Photo-steered rapid and multimodal locomotion of 3D-printed tough hydrogel robots.

Hydrogels are an ideal material to develop soft robots. However, it remains a grand challenge to develop miniaturized hydrogel robots with mechanical robustness, rapid actuation, and multi-gait motions. Reported here is a facile strategy to fabricate hydrogel-based soft robots by three-dimensional (3D) printing of responsive and nonresponsive tough gels for programmed morphing and locomotion upon stimulations.

Bistable Joints Enable the Morphing of Hydrogel Sheets with Multistable Configurations.

Joints, as a flexing element to connect different parts, are widespread in natural systems. Various joints exist in the body and play crucial roles to execute gestures and gaits. These scenarios have inspired the design of mechanical joints with passive, hard materials, which usually need an external power supply to drive the transformations.

Magneto-Orientation of Magnetic Double Stacks for Patterned Anisotropic Hydrogels with Multiple Responses and Modulable Motions.

Reported here is a multi-response anisotropic poly(N-isopropylacrylamide) hydrogel developed by using a rotating magnetic field to align magnetic double stacks (MDSs) that are fixed by polymerization. The magneto-orientation of MDSs originates from the unique structure with γ-Fe O nanoparticles sandwiched by two silicate nanosheets. The resultant gels not only exhibit anisotropic optical and mechanical properties but also show anisotropic responses to temperature and light.

An Opto- and Thermal-Rewrite PCM/CNF-IR 780 Energy Storage Nanopaper with Mechanical Regulated Performance.

In spite of efforts to fabricate self-assembled energy storage nanopaper with potential applications in displays, greenhouses, and sensors, few studies have investigated their multiple stimuli-sensitivities. Here, an opto- and thermal-rewrite phase change material/cellulose nanofibril (PCM/CNF) energy storage nanopaper with mechanical regulated performance is facilely fabricated, through 5 min sonication of PCMs and CNFs in an aqueous system. The combination of PCM and CNF not only guarantees the recyclability of PCM without leakage, but also offers nanopaper adaptive properties by leveraging the mobility and optical variation accompanying solid-to-liquid transition of PCM.

Programmable Morphing Hydrogels for Soft Actuators and Robots: From Structure Designs to Active Functions.

Nature provides abundant inspiration and elegant paradigms for the development of smart materials that can actuate, morph, and move on demand. One remarkable capacity of living organisms is to adapt their shapes or positions in response to stimuli. Programmed deformations or movements in plant organs are mainly driven by water absorption/dehydration of cells, while versatile motions of mollusks are based on contraction/extension of muscles.

Electrical switching of high-performance bioinspired nanocellulose nanocomposites.

Nature fascinates with living organisms showing mechanically adaptive behavior. In contrast to gels or elastomers, it is profoundly challenging to switch mechanical properties in stiff bioinspired nanocomposites as they contain high fractions of immobile reinforcements. Here, we introduce facile electrical switching to the field of bioinspired nanocomposites, and show how the mechanical properties adapt to low direct current (DC).

Recyclable and Light-Adaptive Vitrimer-Based Nacre-Mimetic Nanocomposites.

Nacre's natural design consists of a perfect hierarchical assembly that resembles a brick-and-mortar structure with synergistic stiffness and toughness. The field of bioinspired materials often provides attractive architecture and engineering pathways which allow to explore outstanding property areas. However, the study of nacre-mimetic materials should not be limited to the design of its architecture but ought to include the understanding, operation, and improvement of internal interactions between their components.

Room-Temperature Phosphorescence Enabled through Nacre-Mimetic Nanocomposite Design.

A generic, facile, and waterborne strategy is introduced to fabricate flexible, low-cost nanocomposite films with room-temperature phosphorescence (RTP) by incorporating waterborne RTP polymers into self-assembled bioinspired polymer/nanoclay nanocomposites. The excellent oxygen barrier of the lamellar nanoclay structure suppresses the quenching effect from ambient oxygen (k ) and broadens the choice of polymer matrices towards lower glass transition temperature (T ), while providing better mechanical properties and processability. Moreover, the oxygen permeation and diffusion inside the films can be fine-tuned by varying the polymer/nanoclay ratio, enabling programmable retention times of the RTP signals, which is exploited for transient information storage and anti-counterfeiting materials.

Self-Assembled Bioinspired Nanocomposites.

Bioinspired materials engineering impacts the design of advanced functional materials across many domains of sciences from wetting behavior to optical and mechanical materials. In all cases, the advances in understanding how biology uses hierarchical design to create failure and defect-tolerant materials with emergent properties lays the groundwork for engaging into these topics. Biological mechanical materials are particularly inspiring for their unique combinations of stiffness, strength, and toughness together with lightweightness, as assembled and grown in water from a limited set of building blocks at room temperature.

