Issue

Vol. 16 (2024)

A Generic Strategy to Create Mechanically Interlocked Nanocomposite/Hydrogel Hybrid Electrodes for Epidermal Electronics

https://doi.org/10.1007/s40820-023-01314-z
Qian Wang
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Yanyan Li
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Yong Lin
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Yuping Sun
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Chong Bai
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Haorun Guo
College of Chemical Engineering and Technology, Engineering Research Center of Seawater Utilization Technology of Ministry of Education, State Key Laboratory of Reliability and Intelligence of Electrical Equipment, Hebei University of Technology, Tianjin 300130, People’s Republic of China
Ting Fang
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Gaohua Hu
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Yanqing Lu
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China
Desheng Kong
College of Engineering and Applied Sciences, National Laboratory of Solid State Microstructure, and Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210023, People’s Republic of China

Corresponding Author: Desheng Kong

dskong@nju.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 87

Abstract

Stretchable electronics are crucial enablers for next-generation wearables intimately integrated into the human body. As the primary compliant conductors used in these devices, metallic nanostructure/elastomer composites often struggle to form conformal contact with the textured skin. Hybrid electrodes have been consequently developed based on conductive nanocomposite and soft hydrogels to establish seamless skin-device interfaces. However, chemical modifications are typically needed for reliable bonding, which can alter their original properties. To overcome this limitation, this study presents a facile fabrication approach for mechanically interlocked nanocomposite/hydrogel hybrid electrodes. In this physical process, soft microfoams are thermally laminated on silver nanowire nanocomposites as a porous interface, which forms an interpenetrating network with the hydrogel. The microfoam-enabled bonding strategy is generally compatible with various polymers. The resulting interlocked hybrids have a 28-fold improved interfacial toughness compared to directly stacked hybrids. These electrodes achieve firm attachment to the skin and low contact impedance using tissue-adhesive hydrogels. They have been successfully integrated into an epidermal sleeve to distinguish hand gestures by sensing muscle contractions. Interlocked nanocomposite/hydrogel hybrids reported here offer a promising platform to combine the benefits of both materials for epidermal devices and systems.


Highlights:
1 Nanocomposite/hydrogel hybrid electrodes are created with high interfacial toughness by introducing soft microfoams as the mechanically interlocking layer.
2 In the hybrid electrodes, silver nanowires and hydrogels are electrically connected through the porous microfoams, achieving high conductivity and low contact impedance for high-quality biopotential recordings.
3 The microfoam-enabled bonding strategy is generally applicable to diverse polymer substrates.

