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Cation-Dipole Interaction-Induced Coacervate Underwater Adhesives in Natural Seawater

  • Research Article
  • Special Issue: Functional Polymer Materials
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Abstract

Significant progress has been made in wet adhesives for low salinity water, but exploration of general ionic adhesives for natural seawater is less developed because the high salinity could weaken interfacial bonding and shields electrostatic interactions, resulting in adhesion failure. Thus, the design of adhesives for natural seawater represents challenges less resolved. Herein, a cationic polyelectrolyte (PECHIA) containing imidazolacetonitrile unit was explored to prepare adhesives enabled by natural seawater. By combining the ion shielding effect with the “cation-dipole” interactions between PECHIA chains, aqueous solution of the PECHIA underwent coacervation and self-crosslinking in natural seawater, allowing for underwater adhesion to various substrates in seawater. The instantaneous lap-shear and tensile adhesion strengths are 47 and 119 kPa, respectively, while the cured adhesive shows ∼739 kPa tensile adhesion in natural seawater. The design of PECHIA enables wet adhesives viable for applications in the diversified scenarios of natural seawater.

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References

  1. Li, J.; Celiz, A. D.; Yang, J.; Yang, Q.; Wamala, I.; Whyte, W.; Seo, B. R.; Vasilyev, N. V.; Vlassak, J. J.; Suo, Z.; Mooney, D. J. Tough adhesives for diverse wet surfaces. Science 2017, 357, 378–381.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  2. Ma, C.; Sun, J.; Li, B.; Feng, Y.; Sun, Y.; Xiang, L.; Wu, B.; Xiao, L.; Liu, B.; Petrovskii, V. S.; Bin, L.; Zhang, J.; Wang, Z.; Li, H.; Zhang, L.; Li, J.; Wang, F.; Göstl, R.; Potemkin, II; Chen, D.; Zeng, H.; Zhang, H.; Liu, K.; Herrmann, A. Ulrra-strong bio-glue from genetically engineered polypeptides. Nat. Commun. 2021, 12, 3613.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  3. Cui, C.; Sun, Y.; Nie, X.; Yang, X.; Wang, F.; Liu, W. A coenzyme-based deep eutectic supramolecular polymer bioadhesive. Adv. Funct. Mater. 2023, 33, 2307543.

    Article  CAS  Google Scholar 

  4. Wang, Y. Q.; Dou, X. Y.; Wang, H. F.; Wang, X.; Wu, D. C. Dendrimer-based hydrogels with controlled drug delivery property for tissue adhesion. Chinese J. Polym. Sci. 2021, 39, 1421–1430.

    Article  CAS  Google Scholar 

  5. Balkenende, D. W. R.; Winkler, S. M.; Messersmith, P. B. Marine-inspired polymers in medical adhesion. Eur. Polym. J. 2019, 116, 134–143.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  6. Yau, Y.; Zeighami, Y.; Baker, T. E.; Larcher, K.; Vainik, U.; Dadar, M.; Fonov, V. S.; Hagmann, P.; Griffa, A.; Misic, B.; Collins, D. L.; Dagher, A. Network connectivity determines cortical thinning in early Parkinson’s disease progression. Nat. Commun. 2018, 9, 12.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  7. Wan, X.; Gu, Z.; Zhang, F.; Hao, D.; Liu, X.; Dai, B.; Song, Y.; Wang, S. Asymmetric Janus adhesive tape prepared by interfacial hydrosilylation for wet/dry amphibious adhesion. NPG Asia Mater. 2019, 11, 49.

    Article  CAS  Google Scholar 

  8. Han, Q.; Zhang, C.; Guo, T.; Tian, Y.; Song, W.; Lei, J.; Li, Q.; Wang, A.; Zhang, M.; Bai, S.; Yan, X. Hydrogel nanoarchitectonics of a flexible and self-adhesive electrode for long-term wireless electroencephalogram recording and high-accuracy sustained attention evaluation. Adv. Mater. 2023, 35, e2209606.

    Article  PubMed  Google Scholar 

  9. Yu, Z.; Wu, P. Underwater communication and optical camouflage ionogels. Adv. Mater. 2021, 33, 2008479.

    Article  CAS  Google Scholar 

  10. Baik, S.; Hwang, G. W.; Jang, S.; Jeong, S.; Kim, K. H.; Yang, T. H.; Pang, C. Bioinspired microsphere-embedded adhesive architectures for an electrothermally actuating transport device of dry/wet pliable surfaces. ACS Appl. Mater. Interfaces 2021, 13, 6930–6940.

