Introducing methods for instant tough bonding between hydrogels and antagonistic materials—from soft to hard—allows us to demonstrate elastic yet tough biomimetic devices and machines with a high level of complexity. Tough hydrogels strongly attach, within seconds, to plastics, elastomers, leather, bone, and metals, reaching unprecedented interfacial toughness exceeding 2000 J/m². Healing of severed ionic hydrogel conductors becomes feasible and restores function instantly. Soft, transparent multilayered hybrids of elastomers and ionic hydrogels endure biaxial strain with more than 2000% increase in area, facilitating soft transducers, generators, and adaptive lenses. We demonstrate soft electronic devices, from stretchable batteries, self-powered compliant circuits, and autonomous electronic skin for triggered drug delivery. Our approach is applicable in rapid prototyping and in delicate environments inaccessible for extended curing and cross-linking.

Purpose: This papers aims to study the influence of water absorption on the mechanical properties of poly lactic acid (PLA) and PLA/Wood composites. Virgin PLA and PLA/Wood double-bone-shaped specimens were prepared by two methods: injection moulding and 3D printing. The results were compared to each other and showed the influence of the production method on the properties of the produced parts. Design/methodology/approach: Morphology studies were done by scanning electron microscopy (SEM) from fracture surfaces of tensile and notched impact specimens of all samples. Tensile properties were analysed by the production and testing of dog-bone-shaped samples. Heat deflection temperature (HDT) was tested, as also was the crystallinity of the tested samples by differential scanning calorimetry. Findings: The values for notched impact strength were higher upon water uptake in the case of injection-moulded specimens, which was not the case with 3D-printed specimens. Tensile properties of the specimens produced by both methods were reduced after water absorption tests. Values of the HDT were also lower after water absorption tests studied for both processing methods. Originality/value: Morphology studies were done by SEM from fracture surfaces of tensile as well as notched impact specimens of injection-moulded and 3D-printed samples. The effect of water storage on various samples was tested. The two different production technologies were compared to each other owing to their influence of water storage. This study also dealt with NFC compounds and produced NFC composites and the influence of water storage on these samples.

The crustacean cuticle is a composite material that covers the whole animal and forms the continuous exoskeleton. Nano-fibers composed of chitin and protein molecules form most of the organic matrix of the cuticle that, at the macroscale, is organized in up to eight hierarchical levels. At least two of them, the exo- and endocuticle, contain a mineral phase of mainly Mg-calcite, amorphous calcium carbonate and phosphate. The high number of hierarchical levels and the compositional diversity provide a high degree of freedom for varying the physical, in particular mechanical, properties of the material. This makes the cuticle a versatile material ideally suited to form a variety of skeletal elements that are adapted to different functions and the eco-physiological strains of individual species. This review presents our recent analytical, experimental and theoretical studies on the cuticle, summarising at which hierarchical levels structure and composition are modified to achieve the required physical properties. We describe our multi-scale hierarchical modeling approach based on the results from these studies, aiming at systematically predicting the structure-composition-property relations of cuticle composites from the molecular level to the macro-scale. This modeling approach provides a tool to facilitate the development of optimized biomimetic materials within a knowledge-based design approach.

The most active and efficient catalysts for the electrochemical hydrogen evolution reaction (HER) rely on platinum, a fact that increases the cost of producing hydrogen and thereby limits the widespread adoption of this fuel. Here, a metal‐free organic electrocatalyst that mimics the platinum surface by implementing a high work function and incorporating hydrogen‐affine hydrogen bonds is introduced. These motifs, inspired from enzymology, are deployed here as selective reaction centres. It is shown that the keto‐amine hydrogen‐bond motif enhances the rate‐determining step in proton reduction to molecular hydrogen. The keto‐amine‐functionalized polymers reported herein evolve hydrogen at an overpotential of 190 mV. They share certain key properties with platinum: a similar work function and excellent electrochemical stability and chemical robustness. These properties allow the demonstration of one week of continuous HER operation without notable degradation nor delamination from the carrier electrode. Scaled continuous‐flow electrolysis is reported and 1 L net molecular hydrogen is produced within less than 9 h using 2.3 mg of polymer electrocatalyst.

A simple supramolecular crosslinked gel is reported with a photosensitive ruthenium bipyridine complex functioning as a crosslinker and poly(4‐vinylpyridine) (P4VP) as a macromolecular ligand. Irradiation of the organogels in H₂O/MeOH with visible and NIR light (in a multiphoton process) leads to cleavage of pyridine moieties from the ruthenium complex breaking the cross‐links and causing degelation and hence solubilization of the P4VP chains. Real‐time (RT) photorheology experiments of thin films showed a rapid degelation in several seconds, whereas larger bulk samples could also be photocleaved. Furthermore, the gels could be reformed or healed by simple heating of the system and restoration of the metal–ligand crosslinks. The relatively simple dynamic system with a high sensitivity towards light in the visible and NIR region make them interesting positive photoresists for nano/micropatterning applications, as was demonstrated by writing, erasing, and rewriting of the gels by single‐ and multiphoton lithography.