Keywords

Stretchable electronics Epidermal electronics Silver nanowire Conductive nanocomposites Hydrogel
Wang, Qian, Yanyan Li, Yong Lin, Yuping Sun, Chong Bai, Haorun Guo, Ting Fang, Gaohua Hu, Yanqing Lu, and Desheng Kong. 2024. “A Generic Strategy to Create Mechanically Interlocked Nanocomposite/Hydrogel Hybrid Electrodes for Epidermal Electronics”. Nano-Micro Letters 16 (January):87. https://doi.org/10.1007/s40820-023-01314-z.
Download Citation
Endnote/Zotero/Mendeley (RIS)
BibTeX
References
  1. J.A. Rogers, T. Someya, Y. Huang, Materials and mechanics for stretchable electronics. Science 327, 1603–1607 (2010). https://doi.org/10.1126/science.1182383
  2. S. Choi, H. Lee, R. Ghaffari, T. Hyeon, D.-H. Kim, Recent advances in flexible and stretchable bio-electronic devices integrated with nanomaterials. Adv. Mater. 28, 4203–4218 (2016). https://doi.org/10.1002/adma.201504150
  3. Z. Ma, D. Kong, L. Pan, Z. Bao, Skin-inspired electronics: emerging semiconductor devices and systems. J. Semicond. 41, 041601 (2020). https://doi.org/10.1088/1674-4926/41/4/041601
  4. D.-H. Kim, N. Lu, R. Ma, Y.-S. Kim, R.-H. Kim et al., Epidermal electronics. Science 333, 838–843 (2011). https://doi.org/10.1126/science.1206157
  5. J.C. Yang, J. Mun, S.Y. Kwon, S. Park, Z. Bao et al., Electronic skin: recent progress and future prospects for skin-attachable devices for health monitoring, robotics, and prosthetics. Adv. Mater. 31, e1904765 (2019). https://doi.org/10.1002/adma.201904765
  6. H.U. Chung, B.H. Kim, J.Y. Lee, J. Lee, Z. Xie et al., Binodal, wireless epidermal electronic systems with in-sensor analytics for neonatal intensive care. Science 363, eaau0780 (2019). https://doi.org/10.1126/science.aau0780
  7. G.H. Lee, H. Woo, C. Yoon, C. Yang, J.Y. Bae et al., A personalized electronic tattoo for healthcare realized by on-the-spot assembly of an intrinsically conductive and durable liquid-metal composite. Adv. Mater. 34, e2204159 (2022). https://doi.org/10.1002/adma.202204159
  8. S. Wang, Y. Nie, H. Zhu, Y. Xu, S. Cao et al., Intrinsically stretchable electronics with ultrahigh deformability to monitor dynamically moving organs. Sci. Adv. 8, eabl5511 (2022). https://doi.org/10.1126/sciadv.abl5511
  9. H. Lee, T.K. Choi, Y.B. Lee, H.R. Cho, R. Ghaffari et al., A graphene-based electrochemical device with thermoresponsive microneedles for diabetes monitoring and therapy. Nat. Nanotechnol. 11, 566–572 (2016). https://doi.org/10.1038/nnano.2016.38
  10. M. Wang, Z. Yan, T. Wang, P. Cai, S. Gao et al., Gesture recognition using a bioinspired learning architecture that integrates visual data with somatosensory data from stretchable sensors. Nat. Electron. 3, 563–570 (2020). https://doi.org/10.1038/s41928-020-0422-z
  11. H. Zhao, Y. Zhou, S. Cao, Y. Wang, J. Zhang et al., Ultrastretchable and washable conductive microtextiles by coassembly of silver nanowires and elastomeric microfibers for epidermal human–machine interfaces. ACS Mater. Lett. 3, 912–920 (2021). https://doi.org/10.1021/acsmaterialslett.1c00128
  12. A. Chortos, G.I. Koleilat, R. Pfattner, D. Kong, P. Lin et al., Mechanically durable and highly stretchable transistors employing carbon nanotube semiconductor and electrodes. Adv. Mater. 28, 4441–4448 (2016). https://doi.org/10.1002/adma.201501828
  13. J. Zhang, X. Liu, W. Xu, W. Luo, M. Li et al., Stretchable transparent electrode arrays for simultaneous electrical and optical interrogation of neural circuits in vivo. Nano Lett. 18, 2903–2911 (2018). https://doi.org/10.1021/acs.nanolett.8b00087
