Rapid advancements in flexible electronics technology propel soft tactile sensing devices toward high-level biointegration, even attaining tactile perception capabilities surpassing human skin. However, the inherent mechanical mismatch resulting from deficient biomimetic mechanical properties of sensing materials poses a challenge to the application of wearable tactile sensing devices in human-machine interaction. Inspired by the innate biphasic structure of human subcutaneous tissue, this study discloses a skin-compliant wearable iontronic triboelectric gel via phase separation induced by competitive hydrogen bonding. Solvent-nonsolvent interactions are used to construct competitive hydrogen bonding systems to trigger phase separation, and the resulting soft-hard alternating phase-locked structure confers the iontronic triboelectric gel with Young's modulus (6.8-281.9 kPa) and high tensile properties (880%) compatible with human skin. The abundance of reactive hydroxyl groups gives the gel excellent tribopositive and self-adhesive properties (peel strength > 70 N m−1). The self-powered tactile sensing skin based on this gel maintains favorable interface and mechanical stability with the working object, which greatly ensures the high fidelity and reliability of soft tactile sensing signals. This strategy, enabling skin-compliant design and broad dynamic tunability of the mechanical properties of sensing materials, presents a universal platform for broad applications from soft robots to wearable electronics.
H.C.Ates, P.Q.Nguyen, L.Gonzalez-Macia, E.Morales-Narváez, F.Güder et al., End-to-end design of wearable sensors. Nat. Rev. Mater. 7, 887-907 (2022).
11.
S.Chen, L.Sun, X.Zhou, Y.Guo, J.Song et al., Mechanically and biologically skin-like elastomers for bio-integrated electronics. Nat. Commun. 11, 1107 (2020).
12.
Z.Yan, D.Xu, Z.Lin, P.Wang, B.Cao et al., Highly stretchable van der Waals thin films for adaptable and breathable electronic membranes. Science375, 852-859 (2022).
13.
S.Wang, Y.Fang, H.He, L.Zhang, C.-A.Li et al., Wearable stretchable dry and self-adhesive strain sensors with conformal contact to skin for high-quality motion monitoring. Adv. Funct. Mater. 31, 2007495 (2021).
14.
Z.Li, P.Zhang, Y.Shao, Z.-H.Guo, X.Pu, Stretchable iontronics with robust interface bonding between dielectric and ion-conducting elastomers. Nano Res.16, 11862-11870 (2023).
15.
J.Min, J.Tu, C.Xu, H.Lukas, S.Shin et al., Skin-interfaced wearable sweat sensors for precision medicine. Chem. Rev.123, 5049-5138 (2023).
16.
D.Choi, Y.Lee, Z.-H.Lin, S.Cho, M.Kim et al., Recent advances in triboelectric nanogenerators: from technological progress to commercial applications. ACS Nano17, 11087-11219 (2023).
17.
H.L.Wang, Z.H.Guo, X.Pu, Z.L.Wang, Ultralight iontronic triboelectric mechanoreceptor with high specific outputs for epidermal electronics. Nano-Micro Lett. 14, 86 (2022).
M.Ilami, H.Bagheri, R.Ahmed, E.O.Skowronek, H.Marvi, Materials, actuators, and sensors for soft bioinspired robots. Adv. Mater. 33, e2003139 (2021).
20.
L.Li, J.Wang, K.Yang, Z.H.Guo, J.Zhang et al., A recyclable, adhesive and fast self-healable ionic conducting elastomer based on a poly-zwitterionic liquid for soft iontronics. J. Mater. Chem. A10, 24581-24589 (2022).
J.Chen, Y.Gao, L.Shi, W.Yu, Z.Sun et al., Phase-locked constructing dynamic supramolecular ionic conductive elastomers with superior toughness, autonomous self-healing and recyclability. Nat. Commun. 13, 4868 (2022).
25.
M.Zhang, R.Yu, X.Tao, Y.He, X.Li et al., Mechanically robust and highly conductive ionogels for soft ionotronics. Adv. Funct. Mater. 33, 2208083 (2023).
26.
B.Bao, Q.Zeng, K.Li, J.Wen, Y.Zhang et al., Rapid fabrication of physically robust hydrogels. Nat. Mater. 22, 1253-1260 (2023).
27.
J.Wang, Y.Zheng, T.Cui, T.Huang, H.Liu et al., Bioinspired ultra-robust ionogels constructed with soft-rigid confinement space for multimodal monitoring electronics. Adv. Funct. Mater. 34, 2312383 (2024).
28.
H.Xiang, X.Li, B.Wu, S.Sun, P.Wu, Highly damping and self-healable ionic elastomer from dynamic phase separation of sticky fluorinated polymers. Adv. Mater. 35, e2209581 (2023).
29.
M.Wang, P.Zhang, M.Shamsi, J.L.Thelen, W.Qian et al., Tough and stretchable ionogels by in situ phase separation. Nat. Mater. 21, 359-365 (2022).
30.
J.Wu, Z.Zhang, Z.Wu, D.Liu, X.Yang et al., Strong and ultra-tough supramolecular hydrogel enabled by strain-induced microphase separation. Adv. Funct. Mater. 33, 2210395 (2023).
31.
H.Wan, B.Wu, L.Hou, P.Wu, Amphibious polymer materials with high strength and superb toughness in various aquatic and atmospheric environments. Adv. Mater. 36, e2307290 (2024).
32.
A.N.Annaidh, K.Bruyère, M.Destrade, M.D.Gilchrist, M.Otténio, Characterization of the anisotropic mechanical properties of excised human skin. J. Mech. Behav. Biomed. Mater. 5, 139-148 (2012).
