Recent advances in soft materials and system integration technologies have provided a unique opportunity to design various types of wearable flexible hybrid electronics (WFHE) for advanced human healthcare and human-machine interfaces. The hybrid integration of soft and biocompatible materials with miniaturized wireless wearable systems is undoubtedly an attractive prospect in the sense that the successful device performance requires high degrees of mechanical flexibility, sensing capability, and user-friendly simplicity. Here, the most up-to-date materials, sensors, and system-packaging technologies to develop advanced WFHE are provided. Details of mechanical, electrical, physicochemical, and biocompatible properties are discussed with integrated sensor applications in healthcare, energy, and environment. In addition, limitations of the current materials are discussed, as well as key challenges and the future direction of WFHE. Collectively, an all-inclusive review of the newly developed WFHE along with a summary of imperative requirements of material properties, sensor capabilities, electronics performance, and skin integrations is provided.

Advanced Soft Materials, Sensor Integrations, and Applications of Wearable Flexible Hybrid Electronics in Healthcare, Energy, and Environment.

Mussel-inspired chemistry, owing to its unique and versatile functions to manipulate dynamic molecular-scale interactions, has emerged as a powerful tool for the rational design and synthesis of new hydrogels. In particular, possessing a myriad of unique advantages that are otherwise impossible by conventional counterparts, mussel-inspired hydrogels have been widely explored in numerous fields such as biomedical engineering, soft electronics and actuators, and wearable sensors. Despite great excitement and vigor, a comprehensive and timely review on this emerging topic is missing. In this review, we discuss (1) the fundamental interaction mechanisms underpinning the spectacular wet adhesion in natural mussels and mussel-inspired materials; (2) the key routes to engineering hydrogels by leveraging on the interactions of mussel-inspired building blocks; (3) the emerging applications of mussel-inspired hydrogels, especially in the areas of flexible electronics and biomedical engineering; (4) the future perspectives and unsolved challenges of this multidisciplinary field. We envision that this review will provide an insightful perspective to stimulate new thinking and innovation in the development of next-generation hydrogels and beyond.

Mussel-inspired hydrogels: from design principles to promising applications

Copper (Cu(II)) is a very toxic heavy metal that even at low concentration can affect living organisms. Therefore, designing effective materials with high selectivity and cost-efficiency is essential for the control capturing of toxic Cu(II) ions. This study was developed a ligand based composite material for simultaneous Cu(II) detection and removal from wastewater samples. The composite material was fabricated based on the ligand anchoring onto the mesoporous silica by direct coating approach. The application of Cu(II) detection and adsorption was measured at neutral pH region with exhibition of significant color visualization. The experiment conditions were optimized based on contact time, solution acidity, initial Cu(II) concentration and pH value and diverse metal salt concentrations. The results were revealed that the composite material was not affected with the existing foreign ions and the signal intensity was observed only toward the Cu(II) ion. The composite material was able to detected the low level Cu(II) ion as the detection limit was 0.25 μg/L and the adsorption of highest removal capacity was 171.33 mg/g. In addition, the diverse ions were not reduced the Cu(II) ion adsorption significantly, and the composite material has approximately no adsorption capacity for other ions at this pH. The elution of Cu(II) ions from the saturated composite material was desorbed successfully with 0.20 M HCl. The regenerated adsorbent that remained maintained the high selectivity to Cu(II) ions and exhibited almost the same sorption capacity as that of the original adsorbent. However, the sorption efficiency slightly decreased after ten cycles. Therefore, the proposed material offered a cost-effective material and may be considered a viable alternative for effectively toxic Cu(II) ion capturing from water samples without the need for sophisticated instrument.

Novel ligand functionalized composite material for efficient copper(II) capturing from wastewater sample

Stretchable electronics, which can retain their functions under stretching, have attracted great interest in recent decades. Elastic substrates, which bear the applied strain and regulate the strain distribution in circuits, are indispensable components in stretchable electronics. Moreover, the self-healing property of the substrate is a premise to endow stretchable electronics with the same characteristics, so the device may recover from failure resulting from large and frequent deformations. Therefore, the properties of the elastic substrate are crucial to the overall performance of stretchable devices. Poly(dimethylsiloxane) (PDMS) is widely used as the substrate material for stretchable electronics, not only because of its advantages, which include stable chemical properties, good thermal stability, transparency, and biological compatibility, but also because of its capability of attaining designer functionalities via surface modification and bulk property tailoring. Herein, the strategies for fabricating stretchable electronics on PDMS substrates are summarized, and the influence of the physical and chemical properties of PDMS, including surface chemical status, physical modulus, geometric structures, and self-healing properties, on the performance of stretchable electronics is discussed. Finally, the challenges and future opportunities of stretchable electronics based on PDMS substrates are considered.

