Hydrophobic Eutectogels Reinforced by Zn2+-Coordinated Lignin Nanoparticles for Underwater Wearable Electronics
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Abstract
Abstract Wearable flexible sensors for underwater communication and biomotion monitoring are gaining attention. However, developing gel-based strain sensors with high toughness, anti-swelling performance, robust underwater adhesion, and long-term stability remains challenging. Herein, we present a hydrophobic eutectogel (DPF-Zn@LNP-HEG) fabricated via the assembly of a polymerizable hydrophobic deep eutectic solvent (PHDES), 2-phenoxyethyl acrylate (PEA), and Zn 2+ -coordinated lignin nanoparticles (Zn@LNP). The resulting structure, composed of hydrophobic polymer networks and metal-phenolic complexes, forms hydrophobic microdomains that disrupt the hydration layer and prevent water penetration. Meanwhile, Zn@LNP serve as dynamic sacrificial cross-linkers, enhancing the material’s mechanical strength, energy dissipation, and anti-swelling properties. The resulting eutectogel exhibits remarkable tensile strength (1.14 MPa), superior toughness (3.15 MJ m −3 ), excellent anti-swelling properties (< 1% after 30 days), and robust underwater adhesion (1.07 MPa on glass). Based on these properties, we demonstrate an underwater strain sensor with high sensitivity (gauge factor = 8.12) and long-term stability, enabling underwater Morse code transmission, biomotion monitoring, and Bluetooth-based tracking of swimming movements. This work not only provides a versatile design paradigm for multifunctional underwater sensing platforms but also advances the high-value utilization of bio-based materials in next-generation flexible electronics.
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References (65)
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1. H. Liu, H. Chu, H. Yuan, D. Li, W. Deng et al., Bioinspired multifunctional self-sensing actuated gradient hydrogel for soft-hard robot remote interaction. Nano-Micro Lett. 16(1), 69 (2024). https://doi.org/10.1007/s40820-023-01287-z10.1007/s40820-023-01287-z ↗
2. B. Zhao, Z. Bai, H. Lv, Z. Yan, Y. Du et al., Self-healing liquid metal magnetic hydrogels for smart feedback sensors and high-performance electromagnetic shielding. Nano-Micro Lett. 15(1), 79 (2023). https://doi.org/10.1007/s40820-023-01043-310.1007/s40820-023-01043-3 ↗
3. Z.-C. Xu, Y.-Q. Yang, X.-W. Pang, Y.-T. Xu, L.-X. Gong et al., Mechanical tough, non-swelling, self-adhesive and highly conductive amphibious hydrogels for motion sensing in complex conditions. J. Mater. Sci. Technol. 237, 10–19 (2025). https://doi.org/10.1016/j.jmst.2025.02.05210.1016/j.jmst.2025.02.052 ↗
4. M. Li, H. Lu, M. Pi, H. Zhou, Y. Wang et al., Water-induced phase separation for anti-swelling hydrogel adhesives in underwater soft electronics. Adv. Sci. 10(32), 2304780 (2023). https://doi.org/10.1002/advs.20230478010.1002/advs.202304780 ↗
5. J. Ren, G. Chen, H. Yang, J. Zheng, S. Li et al., Super-tough, non-swelling zwitterionic hydrogel sensor based on the hofmeister effect for potential motion monitoring of marine animals. Adv. Mater. 36(48), 2412162 (2024). https://doi.org/10.1002/adma.20241216210.1002/adma.202412162 ↗
