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Laser-assisted direct three-dimensional printing of free-standing thermoset devices

Abstract

The three-dimensional printing of thermoset materials is of use in the development of flexible electronics and soft robotics. However, the process typically involves the deposition and removal of supporting materials that require extensive cycles of pre- and post-processing. Here we describe a three-dimensional printing method for constructing functional and arbitrary free-standing thermoset structures without using supporting materials. The approach integrates in situ laser-induced solidification with direct ink writing. During printing, the integrated laser is focused on a micro-sized polymer jet, leading to thermoset crosslinking in less than 0.25 s through a strong photothermal effect. The process offers a resolution as fine as 50 μm, with mechanical properties tunable by up to tenfold and electrical properties by up to 20-fold. We used this approach to print stretchable electronics with stiffness gradients for strain inhibition, flexible sensors with high sensitivity and three-dimensional soft magnetic robots for actuation functions.

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Fig. 1: Rapid in situ laser-assisted direct 3D printing of thermoset sensors and actuators.
Fig. 2: ISLI printing for rapid in situ gelation based on the photothermal effect.
Fig. 3: Optical pictures of unsupported 3D structures with diverse thermosets.
Fig. 4: Demonstration of ISLI printing of stretchable electronics-based substrates with various stiffness regions.
Fig. 5: ISLI printing for flexible sensors.
Fig. 6: ISLI printing process of free-standing structures for magnetically actuated soft robots.

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Data availability

Source data are provided with this paper. Other data related to this work are available from the corresponding authors upon reasonable request.

Code availability

The code used in this work is available via Zenodo at https://doi.org/10.5281/zenodo.17121654 (ref. 59).

References

  1. Li, G. et al. Three-dimensional flexible electronics using solidified liquid metal with regulated plasticity. Nat. Electron. 6, 154–163 (2023).

    Article  Google Scholar 

  2. Kim, D.-H. et al. Epidermal electronics. Science 333, 838–843 (2011).

    Article  Google Scholar 

  3. Robertson, I. D. et al. Rapid energy-efficient manufacturing of polymers and composites via frontal polymerization. Nature 557, 223–227 (2018).

    Article  Google Scholar 

  4. Kim, Y., Yuk, H., Zhao, R., Chester, S. A. & Zhao, X. Printing ferromagnetic domains for untethered fast-transforming soft materials. Nature 558, 274–279 (2018).

    Article  Google Scholar 

  5. Rich, S. I., Wood, R. J. & Majidi, C. Untethered soft robotics. Nat. Electron. 1, 102–112 (2018).

    Article  Google Scholar 

  6. Shi, J. et al. Embedment of sensing elements for robust, highly sensitive, and cross-talk–free iontronic skins for robotics applications. Sci. Adv. 9, eadf8831 (2023).

    Article  Google Scholar 

  7. Ligon, S. C., Liska, R., Stampfl, J., Gurr, M. & Mülhaupt, R. Polymers for 3D printing and customized additive manufacturing. Chem. Rev. 117, 10212–10290 (2017).

    Article  Google Scholar 

  8. Valino, A. D. et al. Advances in 3D printing of thermoplastic polymer composites and nanocomposites. Prog. Polym. Sci. 98, 101162 (2019).

    Article  Google Scholar 

  9. Liu, Z. et al. Chemical upcycling of commodity thermoset polyurethane foams towards high-performance 3D photo-printing resins. Nat. Chem. 15, 1773–1779 (2023).

    Article  Google Scholar 

  10. Mohanty, A. K. et al. Sustainable polymers. Nat. Rev. Methods PrimERS 2, 46 (2022).

    Article  Google Scholar 

  11. Li, G. et al. Self-powered soft robot in the Mariana Trench. Nature 591, 66–71 (2021).

    Article  Google Scholar 

  12. Zhang, J. et al. Voxelated three-dimensional miniature magnetic soft machines via multimaterial heterogeneous assembly. Sci. Robot. 6, eabf0112 (2021).

    Article  Google Scholar 

  13. Mao, G. et al. Ultrafast small-scale soft electromagnetic robots. Nat. Commun. 13, 4456 (2022).

    Article  Google Scholar 

  14. Yang, Y. et al. Magnetic soft robotic bladder for assisted urination. Sci. Adv. 8, eabq1456 (2022).

    Article  Google Scholar 

  15. Zhou, C. et al. Ferromagnetic soft catheter robots for minimally invasive bioprinting. Nat. Commun. 12, 5072 (2021).

    Article  Google Scholar 

  16. Tang, W. et al. Customizing a self-healing soft pump for robot. Nat. Commun. 12, 2247 (2021).

    Article  Google Scholar 

  17. Kim, Y., Parada, G. A., Liu, S. & Zhao, X. Ferromagnetic soft continuum robots. Sci. Robot. 4, eaax7329 (2019).

    Article  Google Scholar 

  18. Zhu, Z., Ng, D. W. H., Park, H. S. & McAlpine, M. C. 3D-printed multifunctional materials enabled by artificial-intelligence-assisted fabrication technologies. Nat. Rev. Mater. 6, 27–47 (2021).

