In the past two decades, artificial skin-like materials have received increasing research interests for their broad applications in intelligence, wearable devices, and soft robotics. However, profound challenges remain terms of imitating human skin because its unique combination mechanical sensory properties. this work, a bioinspired mineral hydrogel is developed to fabricate novel type mechanically adaptable ionic sensor. Due viscoelastic properties, hydrogel-based capacitive sensor...

Abstract Stretchable ionic skins are intriguing in mimicking the versatile sensations of natural skins. However, for their applications advanced electronics, good elastic recovery, self-healing, and more importantly, skin-like nonlinear mechanoresponse (strain-stiffening) essential but can be rarely met one material. Here we demonstrate a robust proton-conductive skin design via introducing an entropy-driven supramolecular zwitterionic reorganizable network to hydrogen-bonded polycarboxylic...

A facile one-step strategy for graphene oxide interpenetrating PNIPAM hydrogel networks is developed by covalently bonding GO sheets and PNIPAM-co-AA microgels directly in water, which exhibit dual thermal pH response with good reversibility.

Azobenzene-containing cross-linked liquid crystal polymer films without hydrophilic groups exhibit dual-responsivity to humidity and UV light. The realize not only a series of large sophisticated contactless motions by utilizing moisture, including an inchworm walk, tumbling locomotion, but also dual-mode actuation that can be applied in flexible electronics.

Coaxial wet-spinning is used to fabricate stretchable liquid metal sheath-core microfibers with consistently high conductance.

Abstract Given increasing environmental issues due to the large usage of non‐biodegradable plastics based on petroleum, new plastic materials, which are economic, environmentally friendly, and recyclable in high demand. One feasible strategy is bio‐inspired synthesis mineral‐based hybrid materials. Herein we report a facile route for an amorphous CaCO 3 (ACC)‐based hydrogel consisting very small ACC nanoparticles physically cross‐linked by poly(acrylic acid). The shapeable, stretchable,...

Hydrogels are usually recognized as soft and weak materials, the poor mechanical properties of which greatly limit their applications structural elements. Designing hydrogels with high strength modulus has both fundamental practical significances. Herein we report a series tough, stiff, transparent facilely prepared by copolymerization 1-vinylimidazole methacrylic acid in dimethyl sulfoxide followed solvent exchange to water. The equilibrated water content 50–60 wt % possessed excellent...

Underwater adhesion is crucial to many marine life forms living a sedentary lifestyle. Amongst them, mussel has been mostly studied, which inspires numerous investigations of 3,4-dihydroxyphenylalanine (DOPA)-based organic adhesives. In contrast, reef-building oysters represent another important "inorganic" strategy molluscs for by generating biomineralized organic–inorganic adhesives, still rarely studied and no synthetic analogues have ever reported so far. Here, novel type oyster-inspired...

Abstract Robust ionic sensing materials that are both fatigue-resistant and self-healable like human skin essential for soft electronics robotics with extended service life. However, most existing artificial skins produced on the basis of network reconfiguration suffer from a low fatigue threshold due to easy fracture low-energy amorphous polymer chains susceptible crack propagation. Here we engineer fatigue-free yet fully healable hybrid toughened by high-energy, elastic nanomesh,...

Abstract Development of a universal stretchable ionic conductor coating on insulating substrates, irrespective surface chemistry and substrate shapes, is immense interest for compliant integrative large‐area electronics but has proved to be extremely challenging. Existing methods relying either the concurrent deposition polymerizing precursors or divided formulation painting processes both suffer from several limitations in terms adhesion, dehydration, processability, pre‐treatment. Here an...

Shock-induced low-frequency vibration damage is extremely harmful to bionic soft robots and machines that may incur the malfunction of fragile electronic elements. However, current skin-like self-healable ionic elastomers as artificial sensing protecting layer still lack ability dampen vibrations, due their almost opposite design for molecular frictions material's elasticity. Inspired by two-phase structure adipose tissue (the natural damping skin layer), here, a highly elastomer with...

Humans use periodically ridged fingertips to precisely perceive the characteristics of objects via ion-based fast- and slow-adaptive mechanotransduction. However, designing artificial ionic skins with fingertip-like tactile capabilities remains challenging because contradiction between structural compliance pressure sensing accuracy (e.g., anti-interference from stretch texture recognition). Inspired by formation modulus-contrast hierarchical structure fingertips, an aesthetic skin grown a...

Robust damage-tolerant hydrogel fibers with high strength, crack resistance, and self-healing properties are indispensable for their long-term uses in soft machines robots as load-bearing actuating elements. However, current inherent homogeneous structure generally vulnerable to defects cracks thus local mechanical failure readily occurs across fiber normal. Here, inspired by spider spinning, we introduce a facile, energy-efficient aqueous pultrusion spinning process continuously produce...

