Triple-network-based conductive polymer hydrogel for soft and elastic bioelectronic interfaces
Yan Chen, Liangpeng Chen, Bowen Geng, Fan Chen, Yuan Yuan, Deling Li, Yi-Xuan Wang, Wang Jia, Wenping Hu
Triple-network-based conductive polymer hydrogel for soft and elastic bioelectronic interfaces
Conductive polymer hydrogels have greatly improved the compatibility of electronic devices with biological tissues for human–machine interfacing. Hydrogels that possess low Young's modulus, low interfacial impedance, and high tensile properties facilitate high-quality signal transmission across dynamic biointerfaces. Direct incorporation of elastomers with conductive polymers may result in undesirable mechanical and/or electrical performance. Here, a covalent cross-linking network and an entanglement-driven network with conductive poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) have been combined. The triple-network conductive hydrogel shows high stretchability (with fracture strain up to 900%), low impedance (down to 91.2 Ω·cm2), and reversible adhesion. Importantly, ultra-low modulus (down to 6.3 kPa) and strain-insensitive electrical/electrochemical performance were achieved, which provides a guarantee for low current stimulation. The material design will contribute to the progression of soft and conformal bioelectronic devices, and pave the way to future implantable electronics.
conductive polymer hydrogel / neurostimulation / PEDOT:PSS / triple interpenetrating network / ultrasoft bioelectronics
[1] |
Yuk H, Lu B, Zhao X. Hydrogel bioelectronics. Chem Soc Rev. 2019;48(6):1642-1667.
|
[2] |
Jeong JW, Shin G, Park SI, Yu KJ, Xu L, Rogers JA. Soft materials in neuroengineering for hard problems in neuroscience. Neuron. 2015;86(1):175-186.
|
[3] |
Jonsson A, Song Z, Nilsson D, et al. Therapy using implanted organic bioelectronics. Sci Adv. 2015;1(4):e1500039.
|
[4] |
Kim DH, Lu N, Ma R, et al. Epidermal electronics. Science. 2011;333(6044):838-843.
|
[5] |
Xin M, Yu T, Jiang Y, et al. Multi-vital on-skin optoelectronic biosensor for assessing regional tissue hemodynamics. SmartMat. 2023;4(3):e1157.
|
[6] |
Ding Q, Wang H, Zhou Z, et al. Stretchable, self-healable, and breathable biomimetic iontronics with superior humidity-sensing performance for wireless respiration monitoring. SmartMat. 2023;4(2):e1147.
|
[7] |
Zhang Z, Yu Y, Yu H, Feng Y, Feng W. Water-resistant conductive organogels with sensation and actuation functions for artificial neuro-sensory muscular systems. SmartMat. 2022;3(4):632-643.
|
[8] |
Yu X, Li C, Gao C, Zhang X, Zhang G, Zhang D. Incorporation of hydrogen-bonding units into polymeric semiconductors toward boosting charge mobility, intrinsic stretchability, and self-healing ability. SmartMat. 2021;2(3):347-366.
|
[9] |
Xu L, Gutbrod SR, Bonifas AP, et al. 3D multifunctional integumentary membranes for spatiotemporal cardiac measurements and stimulation across the entire epicardium. Nat Commun. 2014;5(1):3329.
|
[10] |
Song E, Li J, Won SM, Bai W, Rogers JA. Materials for flexible bioelectronic systems as chronic neural interfaces. Nat Mater. 2020;19(6):590-603.
|
[11] |
Lacour SP, Courtine G, Guck J. Materials and technologies for soft implantable neuroprostheses. Nat Rev Mater. 2016;1(10):16063.
|
[12] |
Liu Y, Pharr M, Salvatore GA. Lab-on-skin: a review of flexible and stretchable electronics for wearable health monitoring. ACS Nano. 2017;11(10):9614-9635.
|
[13] |
Rivnay J, Wang H, Fenno L, Deisseroth K, Malliaras GG. Next-generation probes, particles, and proteins for neural interfacing. Sci Adv. 2017;3(6):e1601649.
|
[14] |
Liu X, Liu J, Lin S, Zhao X. Hydrogel machines. Mater Today. 2020;36:102-124.
|
[15] |
Lei Z, Wang Q, Sun S, Zhu W, Wu P. A bioinspired mineral hydrogel as a self-healable, mechanically adaptable ionic skin for highly sensitive pressure sensing. Adv Mater. 2017;29(22):1700321.
|
[16] |
Lin Y, Wu Z, Li C, et al. Deformable, transparent, high-performance, room-temperature oxygen sensors based on ion-conductive, environment-tolerant, and green organohydrogels. EcoMat. 2022;4(6):e12220.
|
[17] |
Xue J, Zou Y, Deng Y, Li Z. Bioinspired sensor system for health care and human-machine interaction. EcoMat. 2022;4(5):e12209.
|
[18] |
Han SA, Naqi M, Kim S, Kim JH. All-day wearable health monitoring system. EcoMat. 2022;4(4):e12198.
