The hydrogels are widely used in various applications, and their successful uses depend on controlling the mechanical properties. In this study, we present an advanced strategy to develop hydrogel actuator designed to stimulate live cell clusters by self-folding. The hydrogel actuator consisting of two layers with different expansion ratios were fabricated to have various curvatures in self-folding. The expansion ratio of the hydrogel tuned with the molecular weight and concentration of gel-forming polymers, and temperature-sensitive molecules in a controlled manner. As a result, the hydrogel actuator could stimulate live cell clusters by compression and tension repeatedly, in response to temperature. The cell clusters were compressed in the 0.7-fold decreases of the radius of curvature with 1.0 mm in room temperature, as compared to that of 1.4 mm in 37 °C. Interestingly, the vascular endothelial growth factor (VEGF) and insulin-like growth factor-binding protein-2 (IGFBP-2) in MCF-7 tumor cells exposed by mechanical stimulation was expressed more than in those without stimulation. Overall, this new strategy to prepare the active and soft hydrogel actuator would be actively used in tissue engineering, drug delivery, and micro-scale actuators.

To use implantable biomedical devices such as electrocardiograms and neurostimulators in the human body, it is necessary to package them with biocompatible materials that protect the internal electronic circuits from the body’s internal electrolytes and moisture without causing foreign body reactions. Herein, we describe a hydrogel surface-modified polyurethane copolymer film with concurrent water permeation resistance and biocompatibility properties for application to an implantable biomedical device. To achieve this, hydrophobic polyurethane copolymers comprising hydrogenated poly(ethylene-co-butylene) (HPEB) and aliphatic poly(carbonate) (PC) were synthesized and their hydrophobicity degree and mechanical properties were adjusted by controlling the copolymer composition ratio. When 10 wt% PC was introduced, the polyurethane copolymer exhibited hydrophobicity and water permeation resistance similar to those of HPEB; however, with improved mechanical properties. Subsequently, a hydrophilic poly(vinyl pyrrolidone) (PVP) hydrogel layer was formed on the surface of the polyurethane copolymer film by Fenton reaction using an initiator and crosslinking agent and the effect of the initiator and crosslinking agent immobilization time, PVP concentration and crosslinking agent concentration on the hydrogel properties were investigated. Finally, MTT assay showed that the hydrogel surface-modified polyurethane copolymer film displays excellent biocompatibility.

Multi-layered hydrogels consisting of bi- or tri-layers with different swelling ratios are designed to soft hydrogel actuators by self-folding. The successful use of multi-layered hydrogels in this application greatly relies on the precise design and fabrication of the curvature of self-folding. In general, however, the self-folding often results in an undesired mismatch with the expecting value. To address this issue, this study introduces an interfacial layer formed between each layered hydrogel, and this layer is evaluated to enhance the design and fabrication precision. By considering the interfacial layer, which forms through diffusion, as an additional layer in the multi-layered hydrogel, the degree of mismatch in the self-folding is significantly reduced. Experimental results show that as the thickness of the interfacial layer increases, the multi-layered hydrogel exhibits a 3.5-fold increase in its radius of curvature during the self-folding. In addition, the diffusion layer is crucial for creating robust systems by preventing the separation of layers in the muti-layered hydrogel during actuation, thereby ensuring the integrity of the system in operation. This new strategy for designing multi-layered hydrogels including an interfacial layer would greatly serve to fabricate precise and robust soft hydrogel actuators.

This study presents the synthesis and characterization of hexadecyl-modified SiO₂ (HD-SiO₂) nanoparticles and their application in the fabrication of a multilayered elastomer hybrid sheet to enhance water resistance in implantable biomedical devices. The surface modification of SiO₂ nanoparticles was confirmed via FT-IR and TGA analyses, showing the successful grafting of hydrophobic hexadecyl groups. FE-SEM and DLS analyses revealed spherical HD-SiO₂ nanoparticles with an average size of 360 nm. A multilayered elastomer hybrid sheet, consisting of a PDMS-based circuit-protecting body, a water resistance layer of HD-SiO₂, a planarization layer, and a biocompatible layer of polydopamine, was fabricated and characterized. The water resistance layer exhibited superhydrophobic properties, with a water contact angle of 154.7° and a 27% reduction in water vapor transmission rate (WVTR) compared to the circuit-protecting body alone. The device packaged with both the circuit-protecting body and water resistance layer demonstrated a tenfold increase in operational lifespan in water medium compared to the device without the water resistance layer. Cytotoxicity and cell proliferation tests on human dermal fibroblast cells (HDFn) confirmed the biocompatibility of the multilayered sheet, with no significant cytotoxicity observed over 48 h.