Abstract Self‐adhesive materials that can directly adhere to diverse solid surfaces are indispensable in modern life and technologies. However, it remains a challenge develop self‐adhesive with strong adhesion while maintaining its intrinsic softness for efficient tackiness. Here, peeling–stiffening ionogel reconciles the seemingly contradictory properties of is reported. The contains two ionophilic repeating units distinct associating affinities, which allows adaptively wet rough surface...

Abstract Robust interfacial compliance is essential for long-term physiological monitoring via skin-mountable ionic materials. Unfortunately, existing epidermal skins are not compliant and durable enough to accommodate the time-varying deformations of convoluted skin surface, due an imbalance in viscosity elasticity. Here we introduce a self-compliant that consistently works at critical gel point state with almost equal elasticity over super-wide frequency range. The material designed by...

Impact-stiffening materials that undergo a strain rate-induced soft-to-rigid transition hold great promise as soft armors in the protection of human body and equipment. However, current impact-stiffening materials, such polyborosiloxanes shear-thickening fluids, often exhibit limited response. Herein, we propose design strategy for fabricating highly supramolecular polymer networks by leveraging high-entropy-penalty physical interactions. We synthesized fully biobased comprising...

Dynamic thermally reversible hydration behavior of a well-defined thermoresponsive copolymer P(MEO2MA-co-OEGMA475) in D2O synthesized by ATRP random copolymerization 2-(2-methoxyethoxy)ethyl methacrylate (MEO2MA) and oligo(ethylene glycol) (Mn = 475 g/mol) was studied means IR spectroscopy combination with perturbation correlation moving window (PCMW) technique two-dimensional (2DCOS). Largely different from poly(N-isopropylacrylamide) (PNIPAM), exhibits sharp change below LCST gradual above...

A facile methodology has been developed to immobilize well-defined polymers onto graphene sheets using "click" chemistry; upon polystyrene coupling, the resulting can be well dispersed and fully exfoliated in common organic media.

Abstract Inorganic nanoparticles (NPs) are promising drug delivery carriers owing to their high loading efficiency, scalable preparation, facile functionalization, and chemical/thermal stability. However, the clinical translation of inorganic nanocarriers is often hindered by poor biodegradability lack controlled pH response. Herein, a fully degradable pH‐responsive DOX@ACC/PAA NP (pH 7.4–5.6) developed encapsulating doxorubicin (DOX) in poly(acrylic acid) (PAA) stabilized amorphous calcium...

IR spectroscopy in combination with two-dimensional correlation (2DCOS) and the perturbation moving window (PCMW) technique is employed to illustrate dynamic hydration behavior of poly(N-vinylcaprolactam) (PVCL) water, which exhibits a typical type I continuous lower critical solution temperature (LCST) behavior. PCMW easily determined transition be ca. 43.5 °C during heating 42.5 cooling range 39.5-45 °C. On other hand, 2DCOS was used discern sequence order different species PVCL concluded...

Abstract Stretchable hydrogel microfibers as a novel type of ionic conductors are promising in gaining skin‐like sensing applications more diverse scenarios. However, it remains great challenge to fabricate coating‐free but water‐retaining conductive with good balance spinnability and mechanical strength. Here the old yet significant redox chemistry Fe‐citrate complex is employed solve this issue continuous draw‐spinning process poly(acrylamide‐ co ‐sodium acrylate) microfiber nets from...

Stretchable ionic conductors are appealing for tissue-like soft electronics, yet suffer from a tardy mechanoelectric response due to their poor modulation of conduction arising intrinsic homogeneous chain network. Here, highly robust ionotronic fiber is designed by synergizing liquid and crystal elastomer with alternate rigid mesogen units spacers, which shows an unprecedented strain-induced conductivity boost (≈103 times enhanced as stretched 2000% strain). Such surprisingly high...

Thermal stiffening materials that are naturally soft but adaptively self-strengthen upon heat intriguing for load-bearing and self-protection applications at elevated temperatures. However, to simultaneously achieve high modulus change amplitude mechanical strength the stiffened state remains challenging. Herein, entropy-mediated polymer-mineral cluster interactions exploited afford thermal hydrogels with a record-high storage enhancement of 13 000 times covering super wide regime from 1.3...

Stretchable ionic conductors are crucial for enabling advanced iontronic devices to operate under diverse deformation conditions. However, when employed as interconnects, existing struggle maintain stable conduction strain, hindering high-fidelity signal transmission. Here, it is shown that strain-insensitive can be achieved by creating a solid-liquid bicontinuous microstructure. A fiber from polymerization-induced phase separation, which contains solid elastomer interpenetrated liquid...