    Article  CAS  PubMed  Google Scholar 

  11. Jeong, D.; Kwon, D. S.; Kim, H. J.; Shim, J. Striking a balance: Exploring optimal functionalities and composition of highly adhesive and dispersing binders for high-nickel cathodes in lithium-ion batteries. Adv. Energy Mater. 2023, 13, 2302845.

    Article  CAS  Google Scholar 

  12. Wang, L.; Ma, Z.; Zhang, Y.; Chen, L.; Cao, D.; Gu, J. Polymer-based EMI shielding composites with 3D conductive networks: a mini-review. SusMat 2021, 1, 413–431.

    Article  CAS  Google Scholar 

  13. Liu, Y.; Guan, G.; Li, Y.; Tan, J.; Cheng, P.; Yang, M.; Li, B.; Wang, Q.; Zhong, W.; Mequanint, K.; Zhu, C.; Xing, M. Gelation of highly entangled hydrophobic macromolecular fluid for ultrastrong underwater in situ fast tissue adhesion. Sci. Adv. 2022, 8, eabm9744.

    Google Scholar 

  14. Cai, C.; Chen, Z.; Chen, Y.; Li, H.; Yang, Z.; Liu, H. Mechanisms and applications of bioinspired underwater/wet adhesives. J. Polym. Sci. 2021, 59, 2911–2945.

    Article  CAS  Google Scholar 

  15. Gao, L.; Ma, S.; Bao, L.; Zhao, X.; Xiang, Y.; Zhang, Z.; Ma, Y.; Ma, Z.; Liang, Y. M.; Zhou, F. Molecular engineering super-robust dry/wet adhesive with strong interface bonding and excellent mechanical tolerance. ACS Appl. Mater. Interfaces 2022, 14, 12684–12692.

    Article  CAS  PubMed  Google Scholar 

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

    Article  CAS  Google Scholar 

  17. Liu, H.; Qin, S.; Liu, J.; Zhou, C.; Zhu, Y.; Yuan, Y.; Fu, D. a.; Lv, Q.; Song, Y.; Zou, M.; Wang, Z.; Wang, L. Bio-inspired self-hydrophobized sericin adhesive with tough underwater adhesion enables wound healing and fluid leakage sealing. Adv. Funct. Mater. 2022, 32, 2201108.

    Article  CAS  Google Scholar 

  18. Fan, H.; Gong, J. P. Bioinspired underwater adhesives. Adv. Mater. 2021, 33, 2102983.

    Article  CAS  Google Scholar 

  19. Frey, S. T.; Haque, A.; Tutika, R.; Krotz, E. V.; Lee, C.; Haverkamp, C. B.; Markvicka, E. J.; Bartlett, M. D. Octopus-inspired adhesive skins for intelligent and rapidly switchable underwater adhesion. Sci. Adv. 2022, 8, eabq1905.

    Article  PubMed  PubMed Central  Google Scholar 

  20. Cui, C.; Fan, C.; Wu, Y.; Xiao, M.; Wu, T.; Zhang, D.; Chen, X.; Liu, B.; Xu, Z.; Qu, B.; Liu, W. Water-triggered hyperbranched polymer universal adhesives: from strong underwater adhesion to rapid sealing hemostasis. Adv. Mater. 2019, 31, 1905761.

    Article  CAS  Google Scholar 

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

    Article  CAS  PubMed  Google Scholar 

  22. Zhang, W.; Wang, R.; Sun, Z.; Zhu, X.; Zhao, Q.; Zhang, T.; Cholewinski, A.; Yang, F. K.; Zhao, B.; Pinnaratip, R.; Forooshani, P. K.; Lee, B. P. Catechol-functionalized hydrogels: biomimetic design, adhesion mechanism, and biomedical applications. Chem. Soc. Rev. 2020, 49, 433–464.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  23. Chen, M. X.; Dai, J. Y.; Zhang, L. Y.; Wang, S. P.; Liu, J. K.; Wu, Y. G.; Ba, X. W.; Liu, X. Q. The role of renewable protocatechol acid in epoxy coating modification: significantly improved antibacterial and adhesive properties. Chinese J. Polym. Sci. 2023, 42, 63–72.

    Article  Google Scholar 

  24. Wei, Y.; Mei, Y.; Wu, M.; Chen, S.; Liu, L. Electrically detaching behavior and mechanism of ionic conductive adhesives. Chinese J. Polym. Sci. 2023, 41, 1142–1154.

