Press-N-Go On-Skin Sensor with High Interfacial Toughness for Continuous Healthcare Monitoring.

On-skin electronic sensors are demanded for healthcare monitoring such as the continuous recording of biopotential and motion signals from patients. However, the mechanical mismatches and poor interface adhesion at the skin/sensor interfaces always cause high interfacial impedance and artifacts, frequent interfacial failure, and unexpected depletion of the device, which significantly limit the performance of the sensors. We here develop an on-skin sensor based on a conductive pressure-sensitive tape, which is assembled from supramolecular dual-cross-linked hydrogel composites. Both covalent and noncovalent cross-links in the hydrogel networks could harvest high flexibility, pressure-sensitive adhesion, and high interfacial toughness altogether, enabling a convenient "Press-N-Go" application of the sensor on human skin without additional pre/post-treatment on the skin or the senor. The high conformability and low resistivity of the tape can sustainably lower the interfacial impedance and thus improve signal quality in various measurement conditions. Our design provides a feasible path to develop interface-toughened on-skin electronics, which is desired in dynamic human-machine interfaces.

Supramolecular Adhesive Materials with Antimicrobial Activity for Emerging Biomedical Applications.

Traditional adhesives or glues such as cyanoacrylates, fibrin glue, polyethylene glycol, and their derivatives have been widely used in biomedical fields. However, they still suffer from numerous limitations, including the mechanical mismatch with biological tissues, weak adhesion on wet surfaces, biological incompatibility, and incapability of integrating desired multifunction. In addition to adaptive mechanical and adhesion properties, adhesive biomaterials should be able to integrate multiple functions such as stimuli-responsiveness, control-releasing of small or macromolecular therapeutic molecules, hosting of various cells, and programmable degradation to fulfill the requirements in the specific biological systems. Therefore, rational molecular engineering and structural designs are required to facilitate the development of functional adhesive materials. This review summarizes and analyzes the current supramolecular design strategies of representative adhesive materials, serving as a general guide for researchers seeking to develop novel adhesive materials for biomedical applications.

Liquid Metal Nanoparticles as a Highly Efficient Photoinitiator to Develop Multifunctional Hydrogel Composites.

Liquid metal (LM) composites are a class of emerging soft multifunctional materials that are promising for a variety of applications, yet the chemistry properties of LM have not been fully understood. Here, we report that LM nanoparticles can directly perform as a photoinitiator for radical polymerization and the in situ development of highly tough and multifunctional LM hydrogel composites. It is revealed that the photocatalytic activity of LM nanoparticles originates from the oxide layer on LM. Significantly, positively charged metal-organic framework (MOF) nanoparticles are used to stabilize LM nanoparticles in aqueous solutions, where the MOF can anchor on the surface of LM nanoparticles by electrostatic interaction while helping to preserve the unshielded oxide layer, therefore realizing the highly efficient photoinitiation and polymerization. The LM nanoparticle-initiated photopolymerization is shown to develop hydrogel composites featuring excellent stretchability, stimuli responsiveness, and sustained photocatalytic activity. The photocatalytic polymerization initiated by LM nanoparticles not only deepens the understanding on the semiconductor properties of the oxide skin on LM but also broadens the application scenarios of multifunctional LM/polymer composites in smart materials, wearable electronics, and soft robotics.

Bactericidal, anti-biofilm, and anti-virulence activity of vitamin C against carbapenem-resistant hypervirulent Klebsiella pneumoniae.

The emergence of carbapenem-resistant hypervirulent Klebsiella pneumoniae (CR-hvKP) causing high mortality in clinical patients infers the urgent need for developing therapeutic agents. Here, we demonstrated vitamin C (VC) exhibited strong bactericidal, anti-biofilm, and virulence-suppressing effects on CR-hvKP. Our results showed such a bactericidal effect is dose-dependent both in vitro and in the mouse infection model and is associated with induction of reactive oxygen species (ROS) generation. In addition, VC inhibited biofilm formation of CR-hvKP through suppressing the production of exopolysaccharide (EPS). In addition, VC acted as an efflux pump inhibitor at subminimum inhibitory concentration (sub-MIC) to disrupt transportation of EPS and capsular polysaccharide to bacterial cell surface, thereby further inhibiting biofilm and capsule formation. Furthermore, virulence-associated genes in CR-hvKP exposed to sub-MIC of VC were downregulated. Our findings indicated VC could be an effective and safe therapeutic agent to treat CR-hvKP infections in urgent cases when all current treatment options fail.