  14. N. Matsuhisa, D. Inoue, P. Zalar, H. Jin, Y. Matsuba et al., Printable elastic conductors by in situ formation of silver nanops from silver flakes. Nat. Mater. 16, 834–840 (2017). https://doi.org/10.1038/nmat4904
  15. Y. Kim, J. Zhu, B. Yeom, M. Di Prima, X. Su et al., Stretchable nanop conductors with self-organized conductive pathways. Nature 500, 59–63 (2013). https://doi.org/10.1038/nature12401
  16. F. Xu, Y. Zhu, Highly conductive and stretchable silver nanowire conductors. Adv. Mater. 24, 5117–5122 (2012). https://doi.org/10.1002/adma.201201886
  17. S. Choi, S.I. Han, D. Jung, H.J. Hwang, C. Lim et al., Highly conductive, stretchable and biocompatible Ag-Au core-sheath nanowire composite for wearable and implantable bioelectronics. Nat. Nanotechnol. 13, 1048–1056 (2018). https://doi.org/10.1038/s41565-018-0226-8
  18. J. Liang, L. Li, X. Niu, Z. Yu, Q. Pei, Elastomeric polymer light-emitting devices and displays. Nat. Photon. 7, 817–824 (2013). https://doi.org/10.1038/nphoton.2013.242
  19. D. Jung, C. Lim, H.J. Shim, Y. Kim, C. Park et al., Highly conductive and elastic nanomembrane for skin electronics. Science 373, 1022–1026 (2021). https://doi.org/10.1126/science.abh4357
  20. W. Guo, P. Zheng, X. Huang, H. Zhuo, Y. Wu et al., Matrix-independent highly conductive composites for electrodes and interconnects in stretchable electronics. ACS Appl. Mater. Interfaces 11, 8567–8575 (2019). https://doi.org/10.1021/acsami.8b21836
  21. C. Ding, J. Wang, W. Yuan, X. Zhou, Y. Lin et al., Durability study of thermal transfer printed textile electrodes for wearable electronic applications. ACS Appl. Mater. Interfaces 14, 29144–29155 (2022). https://doi.org/10.1021/acsami.2c03807
  22. W.H. Yeo, Y.S. Kim, J. Lee, A. Ameen, L. Shi et al., Multifunctional epidermal electronics printed directly onto the skin. Adv. Mater. 25, 2773–2778 (2013). https://doi.org/10.1002/adma.201204426
  23. S. Liu, Y. Rao, H. Jang, P. Tan, N. Lu, Strategies for body-conformable electronics. Matter 5, 1104–1136 (2022). https://doi.org/10.1016/j.matt.2022.02.006
  24. Q. Tian, H. Zhao, X. Wang, Y. Jiang, M. Zhu et al., Hairy-skin-adaptive viscoelastic dry electrodes for long-term electrophysiological monitoring. Adv. Mater. 35, e2211236 (2023). https://doi.org/10.1002/adma.202211236
  25. C. Lim, Y.J. Hong, J. Jung, Y. Shin, S.H. Sunwoo et al., Tissue-like skin-device interface for wearable bioelectronics by using ultrasoft, mass-permeable, and low-impedance hydrogels. Sci. Adv. 7, eabd3716 (2021). https://doi.org/10.1126/sciadv.abd3716
  26. H. Jin, N. Matsuhisa, S. Lee, M. Abbas, T. Yokota et al., Enhancing the performance of stretchable conductors for E-textiles by controlled ink permeation. Adv. Mater. 29, 1605848 (2017). https://doi.org/10.1002/adma.201605848
  27. K.-I. Jang, S.Y. Han, S. Xu, K.E. Mathewson, Y. Zhang et al., Rugged and breathable forms of stretchable electronics with adherent composite substrates for transcutaneous monitoring. Nat. Commun. 5, 4779 (2014). https://doi.org/10.1038/ncomms5779
  28. Y. Zhou, C. Zhao, J. Wang, Y. Li, C. Li et al., Stretchable high-permittivity nanocomposites for epidermal alternating-current electroluminescent displays. ACS Mater. Lett. 1, 511–518 (2019). https://doi.org/10.1021/acsmaterialslett.9b00376
  29. O. Wichterle, D. Lím, Hydrophilic gels for biological use. Nature 185, 117–118 (1960). https://doi.org/10.1038/185117a0
