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Bioelectronic devices made of soft elastic materials exhibit motion-adaptive properties suitable for brain-machine interfaces and for investigating complex neural circuits. While two-dimensional microfabrication strategies enable miniaturizing devices to access delicate nerve structures, creating 3D architecture for expansive implementation requires more accessible and scalable manufacturing approaches. Here we present a fabrication strategy through the control of metamorphic polymers’ amorphous-crystalline transition (COMPACT), for hydrogel bioelectronics with miniaturized fiber shape and multifunctional interrogation of neural circuits. By introducing multiple cross-linkers, acidification treatment, and oriented polymeric crystalline growth under deformation, we observed about an 80% diameter decrease in chemically cross-linked polyvinyl alcohol (PVA) hydrogel fibers, stably maintained in a fully hydrated state. We revealed that the addition of cross-linkers and acidification facilitated the oriented polymetric crystalline growth under mechanical stretching, which contributed to the desired hydrogel fiber diameter decrease. Our approach enabled the control of hydrogels’ properties, including refractive index (RI 1.37-1.40 at 480 nm), light transmission (> 96%), stretchability (95% - 111%), and elastic modulus (10-63 MPa). To exploit these properties, we fabricated step-index hydrogel optical probes with contrasting RIs and applied them in optogenetics and photometric recordings in the mouse brain region of the ventral tegmental area (VTA) with concurrent social behavioral assessment. To extend COMPACT hydrogel multifunctional scaffolds to assimilate conductive nanomaterials and integrate multiple components of optical waveguide and electrodes, we developed carbon nanotubes (CNTs)-PVA hydrogel microelectrodes for hindlimb muscle electromyographic and brain electrophysiological recordings of light-triggered neural activities in transgenic mice expressing Channelrhodopsin-2 (ChR2).

Intense surface eruptions are observed along the curved surface of a confined cylindrical film of hydrogel subject to laser-induced converging-diverging shock loading. Detailed numerical simulations are used to identify the dominant mechanisms causing mechanical instability. The mechanisms that produce surface instability are found to be fundamentally different from both acoustic parametric instability and shock-driven Richtmyer-Meshkov instability. The time scale of observed and simulated eruption formation is much larger than that of a single shock reflection, in stark contrast to previously studied shock-driven instabilities. Moreover, surface undulations are only found along external, as opposed to internal, soft solid boundaries. Specifically, classic bubble surface instability mechanisms do not occur in our experiments and here we comment only on the new surface undulations found along the outer boundary of solid hydrogel cylinders. Our findings indicate a new class of impulsively excited surface instability that is driven by cycles of internal shock reflections.

Neuroprosthetic hands are typically heavy (over 400 g) and expensive (more than US$10,000), and lack the compliance and tactile feedback of human hands. Here, we report the design, fabrication and performance of a soft, low-cost and lightweight (292 g) neuroprosthetic hand that provides simultaneous myoelectric control and tactile feedback. The neuroprosthesis has six active degrees of freedom under pneumatic actuation, can be controlled through the input from four electromyography sensors that measure surface signals from residual forearm muscles, and integrates five elastomeric capacitive sensors on the fingertips to measure touch pressure so as to enable tactile feedback by eliciting electrical stimulation on the skin of the residual limb. In a set of standardized tests performed by two individuals with transradial amputations, we show that the soft neuroprosthetic hand outperforms a conventional rigid neuroprosthetic hand in speed and dexterity. We also show that one individual with a transradial amputation wearing the soft neuroprosthetic hand can regain primitive touch sensation and real-time closed-loop control. A soft and lightweight neuroprosthetic hand that offers simultaneous myoelectric control and tactile feedback outperformed a conventional rigid neuroprosthetic hand in speed and dexterity.

Summary Nanofibrous hydrogels are pervasive in animal and plant bodies and have been widely seen in engineering applications. Electrospinning is one of the most widely used methods for the fabrication of nanofibrous hydrogels. Whereas the biological nanofibrous hydrogels can maintain high strength and high toughness under multiple cycles of mechanical loads, such fatigue-resistant properties have not been achieved in electrospun nanofibrous hydrogels. Here, we report a bioinspired design of strong and fatigue-resistant nanofibrous hydrogels that can closely mimic the bouligand structure of the natural hydrogel in the lobster underbelly. The resultant nanofibrous hydrogel can reach high nominal strength up to 8.4 MPa and high fatigue threshold up to 770 J/m2. We further demonstrate the superior impact resistance of the bioinspired bouligand-type nanofibrous hydrogel with specific penetration energy of 40 kJ/kg. We show that it is critical to weld the interfaces between nanofibers and introduce intrinsically high-energy phases (nanocrystalline domains) into nanofibers.