6. Q. Liang, D. Zhang, T. He, Z. Zhang, H. Wang et al., Fiber-based noncontact sensor with stretchability for underwater wearable sensing and VR applications. ACS Nano 18(1), 600–611 (2024). https://doi.org/10.1021/acsnano.3c0873910.1021/acsnano.3c08739 ↗
7. Z. Ding, G. Li, Y. Wang, C. Du, Z. Ye et al., Ultrafast response and threshold adjustable intelligent thermoelectric systems for next-generation self-powered remote IoT fire warning. Nano-Micro Lett. 16(1), 242 (2024). https://doi.org/10.1007/s40820-024-01453-x10.1007/s40820-024-01453-x ↗
8. S. Zhang, F. Guo, X. Gao, M. Yang, X. Huang et al., High-strength, antiswelling directional layered PVA/MXene hydrogel for wearable devices and underwater sensing. Adv. Sci. 11(39), 2405880 (2024). https://doi.org/10.1002/advs.20240588010.1002/advs.202405880 ↗
9. Y. Liu, J. Song, Z. Liu, J. Chen, D. Wang et al., Anti-swelling polyelectrolyte hydrogel with submillimeter lateral confinement for osmotic energy conversion. Nano-Micro Lett. 17(1), 81 (2024). https://doi.org/10.1007/s40820-024-01577-010.1007/s40820-024-01577-0 ↗
10. H. Guo, T. Nakajima, D. Hourdet, A. Marcellan, C. Creton et al., Hydrophobic hydrogels: hydrophobic hydrogels with fruit-like structure and functions. Adv. Mater. 31(25), 1970177 (2019). https://doi.org/10.1002/adma.20197017710.1002/adma.201970177 ↗
11. D.J.G.P. van Osch, L.F. Zubeir, A. van den Bruinhorst, M.A.A. Rocha, M.C. Kroon, Hydrophobic deep eutectic solvents as water-immiscible extractants. Green Chem. 17(9), 4518–4521 (2015). https://doi.org/10.1039/c5gc01451d10.1039/c5gc01451d ↗
12. M. Cherniakova, V. Varchenko, K. Belikov, Menthol-based (deep) eutectic solvents: a review on properties and application in extraction. Chem. Rec. 24(2), e202300267 (2024). https://doi.org/10.1002/tcr.20230026710.1002/tcr.202300267 ↗
13. W. Deng, L. Yu, X. Li, J. Chen, X. Wang et al., Hexafluoroisopropanol-based hydrophobic deep eutectic solvents for dispersive liquid-liquid microextraction of pyrethroids in tea beverages and fruit juices. Food Chem. (2019). https://doi.org/10.1016/j.foodchem.2018.09.04810.1016/j.foodchem.2018.09.048 ↗
14. Y. Peng, K. Du, H. Yue, H. Li, H. Li et al., Integrated deep eutectic system enrichment and AI-assisted high-throughput visual detection for Hg2+ in environmental samples. J. Adv. Res. 79, 801–817 (2026). https://doi.org/10.1016/j.jare.2025.04.01110.1016/j.jare.2025.04.011 ↗
15. P. Villarim, E. Genty, J. Zemmouri, S. Fourmentin, Deep eutectic solvents and conventional solvents as VOC absorbents for biogas upgrading: a comparative study. Chem. Eng. J. 446, 136875 (2022). https://doi.org/10.1016/j.cej.2022.13687510.1016/j.cej.2022.136875 ↗
16. T. Luo, J. Qi, J. Yu, C. Wang, F. Chu et al., Lignin-based macromolecular photoinitiator for non-migration, self-adhesive, and water-resistant eutectogels toward underwater reliable communication. Adv. Funct. Mater. 35(5), 2414481 (2025). https://doi.org/10.1002/adfm.20241448110.1002/adfm.202414481 ↗
17. J. Cao, E. Su, Hydrophobic deep eutectic solvents: the new generation of green solvents for diversified and colorful applications in green chemistry. J. Clean. Prod. 314, 127965 (2021). https://doi.org/10.1016/j.jclepro.2021.12796510.1016/j.jclepro.2021.127965 ↗
18. G. Yusakul, J. Jomrit, R.G. Bacabac, A. Prasopthum, 3D printed personalized wound dressings using a hydrophobic deep eutectic solvent (HDES)-formulated emulgel. RSC Adv. 14(46), 34175–34191 (2024). https://doi.org/10.1039/d4ra05456c10.1039/d4ra05456c ↗