  30. P.C. Nicolson, J. Vogt, Soft contact lens polymers: an evolution. Biomaterials 22, 3273–3283 (2001). https://doi.org/10.1016/s0142-9612(01)00165-x
  31. Y. Liang, J. He, B. Guo, Functional hydrogels as wound dressing to enhance wound healing. ACS Nano 15, 12687–12722 (2021). https://doi.org/10.1021/acsnano.1c04206
  32. S.O. Blacklow, J. Li, B.R. Freedman, M. Zeidi, C. Chen et al., Bioinspired mechanically active adhesive dressings to accelerate wound closure. Sci. Adv. 5, eaaw3963 (2019). https://doi.org/10.1126/sciadv.aaw3963
  33. J. Li, A.D. Celiz, J. Yang, Q. Yang, I. Wamala et al., Tough adhesives for diverse wet surfaces. Science 357, 378–381 (2017). https://doi.org/10.1126/science.aah6362
  34. S.R. Caliari, J.A. Burdick, A practical guide to hydrogels for cell culture. Nat. Meth. 13, 405–414 (2016). https://doi.org/10.1038/nmeth.3839
  35. N. Peppas, J. Hilt, A. Khademhosseini, R. Langer, Hydrogels in biology and medicine: from molecular principles to bionanotechnology. Adv. Mater. 18, 1345–1360 (2006). https://doi.org/10.1002/adma.200501612
  36. J. Li, D.J. Mooney, Designing hydrogels for controlled drug delivery. Nat. Rev. Mater. 1, 16071 (2016). https://doi.org/10.1038/natrevmats.2016.71
  37. L. Hu, P.L. Chee, S. Sugiarto, Y. Yu, C. Shi et al., Hydrogel-based flexible electronics. Adv. Mater. 35, 2205326 (2023). https://doi.org/10.1002/adma.202205326
  38. H. Yuk, J. Wu, X. Zhao, Hydrogel interfaces for merging humans and machines. Nat. Rev. Mater. 7, 935–952 (2022). https://doi.org/10.1038/s41578-022-00483-4
  39. L. Han, L. Yan, K. Wang, L. Fang, H. Zhang et al., Tough, self-healable and tissue-adhesive hydrogel with tunable multifunctionality. NPG Asia Mater. 9, e372 (2017). https://doi.org/10.1038/am.2017.33
  40. C. Xie, X. Wang, H. He, Y. Ding, X. Lu, Mussel-inspired hydrogels for self-adhesive bioelectronics. Adv. Funct. Mater. 30, 1909954 (2020). https://doi.org/10.1002/adfm.201909954
  41. G. Tian, D. Yang, C. Liang, Y. Liu, J. Chen et al., A nonswelling hydrogel with regenerable high wet tissue adhesion for bioelectronics. Adv. Mater. 35, e2212302 (2023). https://doi.org/10.1002/adma.202212302
  42. J. Tang, J. Li, J.J. Vlassak, Z. Suo, Adhesion between highly stretchable materials. Soft Matter 12, 1093–1099 (2016). https://doi.org/10.1039/c5sm02305j
  43. Q. Liu, G. Nian, C. Yang, S. Qu, Z. Suo, Bonding dissimilar polymer networks in various manufacturing processes. Nat. Commun. 9, 846 (2018). https://doi.org/10.1038/s41467-018-03269-x
  44. J. Yang, R. Bai, B. Chen, Z. Suo, Hydrogel adhesion: a supramolecular synergy of chemistry, topology, and mechanics. Adv. Funct. Mater. 30, 1901693 (2020). https://doi.org/10.1002/adfm.201901693
  45. K. Tian, J. Bae, Z. Suo, J.J. Vlassak, Adhesion between hydrophobic elastomer and hydrogel through hydrophilic modification and interfacial segregation. ACS Appl. Mater. Interfaces 10, 43252–43261 (2018). https://doi.org/10.1021/acsami.8b16445
  46. H. Yuk, T. Zhang, G.A. Parada, X. Liu, X. Zhao, Skin-inspired hydrogel–elastomer hybrids with robust interfaces and functional microstructures. Nat. Commun. 7, 12028 (2016). https://doi.org/10.1038/ncomms12028
  47. S.H. Kim, S. Jung, I.S. Yoon, C. Lee, Y. Oh et al., Ultrastretchable conductor fabricated on skin-like hydrogel-elastomer hybrid substrates for skin electronics. Adv. Mater. 30, e1800109 (2018). https://doi.org/10.1002/adma.201800109
  48. D. Wirthl, R. Pichler, M. Drack, G. Kettlguber, R. Moser et al., Instant tough bonding of hydrogels for soft machines and electronics. Sci. Adv. 3, e1700053 (2017). https://doi.org/10.1126/sciadv.1700053