    Article  CAS  Google Scholar 

  25. Yang, Y.; Ru, Y.; Zhao, T.; Liu, M. Bioinspired multiphase composite gel materials: from controlled micro-phase separation to multiple functionalities. Chem 2023, 9, 3113–3137.

    Article  CAS  Google Scholar 

  26. Yan, C. C.; Li, W.; Liu, Z.; Zheng, S.; Hu, Y.; Zhou, Y.; Guo, J.; Ou, X.; Li, Q.; Yu, J.; Li, L.; Yang, M.; Liu, Q.; Yan, F. Ionogels: preparation, properties and applications. Adv. Funct. Mater. 2023, 33, 2314408.

    Google Scholar 

  27. Narayanan, A.; Menefee, J. R.; Liu, Q.; Dhinojwala, A.; Joy, A. Lower critical solution temperature-driven self-coacervation of nonionic polyester underwater adhesives. ACS Nano 2020, 14, 8359–8367.

    Article  CAS  PubMed  Google Scholar 

  28. Chen, S.; Guo, Q.; Yu, J. Bio-inspired functional coacervates. Aggregate 2022, 3, 293.

    Article  Google Scholar 

  29. Xing, R.; Yuan, C.; Fan, W.; Ren, X.; Yan, X. Biomolecular glass with amino acid and peptide nanoarchitectonics. Sci. Adv. 2023, 9, eadd8105.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  30. Yuan, C.; Xing, R.; Cui, J.; Fan, W.; Li, J.; Yan, X. Multittep desolvation as a fundamental principle governing peptide self-assembly through liquid-liquid phase separation. CCS Chem. 2024, 6, 255–265.

    Article  CAS  Google Scholar 

  31. White, J. D.; Wilker, J. J. Underwater bonding with charged polymer mimics of marine mussel adhesive proteins. Macromolecules 2011, 44, 5085–5088.

    Article  CAS  Google Scholar 

  32. Baer, A.; Horbelt, N.; Nijemeisland, M.; Garcia, S. J.; Fratzl, P.; Schmidt, S.; Mayer, G.; Harrington, M. J. Shear-induced beta-crystallite unfolding in condensed phase nanodroplets promotes fiber formation in a biological adhesive. ACS Nano 2019, 13, 4992–5001.

    Article  CAS  PubMed  Google Scholar 

  33. Dompe, M.; Cedano-Serrano, F. J.; Heckert, O.; van den Heuvel, N.; van der Gucht, J.; Tran, Y.; Hourdet, D.; Creton, C.; Kamperman, M. Thermoresponsive complex coacervate-based underwater adhesive. Adv. Mater. 2019, 31, 1808179.

    Article  Google Scholar 

  34. Chung, H.; Grubbs, R. H. Rapidly cross-linkable DOPA containing terpolymer adhesives and PEG-based cross-linkers for biomedical applications. Macromolecules 2012, 45, 9666–9673.

    Article  CAS  Google Scholar 

  35. Liu, X.; Shi, L.; Wan, X.; Dai, B.; Yang, M.; Gu, Z.; Shi, X.; Jiang, L.; Wang, S. A spider-silk-inspired wet adhesive with supercold tolerance. Adv. Mater. 2021, 33, 2007301.

    Article  CAS  Google Scholar 

  36. Zhu, H.; Xu, G.; He, Y.; Mao, H.; Kong, D.; Luo, K.; Tang, W.; Liu, R.; Gu, Z. A dual-bioinspired tissue adhesive based on peptide dendrimer with fast and strong wet adhesion. Adv. Healthc. Mater. 2022, 11, 2200874.

    Article  CAS  Google Scholar 

  37. Roman, J. K.; Wilker, J. J. Cooking chemistry transforms proteins into high-strength adhesives. J. Am. Chem. Soc. 2019, 141, 1359–1365.

    Article  CAS  PubMed  Google Scholar 

  38. Zhu, X.; Wei, C.; Chen, H.; Zhang, C.; Peng, H.; Wang, D.; Yuan, J.; Waite, J. H.; Zhao, Q. A cation-methylene-phenyl sequence encodes programmable poly(Ionic liquid) coacervation and robust underwater adhesion. Adv. Funct. Mater. 2021, 32, 2105464.