19. D. Du, J. Zhou, T. Kaneko, W. Dong, M. Chen et al., Stretchable and hydrophobic eutectogel for underwater human health monitoring based on hierarchical dynamic interactions. Chem. Eng. J. 474, 145704 (2023). https://doi.org/10.1016/j.cej.2023.14570410.1016/j.cej.2023.145704 ↗
20. Y. Tian, F. Jiang, H. Xie, Z. Chi, C. Liu, Conductive hyaluronic acid/deep eutectic solvent composite hydrogel as a wound dressing for promoting skin burn healing under electrical stimulation. Adv. Healthc. Mater. 13(17), 2304117 (2024). https://doi.org/10.1002/adhm.20230411710.1002/adhm.202304117 ↗
21. P. Yao, Q. Bao, Y. Yao, M. Xiao, Z. Xu et al., Environmentally stable, robust, adhesive, and conductive supramolecular deep eutectic gels as ultrasensitive flexible temperature sensor. Adv. Mater. 35(21), 2300114 (2023). https://doi.org/10.1002/adma.20230011410.1002/adma.202300114 ↗
22. Y. Shi, M. Wu, S. Ge, J. Li, A.S. Alshammari et al., Advanced functional electromagnetic shielding materials: a review based on micro-nano structure interface control of biomass cell walls. Nano-Micro Lett. 17(1), 3 (2024). https://doi.org/10.1007/s40820-024-01494-210.1007/s40820-024-01494-2 ↗
23. F. Lu, Y. Wang, D. Sun, Y. Fu, F. Zhang et al., Research progress on the preparation of lignin micro/nano-particles and their biomedical applications. Green Chem. 27(19), 5400–5422 (2025). https://doi.org/10.1039/d5gc00178a10.1039/d5gc00178a ↗
24. M. Madadi, E. Kargaran, S.S. Hashemi, C. Sun, J.F.M. Denayer et al., Scalable lignin monomer production via machine learning-guided reductive catalytic fractionation of lignocellulose. Adv. Sci. 12(42), e10496 (2025). https://doi.org/10.1002/advs.20251049610.1002/advs.202510496 ↗
25. H. Zhang, C. Hao, T. Fu, D. Yu, J. Howe et al., Gradient-layered MXene/hollow lignin nanospheres architecture design for flexible and stretchable supercapacitors. Nano-Micro Lett. 17(1), 43 (2024). https://doi.org/10.1007/s40820-024-01512-310.1007/s40820-024-01512-3 ↗
26. W. Yang, E. Fortunati, F. Bertoglio, J.S. Owczarek, G. Bruni et al., Polyvinyl alcohol/chitosan hydrogels with enhanced antioxidant and antibacterial properties induced by lignin nanoparticles. Carbohydr. Polym. 181, 275–284 (2018). https://doi.org/10.1016/j.carbpol.2017.10.08410.1016/j.carbpol.2017.10.084 ↗
27. W. Li, F. Wang, J. Liu, J. Wang, L. Deng, Super-adhesive and highly sensitive conductive hydrogel based on halometallate ionic liquid for flexible electronic devices. Chem. Eng. J. 519, 165699 (2025). https://doi.org/10.1016/j.cej.2025.16569910.1016/j.cej.2025.165699 ↗
28. H. Cui, W. Jiang, C. Wang, X. Ji, Y. Liu et al., Lignin nanofiller-reinforced composites hydrogels with long-lasting adhesiveness, toughness, excellent self-healing, conducting, ultraviolet-blocking and antibacterial properties. Compos. Part B Eng. 225, 109316 (2021). https://doi.org/10.1016/j.compositesb.2021.10931610.1016/j.compositesb.2021.109316 ↗
29. F. Wang, C. Chen, D. Zhu, W. Li, J. Liu et al., Ultrastretchable and highly conductive hydrogels based on Fe3+- lignin nanoparticles for subzero wearable strain sensor. Int. J. Biol. Macromol. 253(Pt 2), 126768 (2023). https://doi.org/10.1016/j.ijbiomac.2023.12676810.1016/j.ijbiomac.2023.126768 ↗