Continuous Energy Harvesting from Ubiquitous Humidity Gradients using Liquid-Infused Nanofluidics.

Humidity-based power generation that converts internal energy of water molecules into electricity is an emerging approach for harvesting clean energy from nature. Here it is proposed that intrinsic gradient within a humidity field near sweating surfaces, such as rivers, soil, or animal skin, is a promising power resource when integrated with liquid-infused nanofluidics. Specifically, capillary-stabilized ionic liquid (IL, Omim+ Cl- ) film is exposed to the above humidity field to create a sustained transmembrane water-content difference, which enables asymmetric ion-diffusion across the nanoconfined fluidics, facilitating long-term electricity generation with the power density of ≈12.11 µW cm-2 . This high record is attributed to the nanoconfined IL that integrates van der Waals and electrostatic interactions to block movement of Omim+ clusters while allowing for directional diffusion of moisture-liberated Cl+ . This humidity gradient triggers large ion-diffusion flux for power generation indicates great potential of sweating surfaces considering that most of the earth is covered by water or soil.

An amino acid-based supramolecular nanozyme by coordination self-assembly for cascade catalysis and enhanced chemodynamic therapy towards biomedical applications.

The clinical translation of chemodynamic therapy has been highly obstructed by the insufficient intracellular H2O2 level in diseased tissues. Herein, we developed a supramolecular nanozyme through a facile one-step cooperative coordination self-assembly of an amphipathic amino acid and glucose oxidase (GOx) in the presence of Fe2+. The results demonstrated that the supramolecular nanozyme possessed cascade enzymatic activity (i.e., GOx and peroxidase), which could amplify the killing efficacy of hydroxyl radicals (˙OH) via self-supplying H2O2, finally achieving synergistic starvation-chemodynamic cancer therapy in vitro. Additionally, this cascade nanozyme also exhibited highly effective antibacterial activity on Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus) without the need for additional H2O2. This work provided a promising strategy for the design and development of nanozymes for future biomedical applications.

Mechano-Induced Assembly of a Nanocomposite for "Press-N-Go" Coatings with Highly Efficient Surface Disinfection.

Using antimicrobial coatings to control the spread of pathogenic microbes is appreciated in public and healthcare settings, but the performance of most antimicrobial coatings could not fulfill the increasing requirements, particularly the ease of preparation, high durability, rapid response, and high killing efficiency. Herein, we develop a new type of mechano-induced assembly of nanocomposite coating by simple "Press-N-Go" procedures on various substrates such as glassware, gloves, and fabrics, in which the coating shows strong adhesion, high shear stability, and high stiffness, making it durable in daily use to withstand common mechanical deformation and scratches. The coating also shows remarkable disinfection effectiveness over 99.9% to clinically significant multiple drug-resistant bacterial pathogens upon only 6 s near-infrared irradiation, which can be further improved to over 99.9999% upon another 6 s treatment. We envision that the coating can provide convenience and values to control pathogen spread for easily contaminated substrates in high-risk areas.

Ultrastretchable conductive liquid metal composites enabled by adaptive interfacial polarization.

Gallium-based liquid metals (LMs) are emerging candidates for the development of metal/polymer-based flexible circuits in wearable electronics. However, the high surface energies of LMs make them easily depleted from the polymer matrix and therefore substantially suppress the stretchability of the conductive composites. Here, we reveal that a dynamic interplay between the LM and the polyvinylidene fluoride (PVDF) copolymer can help to address these issues. Weak and abundant interfacial polarization interactions between the PVDF copolymer and the oxide layer allow continuous and adaptive configuration of the compartmented LM channels, enabling ultra-stretchability of the composites. The conductive LM-polymer composites can maintain their structural integrity with a high surface conductivity and small resistance changes under large strains from 1000% to 10 000%. Taking advantage of their flexible processability under mild conditions and exceptional performance, our design strategy allows the scalable fabrication of conductive LM-polymer composites for a range of applications in wearable devices and sensors.