|
[19] |
Gong Y, Zhang YZ, Fang S, Sun Y, Niu J, Lai WY. Wireless human–machine interface based on artificial bionic skin with damage reconfiguration and multisensing capabilities. ACS Appl Mater Interfaces. 2022;14(41):47300-47309.
|
[20] |
Gong Y, Zhang YZ, Fang S, et al. Artificial intelligent optoelectronic skin with anisotropic electrical and optical responses for multi-dimensional sensing. Appl Phys Rev. 2022;9(2):021403.
|
[21] |
Mawad D, Mansfield C, Lauto A, et al. A conducting polymer with enhanced electronic stability applied in cardiac models. Sci Adv. 2016;2(11):e1601007.
|
[22] |
Paulsen BD, Tybrandt K, Stavrinidou E, Rivnay J. Organic mixed ionic–electronic conductors. Nat Mater. 2020;19(1):13-26.
|
[23] |
Someya T, Bao Z, Malliaras GG. The rise of plastic bioelectronics. Nature. 2016;540(7633):379-385.
|
[24] |
Ouyang J. Application of intrinsically conducting polymers in flexible electronics. SmartMat. 2021;2(3):263-285.
|
[25] |
Wang J, Li Q, Li K, et al. Ultra-high electrical conductivity in filler-free polymeric hydrogels toward thermoelectrics and electromagnetic interference shielding. Adv Mater. 2022;34(12):2109904.
|
[26] |
Zhang S, Chen Y, Liu H, et al. Room-temperature-formed PEDOT:PSS hydrogels enable injectable, soft, and healable organic bioelectronics. Adv Mater. 2020;32(1):1904752.
|
[27] |
Venkatraman S, Hendricks J, King ZA, et al. In vitro and in vivo evaluation of PEDOT microelectrodes for neural stimulation and recording. IEEE Trans Neural Syst Rehabil Eng. 2011;19(3):307-316.
|
[28] |
Cheng T, Wang F, Zhang YZ, et al. 3D printable conductive polymer hydrogels with ultra-high conductivity and superior stretchability for free-standing elastic all-gel supercapacitors. Chem Eng J. 2022;450(3):138311.
|
[29] |
Cheng T, Li L, Chen YL, et al. Stretchable and self-healing interlocking all-in-one supercapacitors based on multiple cross-linked hydrogel electrolytes. Adv Mater Interfaces. 2022;9(29):2201137.
|
[30] |
Lu B, Yuk H, Lin S, et al. Pure PEDOT:PSS hydrogels. Nat Commun. 2019;10(1):1043.
|
[31] |
Zhu Z, Liu C, Jiang F, Xu J, Liu E. Effective treatment methods on PEDOT:PSS to enhance its thermoelectric performance. Synth Met. 2017;225:31-40.
|
[32] |
Khasim S, Pasha A, Roy AS, Parveen A, Badi N. Effect of secondary doping using sorbitol on structure and transport properties of PEDOT–PSS thin films. J Electron Mater. 2017;46(7):4439-4447.
|
[33] |
Nardes AM, Kemerink M, de Kok MM, Vinken E, Maturova K, Janssen RAJ. Conductivity, work function, and environmental stability of PEDOT:PSS thin films treated with sorbitol. Org Electron. 2008;9(5):727-734.
|
[34] |
Yamaguchi H, Aizawa K, Chonan Y, et al. Highly flexible and conductive glycerol-doped PEDOT:PSS films prepared under an electric field. J Electron Mater. 2018;47(6):3370-3375.
|
[35] |
Lee JH, Jeong YR, Lee G, et al. Highly conductive, stretchable, and transparent PEDOT:PSS electrodes fabricated with triblock copolymer additives and acid treatment. ACS Appl Mater Interfaces. 2018;10(33):28027-28035.
|
[36] |
Li G, Huang K, Deng J, et al. Highly conducting and stretchable double-network hydrogel for soft bioelectronics. Adv Mater. 2022;34(15):2200261.
|
[37] |
Gong JP. Why are double-network hydrogels so tough? Soft Matter. 2010;6(12):2583-2590.
|
[38] |
Gong JP, Katsuyama Y, Kurokawa T, Osada Y. Double-network hydrogels with extremely high mechanical strength. Adv Mater. 2003;15(14):1155-1158.
|
[39] |
Lee YY, Kang HY, Gwon SH, et al. A strain-insensitive stretchable electronic conductor: PEDOT:PSS/acrylamide organogels. Adv Mater. 2016;28(8):1636-1643.
|
[40] |
Dai T, Qing X, Zhou H, Shen C, Wang J, Lu Y. Mechanically strong conducting hydrogels with special double-network structure. Synth Met. 2010;160(7-8):791-796.
|
[41] |
Xu P, Wang S, Lin A, et al. Conductive and elastic bottlebrush elastomers for ultrasoft electronics. Nat Commun. 2023;14(1):623.