30. X. Gao, Y. Wang, J. Wu, Z. Xue, C. Yan et al., Lignin-ethylene glycol improved hydrogel with antifreezing and antiswelling properties as a flexible sensor for underwater motion monitoring. ACS Sustain. Chem. Eng. 12(41), 15159–15172 (2024). https://doi.org/10.1021/acssuschemeng.4c0536310.1021/acssuschemeng.4c05363 ↗
31. K. Haraźna, K. Walas, P. Urbańska, T. Witko, W. Snoch et al., Polyhydroxyalkanoate-derived hydrogen-bond donors for the synthesis of new deep eutectic solvents. Green Chem. 21(11), 3116–3126 (2019). https://doi.org/10.1039/c9gc00387h10.1039/c9gc00387h ↗
32. Y. Zhan, J. Poisson, X. Meng, Z. Wang, L. Chen et al., Electrospun lignin/ZnO nanofibrous membranes for self-powered ultrasensitive flexible airflow sensor and wearable device. Adv. Mater. 37(37), 2502211 (2025). https://doi.org/10.1002/adma.20250221110.1002/adma.202502211 ↗
33. K.S. Babu, A.R. Reddy, C. Sujatha, K.V. Reddy, A.N. Mallika, Synthesis and optical characterization of porous ZnO. J. Adv. Ceram. 2(3), 260–265 (2013). https://doi.org/10.1007/s40145-013-0069-610.1007/s40145-013-0069-6 ↗
34. S.R. Kadam, V.R. Mate, R.P. Panmand, L.K. Nikam, M.V. Kulkarni et al., A green process for efficient lignin (biomass) degradation and hydrogen production via water splitting using nanostructured C, N, S-doped ZnO under solar light. RSC Adv. 4(105), 60626–60635 (2014). https://doi.org/10.1039/c4ra10760h10.1039/c4ra10760h ↗
35. H. Namduri, S. Nasrazadani, Quantitative analysis of iron oxides using Fourier transform infrared spectrophotometry. Corros. Sci. 50(9), 2493–2497 (2008). https://doi.org/10.1016/j.corsci.2008.06.03410.1016/j.corsci.2008.06.034 ↗
36. S. He, B. Guo, X. Sun, M. Shi, H. Zhang et al., Bio-inspired instant underwater adhesive hydrogel sensors. ACS Appl. Mater. Interfaces 14(40), 45869–45879 (2022). https://doi.org/10.1021/acsami.2c1337110.1021/acsami.2c13371 ↗
37. X. Zhang, D. Li, X. Yang, L. Wang, G. Li et al., Hydro-locking in hydrogel for extreme temperature tolerance. Science 387(6737), 967–973 (2025). https://doi.org/10.1126/science.adq271110.1126/science.adq2711 ↗
38. F. Guo, Z. Ren, S. Wang, Y. Xie, J. Pan et al., Recent progress of electrospun nanofiber-based composite materials for monitoring physical, physiological, and body fluid signals. Nano-Micro Lett. 17(1), 302 (2025). https://doi.org/10.1007/s40820-025-01804-210.1007/s40820-025-01804-2 ↗
39. Y. Liu, X. Wang, J. Wang, Z. Li, K. Ao et al., Bioinspired structural design enables synergistic toughness and conductivity in hydrogels for advanced wearable electronics. Nano-Micro Lett. 18(1), 249 (2026). https://doi.org/10.1007/s40820-026-02094-y10.1007/s40820-026-02094-y ↗
40. J. Jiang, L. Zhao, Halometallate ionic liquid dynamically regulates zwitterionic hydrogels by synergistic multiple-bond networks. Adv. Funct. Mater. 35(12), 2417688 (2025). https://doi.org/10.1002/adfm.20241768810.1002/adfm.202417688 ↗
41. J. Zhang, C. Lin, L. Zeng, H. Lin, L. He et al., A hydrogel electrolyte with high adaptability over a wide temperature range and mechanical stress for long-life flexible zinc-ion batteries. Small 20(30), 2312116 (2024). https://doi.org/10.1002/smll.20231211610.1002/smll.202312116 ↗
42. C. Ma, J. Zhang, Y. Yin, C. Suo, S. Liu, Free radical theory in lignin oxidation depolymerization. Trends Chem. 6(5), 234–247 (2024). https://doi.org/10.1016/j.trechm.2024.03.00610.1016/j.trechm.2024.03.006 ↗
