V., Chikkali, S. H. & Barsu, N. Metal-catalyzed plastic depolymerization. Cell Rep Phys Sci 4, 101341 (2023).

    Article  CAS  Google Scholar 

  42. Kumar, A. et al. Hydrogenative depolymerization of nylons. J. Am. Chem. Soc. 142, 14267–14275 (2020).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Institutes of Health under grant no. R35GM144356 and RePLACE (Redesigning Polymers to Leverage a Circular Economy) funded by the Office of Science of the US Department of Energy through grant no. DE-SC0022290. The authors thank the Analytical Resources Core (RRID: SCR_021759) at Colorado State University for instrument access. G.M.M. acknowledges support from the Dr. Robert Williams Professorship in Organic Chemistry at Colorado State University. Funding for J.M. and N.A.R. was provided by the US Department of Energy, Office of Energy Efficiency and Renewable Energy, Advanced Materials and Manufacturing Technologies Office (AMMTO) and Bioenergy Technologies Office (BETO) as part of the BOTTLE Consortium, supported by AMMTO and BETO under contract no. DE-AC36-08GO28308 with the National Renewable Energy Laboratory, operated by Alliance for Sustainable Energy, LLC.

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Authors

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X.L. and G.M.M. conceived the idea. X.L. designed and conducted experiments and analysed results. X.L., Y.Z., K.L.H., E.M.R., J.M. and N.A.R. performed characterization and analysed results. X.L. wrote the initial manuscript and supplemental materials. All authors read and edited the manuscript. G.M.M. directed the project.

Corresponding author

Correspondence to Garret M. Miyake.

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Nature Sustainability thanks Feng Peng and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Liu, X., Harry, K.L., Zhao, Y. et al. Strong and recyclable bio-derived poly(ester amide) hot-melt adhesive. Nat Sustain 9, 450–458 (2026). https://doi.org/10.1038/s41893-026-01776-0

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