  49. M. Zhu, F. Zhang, X. Chen, Bioinspired mechanically interlocking structures. Small Struct. 1, 2000045 (2020). https://doi.org/10.1002/sstr.202000045
  50. C.W. Jennings, Surface roughness and bond strength of adhesives. J. Adhes. 4, 25–38 (1972). https://doi.org/10.1080/00218467208072208
  51. S. Pan, F. Zhang, P. Cai, M. Wang, K. He et al., Mechanically interlocked hydrogel–elastomer hybrids for on-skin electronics. Adv. Funct. Mater. 30, 1909540 (2020). https://doi.org/10.1002/adfm.201909540
  52. T. Kurokawa, H. Furukawa, W. Wang, Y. Tanaka, J.P. Gong, Formation of a strong hydrogel–porous solid interface via the double-network principle. Acta Biomater. 6, 1353–1359 (2010). https://doi.org/10.1016/j.actbio.2009.10.046
  53. Y. Lin, L. Wang, T. Ma, L. Ding, S. Cao et al., Highly conductive and compliant silver nanowire nanocomposites by direct spray deposition. ACS Appl. Mater. Interfaces 14, 57290–57298 (2022). https://doi.org/10.1021/acsami.2c18761
  54. T.B. Tierney, Å.C. Rasmuson, S.P. Hudson, Size and shape control of micron-sized salicylic acid crystals during antisolvent crystallization. Org. Process Res. Dev. 21, 1732–1740 (2017). https://doi.org/10.1021/acs.oprd.7b00181
  55. Y. Li, S. Wang, J. Zhang, X. Ma, S. Cao et al., A highly stretchable and permeable liquid metal micromesh conductor by physical deposition for epidermal electronics. ACS Appl. Mater. Interfaces 14, 13713–13721 (2022). https://doi.org/10.1021/acsami.1c25206
  56. C.-W. Tsao, D.L. DeVoe, Bonding of thermoplastic polymer microfluidics. Microfluid. Nanofluid. 6, 1–16 (2009). https://doi.org/10.1007/s10404-008-0361-x
  57. Y. Zhou, S. Cao, J. Wang, H. Zhu, J. Wang et al., Bright stretchable electroluminescent devices based on silver nanowire electrodes and high-k thermoplastic elastomers. ACS Appl. Mater. Interfaces 10, 44760–44767 (2018). https://doi.org/10.1021/acsami.8b17423
  58. L. Mou, J. Qi, L. Tang, R. Dong, Y. Xia et al., Highly stretchable and biocompatible liquid metal-elastomer conductors for self-healing electronics. Small 16, e2005336 (2020). https://doi.org/10.1002/smll.202005336
  59. S. Trasatti, O.A. Petrii, Real surface area measurements in electrochemistry. J. Electroanal. Chem. 327, 353–376 (1992). https://doi.org/10.1016/0022-0728(92)80162-w
  60. D. Kong, H. Wang, Z. Lu, Y. Cui, CoSe2 nanops grown on carbon fiber paper: an efficient and stable electrocatalyst for hydrogen evolution reaction. J. Am. Chem. Soc. 136, 4897–4900 (2014). https://doi.org/10.1021/ja501497n
  61. H. Jung, M.K. Kim, J.Y. Lee, S.W. Choi, J. Kim, Adhesive hydrogel patch with enhanced strength and adhesiveness to skin for transdermal drug delivery. Adv. Funct. Mater. 30, 2004407 (2020). https://doi.org/10.1002/adfm.202004407
  62. L. Wang, N. Lu, Conformability of a thin elastic membrane laminated on a soft substrate with slightly wavy surface. J. Appl. Mech. 83, 041007 (2016). https://doi.org/10.1115/1.4032466
  63. N. Isakadze, S.S. Martin, How useful is the smartwatch ECG? Trends Cardiovasc. Med. 30, 442–448 (2020). https://doi.org/10.1016/j.tcm.2019.10.010
  64. J.M. Kwon, Y. Cho, K.H. Jeon, S. Cho, K.H. Kim et al., A deep learning algorithm to detect anaemia with ECGs: a retrospective, multicentre study. Lancet Digit. Health 2, e358–e367 (2020). https://doi.org/10.1016/S2589-7500(20)30108-4
Read More
Author biographies are not available.
Statistic
Read Counter : 2622 Download : 1925

Most read articles by the same author(s)