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Hydrogels are ideal interfacing materials for on-skin healthcare devices, yet their susceptibility to dehydration hinders their practical use. While incorporating hygroscopic metal salts can prevent dehydration and maintain ionic conductivity, concerns arise regarding metal toxicity due to the passage of small ions through the skin barrier. Herein, an antidehydration hydrogel enabled by the incorporation of zwitterionic oligomers into its network is reported. This hydrogel exhibits exceptional water retention properties, maintaining ≈88% of its weight at 40% relative humidity, 25 °C for 50 days and about 84% after being heated at 50 °C for 3 h. Crucially, the molecular weight design of the embedded oligomers prevents their penetration into the epidermis, as evidenced by experimental and molecular simulation results. The hydrogel allows stable signal acquisition in electrophysiological monitoring of humans and plants under low-humidity conditions. This research provides a promising strategy for the development of epidermis-safe and biocompatible antidehydration hydrogel interfaces for on-skin devices., (© 2023 Wiley-VCH GmbH.)

Transparent electrodes that form seamless contact and enable optical interrogation at the electrode-brain interface are potentially of high significance for neuroscience studies. Silk hydrogels can offer an ideal platform for transparent neural interfaces owing to their superior biocompatibility. However, conventional silk hydrogels are too weak and have difficulties integrating with highly conductive and stretchable electronics. Here, a transparent and stretchable hydrogel electrode based on poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) and PEGylated silk protein is reported. PEGylated silk protein with poly(ethylene glycol) diglycidyl ether (PEGDE) improves the Young's modulus to 1.51-10.73 MPa and the stretchability to ≈400% from conventional silk hydrogels (<10 kPa). The PEGylated silk also helps form a robust interface with PEDOT:PSS thin film, making the hydrogel electrode synergistically incorporate superior stretchability (≈260%), stable electrical performance (≈4 months), and a low sheet resistance (≈160 ± 56 Ω sq -1 ). Finally, the electrode facilitates efficient electrical recording, and stimulation with unobstructed optical interrogation and rat-brain imaging are demonstrated. The highly transparent and stretchable hydrogel electrode offers a practical tool for neuroscience and paves the way for a harmonized tissue-electrode interface., (© 2021 Wiley-VCH GmbH.)

Plant electrophysiology lays the foundation for smart plant interrogation and intervention. However, plant trichomes with hair-like morphologies present topographical features that challenge stable and high-fidelity non-invasive electrophysiology, due to the inadequate dynamic shape adaptability of conventional electrodes. Here, this issue is overcome using a morphable ionic electrode based on a thermogel, which gradually transforms from a viscous liquid to a viscoelastic gel. This transformation enables the morphable electrode to lock into the abrupt hairy surface irregularities and establish a conformal and adhesive interface. It achieves down to one tenth of the impedance and 4-5 times the adhesive strengths of conventional hydrogel electrodes on hairy leaves. As a result of the improved electrical and mechanical robustness, the morphable electrode can record more than one order of magnitude higher signal-to-noise ratio on hairy plants and maintains high-fidelity recording despite plant movements, achieving superior performance to conventional hydrogel electrodes. The reported morphable electrode is a promising tool for hairy plant electrophysiology and may be applied to diversely textured plants for advanced sensing and modulation., (© 2021 Wiley-VCH GmbH.)

Soft electronics that seamlessly interface with skin are of great interest in health monitoring and human–machine interfaces. However, achieving mechanical softness, skin adhesiveness, and high conductivity concurrently has always been a major challenge due to the difficulty in bonding dissimilar materials while retaining their respective properties. Herein, the mechanically interlocked hydrogel–elastomer hybrid is reported as a viable solution to this problem. Hydrogels with low moduli and high adhesiveness are employed as the substrate, while porous elastomer webs are used as matrices to load conductive films and lock the hydrogels through a mechanically interlocked structure. The bonding strength between the hydrogel and elastomer in the interlocking hybrid structure is 14.3 times of that obtained via the physical stacking method. As a proof of concept, interlocking hybrids are used as on‐skin electrodes for electrophysiological signal recording including electromyography and electrocardiography. The robust hybrid electrodes are able to detect signals after multiple cycles. The proposed strategy not only is an effective approach to achieve interlocking structures, but also provides a new perspective for soft and stretchable electronics. [ABSTRACT FROM AUTHOR]

Underwater adhesion is greatly desired in tissue transplantation, medical treatment, ocean transportation, and so on. However, common commercial polymeric adhesives are rather weakened and easily destroyed in water environment. In nature, some marine organisms, such as mussels, barnacles, or tube worms, exhibiting excellent underwater adhesion up to robust bonding on the rock of sea floor, can give exciting solutions to address the problem. Among these marine organisms, mussels exhibit unique underwater adhesion via the foot proteins of byssus. It has been verified that the catechol groups from the side chain of the mussel foot proteins is the main contribution to the unique underwater adhesion. Hence, inspired by the mussels' underwater adhesion, many mussel-mimetic polymers with catechol as end chains or side chains have been developed in the past decades. Here, we review recent progress of mussel-inspired underwater adhesives polymers from their catechol-functional design to their potential applications in intermediates, anti-biofouling, self-healing of hydrogels, biological adhesives, and drug delivery. The review may provide basis and help for the development of the commercial underwater adhesives. [ABSTRACT FROM AUTHOR]

Liquid spreading is of significant interest in science and technology. Although surface topography engineering and liquid surface-tension regulating can facilitate spreading, the spreading layers in these strategies are inevitably inhomogeneous or contaminated with surfactants. Herein, we show a general strategy to realize the superspreading of liquids on mutually soluble gel surfaces. The cooperation of the hydraulic pressure under liquid phase and liquid-like property of gel surfaces can dramatically eliminate the local pinning effect and enhance the advancement of three-phase contact line, thus forming stable and homogeneous superspreading liquid layers. Such liquid layers can be converted into various functional thin polymer films with controlled thicknesses (nm- to µm-scale) through one-step polymerization of the reactants. Our strategy offers opportunities for large-scale synthesis of versatile functional thin films for various applications. [ABSTRACT FROM AUTHOR]

Liquid spreading is of significant interest in science and technology. Although surface topography engineering and liquid surface-tension regulating can facilitate spreading, the spreading layers in these strategies are inevitably inhomogeneous or contaminated with surfactants. Herein, we show a general strategy to realize the superspreading of liquids on mutually soluble gel surfaces. The cooperation of the hydraulic pressure under liquid phase and liquid-like property of gel surfaces can dramatically eliminate the local pinning effect and enhance the advancement of three-phase contact line, thus forming stable and homogeneous superspreading liquid layers. Such liquid layers can be converted into various functional thin polymer films with controlled thicknesses (nm- to µm-scale) through one-step polymerization of the reactants. Our strategy offers opportunities for large-scale synthesis of versatile functional thin films for various applications. [ABSTRACT FROM AUTHOR]