|
[42] |
Cisnal A, Ihmig FR, Fraile JC, Pérez-Turiel J, Muñoz-Martinez V. Application of a novel measurement setup for characterization of graphene microelectrodes and a comparative study of variables influencing charge injection limits of implantable microelectrodes. Sensors. 2019;19(12):2725.
|
[43] |
Cisnal A, Fraile JC, Pérez-Turiel J, Muñoz-Martinez V, Müller C, Ihmig FR. A measurement setup and automated calculation method to determine the charge injection capacity of implantable microelectrodes. Sensors. 2018;18(12):4152.
|
[44] |
Long TR, Elder RM, Bain ED, et al. Influence of molecular weight between crosslinks on the mechanical properties of polymers formed via ring-opening metathesis. Soft Matter. 2018;14(17):3344-3360.
|
[45] |
Marković G, Marinović-Cincović M, Samaržija-Jovanović S, Jovanović V, Budinski-Simendić J. Crosslinking of Polymers: Rubber Vulcanization. Reactive and Functional Polymers Volume Two: Modification Reactions, Compatibility and Blends. Springer; 2020.
|
[46] |
Chen K, Feng Y, Zhang Y, et al. Entanglement-driven adhesion, self-healing, and high stretchability of double-network PEG-based hydrogels. ACS Appl Mater Interfaces. 2019;11(40):36458-36468.
|
[47] |
Lin P, Ma S, Wang X, Zhou F. Molecularly engineered dual-crosslinked hydrogel with ultrahigh mechanical strength, toughness, and good self-recovery. Adv Mater. 2015;27(12):2054-2059.
|
[48] |
Pasha A, Khasim S. Highly conductive organic thin films of PEDOT-PSS: silver nanocomposite treated with PEG as a promising thermo-electric material. J Mater Sci: Mater Electron. 2020;31(12):9185-9195.
|
[49] |
Cheng W, Liu Y, Tong Z, et al. Micro-interfacial polymerization of porous PEDOT for printable electronic devices. EcoMat. 2023;5(2):e12288.
|
[50] |
Wang Y, Nian G, Kim J, Suo Z. Polyacrylamide hydrogels. VI. synthesis-property relation. J Mech Phys Solids. 2023;170:105099.
|
[51] |
Kim J, Zhang G, Shi M, Suo Z. Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links. Science. 2021;374(6564):212-216.
|
[52] |
Liu Y, Liu J, Chen S, et al. Soft and elastic hydrogel-based microelectronics for localized low-voltage neuromodulation. Nat Biomed Eng. 2019;3(1):58-68.
|
[53] |
Feig VR, Tran H, Lee M, Bao Z. Mechanically tunable conductive interpenetrating network hydrogels that mimic the elastic moduli of biological tissue. Nat Commun. 2018;9(1):2740.
|
[54] |
Lopez-Larrea N, Criado-Gonzalez M, Dominguez-Alfaro A, et al. Digital light 3D printing of PEDOT-based photopolymerizable inks for biosensing. ACS Appl Polym Mater. 2022;4(9):6749-6759.
|
[55] |
Wu Q, Wei J, Xu B, et al. A robust, highly stretchable supramolecular polymer conductive hydrogel with self-healability and thermo-processability. Sci Rep. 2017;7(1):41566.
|
[56] |
Javadi M, Gu Q, Naficy S, et al. Conductive tough hydrogel for bioapplications. Macromol Biosci. 2018;18(2):1700270.
|
[57] |
Wei H, Lei M, Zhang P, Leng J, Zheng Z, Yu Y. Orthogonal photochemistry-assisted printing of 3D tough and stretchable conductive hydrogels. Nat Commun. 2021;12(1):2082.
|
[58] |
Ding Y, Zheng Z. Stretchable ionics: how to measure the electrical resistance/impedance. Matter. 2022;5(9):2570-2573.
|
[59] |
Huang S, Liu Y, Zhao Y, Ren Z, Guo CF. Flexible electronics: stretchable electrodes and their future. Adv Funct Mater. 2019;29(6):1805924.
|
[60] |
Wang J, Gao D, Lee PS. Recent progress in artificial muscles for interactive soft robotics. Adv Mater. 2021;33(19):2003088.
|
[61] |
Yuk H, Zhang T, Parada GA, Liu X, Zhao X. Skin-inspired hydrogel-elastomer hybrids with robust interfaces and functional microstructures. Nat Commun. 2016;7(1):12028.
|
[62] |
Jiang Y, Trotsyuk AA, Niu S, et al. Wireless, closed-loop, smart bandage with integrated sensors and stimulators for advanced wound care and accelerated healing. Nat Biotechnol. 2023;41(5):652-662.
|
[63] |
Missirlis D, Spatz JP. Combined effects of PEG hydrogel elasticity and cell-adhesive coating on fibroblast adhesion and persistent migration. Biomacromolecules. 2014;15(1):195-205.
|
[64] |
Chen N, Zhang Z, Soontornworajit B, Zhou J, Wang Y. Cell adhesion on an artificial extracellular matrix using aptamer-functionalized PEG hydrogels. Biomaterials. 2012;33(5):1353-1362.
|
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