Soft yet tough materials are ubiquitous in nature and everyday life. The ratio between fracture toughness and intrinsic fracture energy of a soft material defines its toughness enhancement. Soft materials' toughness enhancement has been long attributed to their bulk stress-stretch hysteresis induced by dissipation mechanisms such as Mullins effect and viscoelasticity. With a combination of experiments and theory, here we show that the bulk dissipation mechanisms significantly underestimate the toughness enhancement of soft tough materials. We propose a new mechanism and scaling law to account for extreme toughening of diverse soft materials. We show that the toughness enhancement of soft materials relies on both bulk hysteretic dissipation, and near-crack dissipation due to mechanisms such as polymer-chain entanglement. Unlike the bulk hysteretic dissipation, the near-crack dissipation does not necessarily induce large stress-stretch hysteresis of the bulk material. The extreme toughening mechanism can be potentially universally applied to various soft tough materials, ranging from double-network hydrogels, interpenetrating-network hydrogels, entangled-network hydrogels and slide-ring hydrogels, to unfilled and filled rubbers.

The adhesion of soft connective tissues (tendons, ligaments, and cartilages) on bones in many animals can maintain high toughness (∽800 J m−2) over millions of cycles of mechanical loads. Such fatigue-resistant adhesion has not been achieved between synthetic hydrogels and engineering materials, but is highly desirable for diverse applications such as artificial cartilages and tendons, robust antifouling coatings, and hydrogel robots. Inspired by the nanostructured interfaces between tendons/ligaments/cartilages and bones, we report that bonding ordered nanocrystalline domains of synthetic hydrogels on engineering materials can give a fatigue-resistant adhesion with an interfacial fatigue threshold of 800 J m−2, because the fatigue-crack propagation at the interface requires a higher energy to fracture the ordered nanostructures than amorphous polymer chains. Our method enables fatigue-resistant hydrogel coatings on diverse engineering materials with complex geometries. We further demonstrate that the fatigue-resistant hydrogel coatings exhibit low friction and low wear against natural cartilages., Fatigue-resistant adhesion is of interest for a range of applications, but has been limited in synthetic hydrogels. Here, the authors report on a synthetic hydrogel with ordered nanocrystalline domains resulting in high fatigue-resistant adhesion and demonstrate the coating of different surfaces.

Heat-conducting polymers provide a new opportunity to tackle thermal management challenges in advanced technologies such as wearable electronics and soft robotics. One strategy to enhance heat conduction in amorphous polymers has been tuning their intermolecular interactions. These intermolecular forces are often static in nature as the participating molecules are anchored on the polymer chains. In this work, using hydrogel as a model system, we demonstrate how dynamic intermolecular forces, which break and re-form constantly, can also enhance thermal transport. Utilizing calorimetric and spectroscopic measurements, we show that this arises from the hydrogen bonds formed between water and nearby polymer chains, which enhances the inter-chain heat transfer efficiency. This mechanism may potentially allow the design of heat-conducting polymers with self-healing or adaptability functionalities.

Sporopollenin is a mechanically robust and chemically inert biopolymer that constitutes the outer protective exine layer of plant spores and pollen grains. Recent investigation of the molecular structure of pine sporopollenin revealed unique monomeric units and inter-unit linkages distinct from other previously known biopolymers, which could be harnessed for new material design. Here, we report the bioinspired synthesis of a series of sporopollenin analogues. This exercise confirms large portions of the previously proposed pine sporopollenin structural model, while the measured chemical, thermal, and mechanical properties of the synthetic sporopollenins indicate favorable attributes of a new kind of robust material. This study explores a new design framework of robust materials inspired by natural sporopollenins, and provides insights and reagents for future elucidation and engineering of sporopollenin biosynthesis in plants.

