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Bilayer hydrogels encoded with smart functions have emerged as promising soft materials for engineered biological tissues and human-machine interfaces, due to the versatility and flexibility in designing their mechanical and chemical properties. However, conventional fabrication strategies often require multiple complicated steps to create an anisotropic bilayer structure with poor interfaces, which significantly limit the scope of bilayer hydrogel applications. Here, we reported a general, one-pot, macrophase separation strategy to fabricate a family of bilayer hydrogels made of vinyl and styryl monomers with a seamless interface and a controllable layer separation efficiency (20–99%). The working principle of a macrophase separation strategy allows for the decoupling of the two gelation processes to form distinct vinyl- and styryl-enriched layers by manipulating competitive polymerization reactions between vinyl and styryl monomers. This work presents a straightforward approach and a diverse range of radical monomers, which can be utilized to create next-generation bilayer hydrogels, beyond a few available today. 

Development of highly stretchable and sensitive soft strain sensors is of great importance for broad applications in artificial intelligence, wearable devices, and soft robotics, but it proved to be a profound challenge to integrate the two seemingly opposite properties of high stretchability and sensitivity into a single material. Herein, we designed and synthesized a new fully polymeric conductive hydrogel with an interpenetrating polymer network (IPN) structure made of conductive PEDOT:PSS polymers and zwitterionic poly(HEAA- co -SBAA) polymers to achieve a combination of high mechanical, biocompatible, and sensing properties. The presence of hydrogen bonding, electrostatic interactions, and IPN structures enabled poly(HEAA- co -SBAA)/PEDOT:PSS hydrogels to achieve an ultra-high stretchability of 4000–5000%, a tensile strength of ∼0.5 MPa, a rapid mechanical recovery of 70–80% within 5 min, fast self-healing in 3 min, and a strong surface adhesion of ∼1700 J m −2 on different hard and soft substrates. Moreover, the integration of zwitterionic polySBAA and conductive PEDOT:PSS facilitated charge transfer via optimal conductive pathways. Due to the unique combination of superior stretchable, self-adhesive, and conductive properties, the hydrogels were further designed into strain sensors with high sensing stability and robustness for rapidly and accurately detecting subtle strain- and pressure-induced deformation and human motions. Moreover, an in-house mechanosensing platform provides a new tool to real-time explore the changes and relationship between network structures, tensile stress, and electronic resistance. This new fully polymeric hydrogel strain sensor, without any conductive fillers, holds great promise for broad human-machine interface applications. 

Stimuli-responsive hydrogel strain sensors that synergize the advantages of both soft-wet hydrogels and smart functional materials have attracted rapidly increasing interest for exploring the opportunities from material design principles to emerging applications in electronic skins, health monitors, and human–machine interfaces. Stimuli-responsive hydrogel strain sensors possess smart and on-demand ability to specifically recognize various external stimuli and convert them into strain-induced mechanical, thermal, optical, and electrical signals. This review presents an up-to-date summary over the past five years on hydrogel strain sensors from different aspects, including material designs, gelation/fabrication methods, stimuli-responsive principles, and sensing performance. Hydrogel strain sensors are classified into five major categories based on the nature of the stimuli, and representative examples from each category are carefully selected and discussed in terms of structures, response mechanisms, and potential medical applications. Finally, current challenges and future perspectives of hydrogel strain sensors are tentatively proposed to stimulate more and better research in this emerging field. 

The development of smart materials and surfaces with multiple antibacterial actions is of great importance for both fundamental research and practical applications, but this has proved to be extremely challenging. In this work, we proposed to integrate salt-responsive polyDVBAPS (poly(3-(dimethyl(4-vinylbenzyl) ammonio)propyl sulfonate)), antifouling polyHEAA (poly( N -hydroxyethyl acrylamide)), and bactericidal TCS (triclosan) into single surfaces by polymerizing and grafting polyDVBAPS and polyHEAA onto the substrate in a different way to form two types of polyDVBAPS/poly(HEAA- g -TCS) and poly(DVBAPS- b -HEAA- g -TCS) brushes with different hierarchical structures, as confirmed by X-ray photoelectron spectroscopy (XPS), atom force microscopy (AFM), and ellipsometry. Both types of polymer brushes demonstrated their tri-functional antibacterial activity to resist bacterial attachment by polyHEAA, to release ∼90% of dead bacteria from the surface by polyDVBAPS, and to kill ∼90% of bacteria on the surface by TCS. Comparative studies also showed that removal of any component from polyDVBAPS/poly(HEAA- g -TCS) and poly(DVBAPS- b -HEAA- g -TCS) compromised the overall antibacterial performance, further supporting a synergistic effect of the three compatible components. More importantly, the presence of salt-responsive polyDVBAPS allowed both brushes to regenerate with almost unaffected antibacterial capacity for reuse in multiple kill-and-release cycles. The tri-functional antibacterial surfaces present a promising design strategy for further developing next-generation antibacterial materials and coatings for antibacterial applications. 

Shape adaptable hydrogel actuators, capable for changing their shapes in response to single or multiple thermo/other external stimulus, are considered as new emerging smart materials for a broad range of fundamental/industrial research and applications. This review mainly focuses on the recent progress (particularly over the past 5 years) on such thermo-responsive hydrogel actuators. Recent fundamental advances and engineering applications in materials design/synthesis/characterization, distinct actuation mechanisms, and intriguing examples of these hydrogel actuators of single or dual stimuli are selectively presented. Specific or general design principles for thermo-induced hydrogel actuators are also provided to better illustrate the structure-property relationship. In the end, we offer some personal perspectives on current major challenges and future research directions in this promising field. Overall, this review discusses current status, progress, and challenges of hydrogel actuators, and hopefully will motivate researchers from different fields to explore all the potentials of hydrogel actuators. 

Abstract Development of a universal and stable surface coating, irrespective of surface chemistry or material characteristics, is highly desirable but has proved to be extremely challenging. Conventional coating strategies including the commonly used catechol surface coating are limited to either a certain type of substrates or weak and unreliable surface bonding. Here, a simple, robust, and universal surface coating method capable for attaching any stimuli‐responsive glycidyl methacrylate (GMA)‐based copolymer, consisting of one surface‐adhesive moiety of epoxy groups and one stimuli‐responsive moiety, to any type of hydrophobic and hydrophilic surfaces via a one‐step ring‐opening reaction is proposed and demonstrated. The resultant GMA‐based copolymers are not only strongly adhered on different substrates (e.g., silicon, polypropylene, polyvinyl chloride, indium tin oxide, polyethylene terephthalate, aluminum, glass, polydimethylsiloxane, and even polyvinylidene fluoride with low surface energy), but also are possessed distinct thermal‐, pH‐, and salt‐responsive functions of bacterial killing, bacterial releasing, tunable multicolor fluorescence emission, and heavy metal detection. This coating method is also compatible with the directional quaternization of GMA‐based copolymers for further improving surface adhesion and functionality. This study provides a simple yet universal coating method to solve the long‐standing challenge of robust integration of stimuli‐responsive polymers with strong adhesion between various polymers and substrates.