33.
A.Pissarenko, M.A.Meyers, The materials science of skin: analysis, characterization, and modeling. Prog. Mater. Sci.110, 100634 (2020).
34.
D.Zhao, B.Pang, Y.Zhu, W.Cheng, K.Cao et al., A stiffness-switchable, biomimetic smart material enabled by supramolecular reconfiguration. Adv. Mater. 34, e2107857 (2022).
35.
X.Liang, S.A.Boppart, Biomechanical properties of in vivo human skin from dynamic optical coherence elastography. IEEE Trans. Biomed. Eng.57, 953-959 (2010).
36.
G.Balakrishnan, J.Song, C.Mou, C.J.Bettinger, Recent progress in materials chemistry to advance flexible bioelectronics in medicine. Adv. Mater. 34, e2106787 (2022).
37.
X.Li, S.Xiang, D.Ling, S.Zhang, C.Li et al., Stretchable, self-healing, transparent macromolecular elastomeric gel and PAM/carrageenan hydrogel for self-powered touch sensors. Mater. Sci. Eng. B283, 115832 (2022).
38.
S.Li, G.Liu, H.Wen, G.Liu, H.Wang et al., A skin-like pressure- and vibration-sensitive tactile sensor based on polyacrylamide/silk fibroin elastomer. Adv. Funct. Mater. 32, 2111747 (2022).
39.
J.Jiang, Q.Guan, Y.Liu, X.Sun, Z.Wen, Abrasion and fracture self-healable triboelectric nanogenerator with ultrahigh stretchability and long-term durability. Adv. Funct. Mater. 31, 2105380 (2021).
40.
Y.Guo, S.Chen, L.Sun, L.Yang, L.Zhang et al., Degradable and fully recyclable dynamic thermoset elastomer for 3D-printed wearable electronics. Adv. Funct. Mater. 31, 2009799 (2021).
41.
Y.Hishikawa, E.Togawa, T.Kondo, Characterization of individual hydrogen bonds in crystalline regenerated cellulose using resolved polarized FTIR spectra. ACS Omega2, 1469-1476 (2017).
42.
S.Zhu, Y.Wu, Q.Chen, Z.Yu, C.Wang et al., Dissolution of cellulose with ionic liquids and its application: a mini-review. Green Chem. 8, 325-327 (2006).
43.
R.Guo, Q.Zhang, Y.Wu, H.Chen, Y.Liu et al., Extremely strong and tough biodegradable poly(urethane) elastomers with unprecedented crack tolerance via hierarchical hydrogen-bonding interactions. Adv. Mater. 35, e2212130 (2023).
Y.Lai, X.Kuang, P.Zhu, M.Huang, X.Dong et al., Colorless, transparent, robust, and fast scratch-self-healing elastomers via a phase-locked dynamic bonds design. Adv. Mater. 30, e1802556 (2018).
G.Ge, K.Mandal, R.Haghniaz, M.Li, X.Xiao et al., Deep eutectic solvents-based ionogels with ultrafast gelation and high adhesion in harsh environments. Adv. Funct. Mater. 33, 2207388 (2023).
48.
D.Zhao, Y.Zhu, W.Cheng, G.Xu, Q.Wang et al., A dynamic gel with reversible and tunable topological networks and performances. Matter2, 390-403 (2020).
49.
C.Zhang, Z.Wang, H.Zhu, Q.Zhang, S.Zhu, Dielectric gels with microphase separation for wide-range and self-damping pressure sensing. Adv. Mater. 36, e2308520 (2024).
50.
E.Ducrot, Y.Chen, M.Bulters, R.P.Sijbesma, C.Creton, Toughening elastomers with sacrificial bonds and watching them break. Science344, 186-189 (2014).
51.
K.Sato, T.Nakajima, T.Hisamatsu, T.Nonoyama, T.Kurokawa et al., Phase-separation-induced anomalous stiffening, toughening, and self-healing of polyacrylamide gels. Adv. Mater. 27, 6990-6998 (2015).
52.
Y.Wang, Y.Liu, N.Hu, P.Shi, C.Zhang et al., Highly stretchable and self-healable ionogels with multiple sensitivity towards compression, strain and moisture for skin-inspired ionic sensors. Sci. China Mater. 65, 2252-2261 (2022).
53.
V.R.Feig, H.Tran, M.Lee, Z.Bao, Mechanically tunable conductive interpenetrating network hydrogels that mimic the elastic moduli of biological tissue. Nat. Commun. 9, 2740 (2018).
54.
K.-X.Hou, S.-P.Zhao, D.-P.Wang, P.-C.Zhao, C.-H.Li et al., A puncture-resistant and self-healing conductive gel for multifunctional electronic skin. Adv. Funct. Mater. 31, 2107006 (2021).
55.
L.Cai, J.Fan, S.Ding, D.He, X.Zeng et al., Soft composite gels with high toughness and low thermal resistance through lengthening polymer strands and controlling filler. Adv. Funct. Mater. 33, 2207143 (2023).
56.
M.Zammali, S.Liu, W.Yu, A biomimetic skin-like sensor with multiple sensory capabilities based on hybrid ionogel. Sens. Actuat. A Phys. 330, 112855 (2021).
X.Qu, Z.Liu, P.Tan, C.Wang, Y.Liu et al., Artificial tactile perception smart finger for material identification based on triboelectric sensing. Sci. Adv.8, eabq2521 (2022).
62.
J.Wang, Y.Liu, T.Liu, S.Zhang, Z.Wei et al., Dynamic thermostable cellulosic triboelectric materials from multilevel-non-covalent interactions. Small (2023).