Mucus-Inspired Supramolecular Adhesives with Oil-Regulated Molecular Configurations and Long-Lasting Antibacterial Properties.

Inspired by mucus, which provides an ideal supramolecular model and whose fluid-like (viscous) and solid-like (elastic) behaviors can be adjusted to meet different physiological requirements, we report oil-regulated supramolecular adhesives by the co-assembly of polyurea oligomers and carvacrol oils. The adhesive is crosslinked by weak but abundant hydrogen bonds, which can be regulated by the incorporated carvacrol oils through the competition of intermolecular hydrogen bonds, presenting a unique set of mucus-mimicking features including oil-regulated mechanics, processability, reusable adhesivity, and extreme longevity in both air and water. Owing to the intrinsic bactericidal effect of the carvacrol oils, the developed adhesives can serve as potent antibacterial coatings with both rapid contact killing (99.9% killing within 15 min) and long-term controlled release abilities (up to 70 days), enabling versatile antibacterial applications in diverse conditions. We envision that these adhesives will be useful in buildings and architectures, community and public facilities, food storage and packaging technologies, functional textiles, and practical biomedical fields.

Particulate-Aggregated Adhesives with Exudate-Sensitive Properties and Sustained Bacteria Disinfection to Facilitate Wound Healing.

Wound-associated infections create additional suffering and come at a high cost for patients and their families, which urgently require wound disinfection biomaterials with improved healing efficacy. Here, we report an adhesive with sustained bacteria disinfection ability, which is aggregated from hydrogen-bonded polymer particulates. The particulate-aggregated adhesive shows strong binding ability on different surfaces from rigid substrates to soft skins. Moreover, water-sensitive mechanical properties are shown in wound exudates, resulting from the dissociation of hydrogen bonds under the competition of water and thus the sustained release of particulates. Synergizing with the strong binding ability, exudate-sensitive behaviors, and sustained release of antibacterial particulates, the adhesive achieves sustained bactericidal activity and can facilitate the healing process in bacteria-infected skin wounds.

Up-to-date vaccine delivery systems: robust immunity elicited by multifarious nanomaterials upon administration through diverse routes.

In this review, we summarize the recent design strategies (2015-present) of nanomaterial-based vaccine delivery systems via multiple routes to induce robust protective immunity. The selected topics are focused on the novel design strategies of nanomaterial carriers for vaccine delivery. Inspired by recent advances, we also briefly introduce the emerging administration routes that may give rise to synergistic immune effects with advanced delivery systems. Ultimately, we present the existing challenges and survey the prospective development of various nanoparticle vaccine delivery systems.

Dual-Cross-Linked Supramolecular Polysiloxanes for Mechanically Tunable, Damage-Healable and Oil-Repellent Polymeric Coatings.

Polymeric coatings that show tunable mechanical strength, healing ability of mechanical damage, and proper liquid repellency will be promising in various areas across life and industry. However, the exploitation of such coating materials is largely limited by their molecular design. In this work, polymeric coatings with ion-controlled mechanics and coloration and damage-healing and oil-sliding properties have been demonstrated based on a supramolecular design of dual-cross-linked polysiloxanes. The coating color and mechanical properties can be adjusted by coordinative metal ions with various metal-ligand binding abilities. Dense and dynamic hydrogen bonds and coordination bonds lead to the ready healing ability and high durability of the coating. The extreme smoothness of the flat silicone coating facilitates not only the sliding of impinging oil but also the restoration of topological integrity from mechanical damage. The coating can be selectively patterned and applied to large-scale substrates by diverse coating operations, making it feasible for versatile applications.

Facile preparation of carbon-dot-supported nanoflowers for efficient photothermal therapy of cancer cells.

Herein, novel self-assembled red-emissive C-dots@Au nanoflowers were developed, and they demonstrated efficient photothermal properties under 750 nm laser irradiation. Moreover, C-dots@Au nanoflowers showed the ability of simultaneous photoacoustic and fluorescence imaging. Our study may provide a novel strategy for the efficient phototherapy of cancer cells based on C-dots.