    Article  Google Scholar 

  19. Lopez de Pariza, X. et al. Recyclable photoresins for light-mediated additive manufacturing towards loop 3D printing. Nat. Commun. 14, 5504 (2023).

    Article  Google Scholar 

  20. Kuang, X. et al. Grayscale digital light processing 3D printing for highly functionally graded materials. Sci. Adv. 5, eaav5790 (2019).

    Article  Google Scholar 

  21. Tumbleston, J. R. et al. Continuous liquid interface production of 3D objects. Science 347, 1349–1352 (2015).

    Article  Google Scholar 

  22. Bhattacharjee, N., Parra-Cabrera, C., Kim, Y. T., Kuo, A. P. & Folch, A. Desktop stereolithography 3D-printing of a poly(dimethylsiloxane)-based material with Sylgard-184 properties. Adv. Mater. 30, 1800001 (2018).

    Article  Google Scholar 

  23. Kim, F. et al. Direct ink writing of three-dimensional thermoelectric microarchitectures. Nat. Electron. 4, 579–587 (2021).

    Article  Google Scholar 

  24. Saadi, M. et al. Direct ink writing: a 3D printing technology for diverse materials. Adv. Mater. 34, 2108855 (2022).

    Article  Google Scholar 

  25. Zhang, P. et al. Integrated 3D printing of flexible electroluminescent devices and soft robots. Nat. Commun. 13, 4775 (2022).

    Article  Google Scholar 

  26. Lewis, J. A. Direct ink writing of 3D functional materials. Adv. Funct. Mater. 16, 2193–2204 (2006).

    Article  Google Scholar 

  27. Ober, T. J., Foresti, D. & Lewis, J. A. Active mixing of complex fluids at the microscale. Proc. Natl Acad. Sci. USA 112, 12293–12298 (2015).

    Article  Google Scholar 

  28. Hardin, J. O., Ober, T. J., Valentine, A. D. & Lewis, J. A. Microfluidic printheads for multimaterial 3D printing of viscoelastic inks. Adv. Mater. 27, 3279–3284 (2015).

    Article  Google Scholar 

  29. Giachini, P. et al. Additive manufacturing of cellulose-based materials with continuous, multidirectional stiffness gradients. Sci. Adv. 6, eaay0929 (2020).

    Article  Google Scholar 

  30. Kokkinis, D., Schaffner, M. & Studart, A. R. Multimaterial magnetically assisted 3D printing of composite materials. Nat. Commun. 6, 8643 (2015).

    Article  Google Scholar 

  31. Xie, R. et al. Magnetically driven formation of 3D freestanding soft bioscaffolds. Sci. Adv. 10, eadl1549 (2024).

    Article  Google Scholar 

  32. Sun, Y. et al. 3D printing of thermosets with diverse rheological and functional applicabilities. Nat. Commun. 14, 245 (2023).

    Article  Google Scholar 

  33. Habibi, M., Foroughi, S., Karamzadeh, V. & Packirisamy, M. Direct sound printing. Nat. Commun. 13, 1800 (2022).

    Article  Google Scholar 

  34. Yao, G. et al. Sound continuous production of thermosets. Adv. Funct. Mater. 34, 2312736 (2024).

    Article  Google Scholar 

  35. Kuang, X. et al. Self-enhancing sono-inks enable deep-penetration acoustic volumetric printing. Science 382, 1148–1155 (2023).

    Article  Google Scholar 

  36. Skylar-Scott, M. A., Gunasekaran, S. & Lewis, J. A. Laser-assisted direct ink writing of planar and 3D metal architectures. Proc. Natl Acad. Sci. 113, 6137–6142 (2016).

    Article  Google Scholar 

  37. Zhao, Y. et al. 3D printing of unsupported multi-scale and large-span ceramic via near-infrared assisted direct ink writing. Nat. Commun. 14, 2381 (2023).

    Article  Google Scholar 

  38. Zhu, J., Zhang, Q., Yang, T., Liu, Y. & Liu, R. 3D printing of multi-scalable structures via high penetration near-infrared photopolymerization. Nat. Commun. 11, 3462 (2020).

    Article  Google Scholar 

  39. Wang, Z. et al. Three-dimensional printing of functionally graded liquid crystal elastomer. Sci. Adv. 6, eabc0034 (2020).

    Article  Google Scholar 

  40. Peng, X. et al. 4D printing of freestanding liquid crystal elastomers via hybrid additive manufacturing. Adv. Mater. 34, 2204890 (2022).

    Article  Google Scholar 

  41. Sun, Y. et al. A 3D printed ferromagnetic liquid crystal elastomer with programmed dual anisotropy and multi responsiveness. Adv. Mater. 35, 2302824 (2023).

    Article  Google Scholar 

  42. Wang, Q. et al. Programmable spatial deformation by controllable off-center freestanding 4D printing of continuous fiber reinforced liquid crystal elastomer composites. Nat. Commun. 14, 3869 (2023).