    Article  Google Scholar 

  39. Wei, C.; Zhu, X.; Peng, H.; Chen, J.; Zhang, F.; Zhao, Q. Facile preparation of lignin-based underwater adhesives with improved performances. ACS Sustainable Chem. Eng. 2019, 7, 4508–4514.

    Article  CAS  Google Scholar 

  40. Fan, H. Getting glued in the sea. Polym. J. 2023, 55, 653–664.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  41. Feng, H.; Zhang, J.; Yang, W.; Ma, Y.; Wang, R.; Ma, S.; Cai, M.; Yu, B.; Zhou, F. Transparent Janus hydrogel wet adhesive for underwater self-cleaning. ACS Appl. Mater. Interfaces 2021, 13, 50505–50515.

    Article  CAS  PubMed  Google Scholar 

  42. Kim, S.; Yoo, H. Y.; Huang, J.; Lee, Y.; Park, S.; Park, Y.; Jin, S.; Jung, Y. M.; Zeng, H.; Hwang, D. S.; Jho, Y. Salt triggers the simple coacervation of an underwater adhesive when cations meet aromatic n electrons in seawater. ACS Nano 2017, 11, 6764–6772.

    Article  CAS  PubMed  Google Scholar 

  43. Zhang, C.; Peng, H.; Waite, J. H.; Zhao, Q. Coacervate phase evolution and membrane formation in natural seawater. J. Am. Chem. Soc. 2024, 146, 2219–2226.

    Article  CAS  PubMed  Google Scholar 

  44. Huang, K. Y.; Yoo, H. Y.; Jho, Y.; Han, S.; Hwang, D. S. Bicontinuous fluid structure with low cohesive energy: molecular basis for exceptionally low interfacial tension of complex coacervate fluids. ACS Nano 2016, 10, 5051–62.

    Article  CAS  PubMed  Google Scholar 

  45. Zhu, X.; Wei, C.; Zhang, F.; Tang, Q.; Zhao, Q. A robust salty water adhesive by counterion exchange induced coacervate. Macromol. Rapid Commun. 2019, 40, e1800758.

    Article  PubMed  Google Scholar 

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

    Article  CAS  Google Scholar 

  47. Li, X.; Deng, Y.; Lai, J.; Zhao, G.; Dong, S. Tough, long-term, water-resistant, and underwater adhesion of low-molecular-weight supramolecular adhesives. J. Am. Chem. Soc. 2020, 142, 5371–5379.

    Article  CAS  PubMed  Google Scholar 

  48. Zheng, S. Y.; Zhou, J.; Wang, S.; Wang, Y. J.; Liu, S.; Du, G.; Zhang, D.; Fu, J.; Lin, J.; Wu, Z. L.; Zheng, Q.; Yang, J. Water-triggered spontaneously solidified adhesive: from instant and strong underwater adhesion to in situ signal transmission. Adv. Funct. Mater. 2022, 32, 2205597.

    Article  CAS  Google Scholar 

  49. Rogers, A. D. Environmental change in the deep ocean. Annu. Rev. Environ. Resour. 2015, 40, 1–38.

    Article  Google Scholar 

  50. Lee, H.; Scherer, N. F.; Messersmith, P. B. Single-molecule mechanics of mussel adhesion. Proc. Natl. Acad. Sci. U. S. A. 2006, 103, 12999–3003.

    Article  CAS  PubMed  PubMed Central  Google Scholar 

  51. Fan, X.; Zhou, W.; Chen, Y.; Yan, L.; Fang, Y.; Liu, H. An antifreezing/antiheating hydrogel containing catechol derivative urushiol for strong wet adhesion to various substrates. ACS Appl. Mater. Interfaces 2020, 12, 32031–32040.

    Article  CAS  PubMed  Google Scholar 

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Acknowledgments

This work was financially supported by the National Key R&D Program of China (No. 2022YFB3805103) and the National Natural Science Foundation of China (No. 22178139).

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Authors and Affiliations

  1. Key Laboratory of Material Chemistry for Energy Conversion and Storage, Ministry of Education, School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan, 430074, China

    Xu-Fei Liu, Chong-Rui Zhang, Hua-Wen Peng & Qiang Zhao

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  1. Xu-Fei Liu
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  2. Chong-Rui Zhang
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Correspondence to Qiang Zhao.

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Liu, XF., Zhang, CR., Peng, HW. et al. Cation-Dipole Interaction-Induced Coacervate Underwater Adhesives in Natural Seawater. Chin J Polym Sci (2024). https://doi.org/10.1007/s10118-024-3141-5

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