Glass Transition Temperature Regulates Mechanical Performance in Nacre-Mimetic Nanocomposites.

Although research in bioinspired nanocomposites is delivering mechanically superior nanocomposite materials, there remain gaps in understanding some fundamental design principles. This article discusses how the mechanical properties of nacre-mimetic polymer/nanoclay nanocomposites with nanoconfined polymer layers are controlled by the thermo-mechanical polymer properties, that is, glass transition temperature, T using a series of poly(ethylene glycol methyl ether methacrylate-co-N,N-dimethylacrylamide) copolymers with tunable T from 130 to -55 °C. It is elucidated that both the type of copolymer and the nanoconfined polymer layer thickness control energy dissipation and inelastic deformation at high fractions of reinforcements in such bioinspired nanocomposites.

Biodegradable Laser Arrays Self-Assembled from Plant Resources.

The transition toward future sustainable societies largely depends on disruptive innovations in biobased materials to substitute nonsustainable advanced functional materials. In the field of optics, advanced devices (e.g.

Hierarchical cross-linking for synergetic toughening in crustacean-mimetic nanocomposites.

The twisted plywood structure as found in crustacean shells possesses excellent mechanical properties with high stiffness and toughness. Synthetic mimics can be produced by evaporation-induced self-assembly of cellulose nanocrystals (CNCs) with polymer components into bulk films with a cholesteric liquid crystal structure. However, these are often excessively brittle and it has remained challenging to make materials combining high stiffness and toughness.

Highly Mineralized Biomimetic Polysaccharide Nanofiber Materials Using Enzymatic Mineralization.

Many biological high-performance composites, such as bone, antler, and crustacean cuticles, are composed of densely mineralized and ordered nanofiber materials. The mimicry of even simplistic bioinspired structures, i.e.

Waterborne Methacrylate-Based Vitrimers.

We demonstrate waterborne, unimolecularly dissolved vitrimer prepolymer systems that can be transferred into a vitrimer material using catalytic transesterification. The one-component prepolymer system can be processed via film casting and subsequent heat-induced cross-linking. A variation of the density of side chain hydroxy groups over ester and amide groups in the methacrylate/methacrylamide backbone, as well as of the Lewis acid catalyst loading, allow control of the extent of cross-linking and exchange rates.

Vitrimer Chemistry Meets Cellulose Nanofibrils: Bioinspired Nanopapers with High Water Resistance and Strong Adhesion.

Nanopapers containing cellulose nanofibrils (CNFs) are an emerging and sustainable class of high performance materials. The diversification and improvement of the mechanical and functional property space critically depend on integration of CNFs with rationally designed, tailor-made polymers following bioinspired nanocomposite designs. Here we combine for the first time CNFs with colloidal dispersions of vitrimer nanoparticles (VP) into mechanically coherent nanopaper materials.

Facile and On-Demand Cross-Linking of Nacre-Mimetic Nanocomposites Using Tailor-Made Polymers with Latent Reactivity.

The development of on-demand cross-linking strategies is a key aspect in promoting mechanical properties of high-performance bioinspired nanocomposites. Here, we embed styrene sulfonyl azide groups with latent chemical reactivity into water-soluble copolymers and assemble those with high-aspect-ratio synthetic nanoclays to generate well-defined layered polymer/nanoclay nacre-mimetics. A considerable stiffening and strengthening occurs upon activation of the covalent cross-linking using simple heating.

Highly Anisotropic Thermal Conductivity of Layer-by-Layer Assembled Nanofibrillated Cellulose/Graphene Nanosheets Hybrid Films for Thermal Management.

An anisotropic thermally conductive film with tailorable microstructures and macroproperties is fabricated using a layer-by-layer (LbL) assembly of graphene oxide (GO) and nanofibrillated cellulose (NFC) on a flexible NFC substrate driven by hydrogen bonding interactions, followed by chemical reduction process. The resulting NFC/reduced graphene oxide (RGO) hybrid film reveals an orderly hierarchical structure in which the RGO nanosheets exhibit a high degree of orientation along the in-plane direction. The assembly cycles dramatically increase the in-plane thermal conductivity (λ) of the hybrid film to 12.

Development of self-assembling peptide nanovesicle with bilayers for enhanced EGFR-targeted drug and gene delivery.

Development of rational vectors for efficient drug and gene delivery is crucial for cancer treatment. In this study, epidermal growth factor receptor (EGFR)-binding peptide amphiphile (PA) were used as the primary bilayer skeleton material to construct ultra-stable self-assembling peptide nanovesicle (SPV). The resulted EGFR-targeted SPV (ESPV) could efficiently encapsulate therapeutic cargos (drugs or small interfering RNAs [siRNAs]) or labelled fluorescent cargo (quantum dots [QDs]) and exhibited excellent affinity for EGFR-positive cancer cells.