Stretchable Electronics Based on PDMS Substrates.

Treatment of wounds in special areas is challenging due to inevitable movements and difficult fixation. Common cotton gauze suffers from incomplete joint surface coverage, confinement of joint movement, lack of antibacterial function, and frequent replacements. Hydrogels have been considered as good candidates for wound dressing because of their good flexibility and biocompatibility. Nevertheless, the adhesive, mechanical, and antibacterial properties of conventional hydrogels are not satisfactory. Herein, cationic polyelectrolyte brushes grafted from bacterial cellulose (BC) nanofibers are introduced into polydopamine/polyacrylamide hydrogels. The 1D polymer brushes have rigid BC backbones to enhance mechanical property of hydrogels, realizing high tensile strength (21-51 kPa), large tensile strain (899-1047%), and ideal compressive property. Positively charged quaternary ammonium groups of tethered polymer brushes provide long-lasting antibacterial property to hydrogels and promote crawling and proliferation of negatively charged epidermis cells. Moreover, the hydrogels are rich in catechol groups and capable of adhering to various surfaces, meeting adhesive demand of large movement for special areas. With the above merits, the hydrogels demonstrate less inflammatory response and faster healing speed for in vivo wound healing on rats. Therefore, the multifunctional hydrogels show stable covering, little displacement, long-lasting antibacteria, and fast wound healing, demonstrating promise in wound dressing.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/advs.202003627

Highly Stretchable, Adhesive, Biocompatible, and Antibacterial Hydrogel Dressings for Wound Healing

Herein, we demonstrate a ternary ionic hydrogel sensor consisting of tannic acid, sodium alginate, and covalent cross-linked polyacrylamide as skin-mountable and wearable sensors. Based on the multiple weak H-bonds and synergistic effects between the three components, the as-prepared hybrid hydrogel exhibits ultrastretchability with high elasticity, good self-healing, excellent conformability, and high self-adhesiveness to diverse substrates both in air and underwater. More importantly, the ternary hydrogel exhibits high strain sensitivity especially under subtle strains with a gauge factor of 2.0, which is close to the theoretical value of the ionic hydrogel sensors; an extremely large workable range of strain (0.05–2100%); and a low operating voltage 0.07 V. Consequently, the sensor demonstrates superior sensing performance for real-time monitoring of the large and subtle human motions, including limb motions, swallowing, smiling, and wrist pulse. Therefore, it is believed that the STP hydrogel has grea...

Multiple Weak H-Bonds Lead to Highly Sensitive, Stretchable, Self-Adhesive, and Self-Healing Ionic Sensors.

Nanofiber membranes from natural alginate are ideal adsorption materials for removing cationic dyes in solution, yet the regulations to their adsorption and desorption properties are of great challenges. In this research, gelatin/calcium alginate (GA) composite nanofiber membranes were successfully prepared via electrospinning to resolve these issues. The structural changes of composite membranes induced by the gelatin addition were confirmed by SEM, FT-IR and BET analysis. The enhanced mechanical strength of GA membranes disclosed the strong interactions between gelatin and alginate chains. Taking methylene blue (MB) as the model cationic dye, it was found the resultant composites could slow down the adsorption rate and obviously improve the adsorption evenness without apparent influences on its adsorption capacity. Moreover, the gelatin modification would generate better reusability for the composite membranes during a serial of adsorption and desorption cycles for strong electrostatic repulsions induced by protonated amino groups in gelatin chains. This effective composite strategy would pave the way for the development of natural alginate to the next generation high-performance adsorbent for cationic dyes.

Pengfei Qi

Papers

Multiple Weak H-Bonds Lead to Highly Sensitive, Stretchable, Self-Adhesive, and Self-Healing Ionic Sensors.

Gelatin/alginate composite nanofiber membranes for effective and even adsorption of cationic dyes

Design of injectable agar/NaCl/polyacrylamide ionic hydrogels for high performance strain sensors.