    Article  Google Scholar 

  43. Wehner, M. et al. An integrated design and fabrication strategy for entirely soft, autonomous robots. Nature 536, 451–455 (2016).

    Article  Google Scholar 

  44. Duraivel, S. et al. A silicone-based support material eliminates interfacial instabilities in 3D silicone printing. Science 379, 1248–1252 (2023).

    Article  Google Scholar 

  45. O’Bryan, C. S. et al. Self-assembled micro-organogels for 3D printing silicone structures. Sci. Adv. 3, e1602800 (2017).

    Article  Google Scholar 

  46. Hui, Y. et al. Three-dimensional printing of soft hydrogel electronics. Nat. Electron. 5, 893–903 (2022).

    Article  Google Scholar 

  47. Lee, A. et al. 3D bioprinting of collagen to rebuild components of the human heart. Science 365, 482–487 (2019).

    Article  Google Scholar 

  48. Ziaee, M., Johnson, J. W. & Yourdkhani, M. 3D printing of short-carbon-fiber-reinforced thermoset polymer composites via frontal polymerization. ACS Appl. Mater. Interfaces 14, 16694–16702 (2022).

    Article  Google Scholar 

  49. Aabith, S. et al. 3D direct-write printing of water soluble micromoulds for high-resolution rapid prototyping. Addit. Manuf. 58, 103019 (2022).

    Google Scholar 

  50. Wang, Z. et al. Stretchable materials of high toughness and low hysteresis. Proc. Natl Acad. Sci. USA 116, 5967–5972 (2019).

    Article  Google Scholar 

  51. Zhou, L. Y., Fu, J. & He, Y. A review of 3D printing technologies for soft polymer materials. Adv. Funct. Mater. 30, 2000187 (2020).

    Article  Google Scholar 

  52. Wang, Y. & Willenbacher, N. Phase change enabled, rapid, high resolution direct ink writing of soft silicone. Adv. Mater. 34, 2109240 (2022).

    Article  Google Scholar 

  53. Sivaraman, D. et al. Additive manufacturing of nanocellulose aerogels with structure oriented thermal, mechanical, and biological properties. Adv. Sci. 11, e2307921 (2024).

    Article  Google Scholar 

  54. Gu, H. et al. Magnetic cilia carpets with programmable metachronal waves. Nat. Commun. 11, 2637 (2020).

    Article  Google Scholar 

  55. Liu, X. et al. Magnetic soft microfiberbots for robotic embolization. Sci. Robot. 9, eadh2479 (2024).

    Article  Google Scholar 

  56. Stieghorst, J. & Doll, T. Rheological behavior of PDMS silicone rubber for 3D printing of medical implants. Addit. Manuf. 24, 217–223 (2018).

    Google Scholar 

  57. Zhao, R., Kim, Y., Chester, S. A., Sharma, P. & Zhao, X. Mechanics of hard-magnetic soft materials. J. Mech. Phys. Solids 124, 244–263 (2019).

    Article  MathSciNet  Google Scholar 

  58. Wang, L. et al. Evolutionary design of magnetic soft continuum robots. Proc. Natl Acad. Sci. USA 118, e2021922118 (2021).

    Article  Google Scholar 

  59. Zhuang, Q. Laser-assisted direct three-dimensional printing of freestanding thermoset devices. Zenodo https://doi.org/10.5281/zenodo.17121654 (2025).

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 52075464) and the Science & Technology Plan of Xiamen City (Grant No. 3502Z20224030, both grants to D.W.).

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Authors and Affiliations

Authors

Contributions

Q.Z. and D.W. conceived the concept and proposed the project. Q.Z., Y.Z. and X.L. conducted the experiments. Z.C., W.X. and L. Lu conducted the FEA. Q.Z. and D.W. wrote the paper. S.C., Q.C. and L.Z. commented on the organization of the figures. Z.D., D.S., C.Y., S.P. and L. Lin revised the paper. All authors discussed the results and commented on the paper.

Corresponding authors

Correspondence to Liwei Lin or Dezhi Wu.

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Nature Electronics thanks Kunal Masania and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

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Supplementary Information (download PDF )

Supplementary Notes 1–4, Tables 1–4, Figs. 1–36, Captions to Videos 1–4 and Refs. 1–41.

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Supplementary Video 1 (download MP4 )

ISLI printing of diverse 3D freestanding thermoset structures.

Supplementary Video 2 (download MP4 )

Stretchable electronics with stiffness gradients.

Supplementary Video 3 (download MP4 )

ISLI printing process of freestanding structures for magnetically actuated soft robots.

Supplementary Video 4 (download MP4 )

Locomotion and potential applications of the magnetically actuated soft robots.

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Source data for Fig. 5d–f,h.

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Zhuang, Q., Zhang, Y., Liu, X. et al. Laser-assisted direct three-dimensional printing of free-standing thermoset devices. Nat Electron 8, 1059–1071 (2025). https://doi.org/10.1038/s41928-025-01491-2

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