43. X. Wu, M. Li, H. Li, H. Gao, Z. Wang, Autonomous underwater self-healable adhesive elastomers enabled by dynamical hydrophobic phase-separated microdomains. Small 20(35), 2311131 (2024). https://doi.org/10.1002/smll.20231113110.1002/smll.202311131 ↗
44. R. Zhu, Y. Zheng, Q. Zhang, C. Yu, Z. Zhang et al., Statistical copolymerization-induced self-assembly (stat-PISA) for colloidal hydrogels. Adv. Funct. Mater. 34(23), 2313155 (2024). https://doi.org/10.1002/adfm.20231315510.1002/adfm.202313155 ↗
45. X. Zhang, S. Liu, X. Wang, J. Peng, W. Yang et al., Hydrophobic deep eutectic solvent-based eutectogels for underwater sensing. J. Colloid Interface Sci. 654, 1348–1355 (2024). https://doi.org/10.1016/j.jcis.2023.10.14210.1016/j.jcis.2023.10.142 ↗
46. G. Zhao, A. Zhang, X. Chen, G. Xiang, T. Jiang et al., Barnacle inspired strategy combined with solvent exchange for enhancing wet adhesion of hydrogels to promote seawater-immersed wound healing. Bioact. Mater. 41, 46–60 (2024). https://doi.org/10.1016/j.bioactmat.2024.07.01110.1016/j.bioactmat.2024.07.011 ↗
47. Z. Yuan, T. Wang, C. Shao, S. Yang, W. Sun et al., Bioinspired green underwater adhesive gelatin-tannic acid hydrogel with wide range adjustable adhesion strength and multiple environmental adaptability. Adv. Funct. Mater. 35(2), 2412950 (2025). https://doi.org/10.1002/adfm.20241295010.1002/adfm.202412950 ↗
48. Q. Li, S. Zheng, Z. Liu, W. Li, X. Wang et al., Strong, spontaneous, and self-healing poly(ionic liquid) elastomer underwater adhesive with borate ester dynamic crosslinking. Adv. Mater. 36(50), 2413901 (2024). https://doi.org/10.1002/adma.20241390110.1002/adma.202413901 ↗
49. M. Ahmadi, K. Ehrmann, T. Koch, R. Liska, J. Stampfl, From unregulated networks to designed microstructures: introducing heterogeneity at different length scales in photopolymers for additive manufacturing. Chem. Rev. 124(7), 3978–4020 (2024). https://doi.org/10.1021/acs.chemrev.3c0057010.1021/acs.chemrev.3c00570 ↗
50. Z. Wang, H. Wei, Y. Huang, Y. Wei, J. Chen, Naturally sourced hydrogels: emerging fundamental materials for next-generation healthcare sensing. Chem. Soc. Rev. 52(9), 2992–3034 (2023). https://doi.org/10.1039/d2cs00813k10.1039/d2cs00813k ↗
51. L. Song, Z. Wang, S. Chen, Y. Shen, J. Yin et al., Phytic acid-induced gradient hydrogels for highly sensitive and broad range pressure sensing. Adv. Mater. 37(9), 2417978 (2025). https://doi.org/10.1002/adma.20241797810.1002/adma.202417978 ↗
52. Y. Dai, S. Wai, P. Li, N. Shan, Z. Cao et al., Soft hydrogel semiconductors with augmented biointeractive functions. Science 386(6720), 431–439 (2024). https://doi.org/10.1126/science.adp931410.1126/science.adp9314 ↗
53. S. Han, Y. Hu, J. Wei, S. Li, P. Yang et al., A semi-interpenetrating poly(ionic liquid) network-driven low hysteresis and transparent hydrogel as a self-powered multifunctional sensor. Adv. Funct. Mater. 34(32), 2401607 (2024). https://doi.org/10.1002/adfm.20240160710.1002/adfm.202401607 ↗
54. J. Zhang, Y. Hu, L. Zhang, J. Zhou, A. Lu, Transparent, ultra-stretching, tough, adhesive carboxyethyl chitin/polyacrylamide hydrogel toward high-performance soft electronics. Nano-Micro Lett. 15(1), 8 (2022). https://doi.org/10.1007/s40820-022-00980-910.1007/s40820-022-00980-9 ↗
55. G. Gao, K. Yin, J. Han, Y. Hu, J. Gu et al., Marine amoebae-inspired salting hydrogels to reconfigure anisotropy for reprogrammable shape morphing. Angew. Chem. Int. Ed. 64(3), e202416672 (2025). https://doi.org/10.1002/anie.20241667210.1002/anie.202416672 ↗
56. Z. Hu, T. Li, Y. Zheng, S. Chen, T. Wan et al., Li/Al-LDH reinforced polyacrylamide/xanthan gum semi-interpenetrating network nano-conductive hydrogels for stress sensing and wearable device applications. Adv. Sci. 12(47), e11903 (2025). https://doi.org/10.1002/advs.20251190310.1002/advs.202511903 ↗
57. Y. Zhang, X. Jing, J. Zou, P. Feng, G. Wang et al., Mechanically robust and anti-swelling anisotropic conductive hydrogel with fluorescence for multifunctional sensing. Adv. Funct. Mater. 34(52), 2410698 (2024). https://doi.org/10.1002/adfm.20241069810.1002/adfm.202410698 ↗
58. R.-A. Li, H. Zhang, L. Li, B. Zhang, X. Du et al., Hydrophobic, ionically conductive, self-adhesive and fully recyclable eutectogels for stretchable wearable sensors and triboelectric nanogenerators. J. Mater. Chem. A 13(18), 12988–12997 (2025). https://doi.org/10.1039/d5ta01250c10.1039/d5ta01250c ↗
59. X. Zou, X. Wang, S. Sun, Z. Bai, Z. Zhou et al., Shape-adaptive underwater adhesive based on supramolecular assembly for robustly integrated underwater wireless sensing/communication and bioelectronic adhesion. Nano Today 56, 102282 (2024). https://doi.org/10.1016/j.nantod.2024.10228210.1016/j.nantod.2024.102282 ↗
60. Z. Zhang, A. Yao, P. Raffa, Physically crosslinked amphiphilic eutectogels with underwater self-healing, strong adhesion, environmental stability and closed-loop recyclability for underwater sensing and information transmission. Chem. Eng. J. 522, 167958 (2025). https://doi.org/10.1016/j.cej.2025.16795810.1016/j.cej.2025.167958 ↗
61. Z. Zhang, A. Yao, P. Raffa, Transparent, highly stretchable, self-healing, adhesive, freezing-tolerant, and swelling-resistant multifunctional hydrogels for underwater motion detection and information transmission. Adv. Funct. Mater. 34(49), 2407529 (2024). https://doi.org/10.1002/adfm.20240752910.1002/adfm.202407529 ↗
62. Q. Cao, W. Yuan, Photochromic hydrophobic eutectogel with high adhesion, stability, and self-healing for information encryption, underwater wireless communications, and motion monitoring. Small 21(42), e04948 (2025). https://doi.org/10.1002/smll.20250494810.1002/smll.202504948 ↗
63. G. Chen, B. Zhang, B. Tan, W. Yuan, Electric eel-inspired elastomer-encapsulated hydrogel sensor with superior anti-swelling, self-adhesion, and electrical stability for diverse underwater applications. Small 21(34), 2503207 (2025). https://doi.org/10.1002/smll.20250320710.1002/smll.202503207 ↗
64. M. Qi, D. Zhang, Y. Guo, H. Zhang, J. Shao et al., A flexible wearable sensor based on anti-swelling conductive hydrogels for underwater motion posture visualization assisted by deep learning. J. Mater. Chem. A 12(27), 16839–16853 (2024). https://doi.org/10.1039/d4ta02979h10.1039/d4ta02979h ↗
65. Y. Yu, S. Wang, H. Yu, X. Liao, W. Feng, Anti-freezing conductive hydrogels with exceptional mechanical properties and stable sensing performance at–30 ℃. Mater. Horiz. 12(8), 2679–2688 (2025). https://doi.org/10.1039/d4mh01115e10.1039/d4mh01115e ↗