Recent experiments on hydrogels subjected to large elongations have shown elastic instabilities resulting in the formation of geometrically intricate fringe and fingering deformation patterns. In this paper, we present a robust numerical framework addressing the challenges that emerge in the simulation of this complex material response from the onset of instability to the post-bifurcation behavior. We observe that the numerical difficulties stem from the non-convexity of the strain energy density in the near-incompressible, large-deformation regime, which is responsible for the coexistence of multiple equilibrium paths with vastly-different, sinuous deformation patterns immediately after bifurcation. We show that these numerical challenges can be overcome by using sufficiently-high order of interpolation in the finite element approximation, an arc-length-based nonlinear solution procedure that follows the entire equilibrium path of the system, and an implementation enabling parallel, large-scale simulations. The resulting computational approach provides the ability to conduct highly-resolved, truly quasi-static simulations of complex elastic instabilities. We present numerical results illustrating the ability of the path-following approach to describe the full evolution of fringe and fingering instabilities observed experimentally in recent experiments of confined cylindrical specimens of soft hydrogels subject to tension. Importantly, we observe that the robustness of the static solution procedure enables complete access to the multiplicity of solutions occurring immediately after the onset of bifurcation, as well as to the settled post-bifurcation states.

In many developmental and pathological processes, including cellular migration during normal development and invasion in cancer metastasis, cells are required to withstand severe deformations. The structural integrity of eukaryotic cells under small deformations has been known to depend on the cytoskeleton including actin filaments (F-actin), microtubules (MT), and intermediate filaments (IFs). However, it remains unclear how cells resist severe deformations since both F-actin and microtubules yield or disassemble under moderate strains. Using vimentin containing IFs (VIFs) as a model for studying the large family of IF proteins, we demonstrate that they dominate cytoplasmic mechanics and maintain cell viability at large deformations. Our results show that cytoskeletal VIFs form a stretchable, hyperelastic network in living cells. This network works synergistically with other cytoplasmic components, substantially enhancing the strength, stretchability, resilience, and toughness of cells. Moreover, we find the hyperelastic VIF network, together with other quickly recoverable cytoskeletal components, forms a mechanically robust structure which can mechanically recover after damage.

Natural microbial sensing circuits can be rewired into new gene networks to build living sensors that detect and respond to disease-associated biomolecules. However, synthetic living sensors, once ingested, are cleared from the gastrointestinal (GI) tract within 48 hours; retaining devices in the intestinal lumen is prone to intestinal blockage or device migration. To localize synthetic microbes and safely extend their residence in the GI tract for health monitoring and sustained drug release, an ingestible magnetic hydrogel carrier is developed to transport diagnostic microbes to specific intestinal sites. The magnetic living hydrogel is localized and retained by attaching a magnet to the abdominal skin, resisting the peristaltic waves in the intestine. The device retention is validated in a human intestinal phantom and an in vivo rodent model, showing that the ingestible hydrogel maintains the integrated living bacteria for up to seven days, which allows the detection of heme for GI bleeding in the harsh environment of the gut. The retention of microelectronics is also demonstrated by incorporating a temperature sensor into the magnetic hydrogel carrier.

Hydrogels are polymer networks infiltrated with water. Many biological hydrogels in animal bodies such as muscles, heart valves, cartilages, and tendons possess extreme mechanical properties including being extremely tough, strong, resilient, adhesive, and fatigue-resistant. These mechanical properties are also critical for hydrogels' diverse applications ranging from drug delivery, tissue engineering, medical implants, wound dressings, and contact lenses to sensors, actuators, electronic devices, optical devices, batteries, water harvesters, and soft robots. Whereas numerous hydrogels have been developed over the last few decades, a set of general principles that can rationally guide the design of hydrogels using different materials and fabrication methods for various applications remain a central need in the field of soft materials. This review is aimed at synergistically reporting: (i) general design principles for hydrogels to achieve extreme mechanical and physical properties, (ii) implementation strategies for the design principles using unconventional polymer networks, and (iii) future directions for the orthogonal design of hydrogels to achieve multiple combined mechanical, physical, chemical, and biological properties. Because these design principles and implementation strategies are based on generic polymer networks, they are also applicable to other soft materials including elastomers and organogels. Overall, the review will not only provide comprehensive and systematic guidelines on the rational design of soft materials, but also provoke interdisciplinary discussions on a fundamental question: why does nature select soft materials with unconventional polymer networks to constitute the major parts of animal bodies?

Entanglement of polymer chains is ubiquitous in elastomers, gels, and biological tissues. While the effects of chain entanglement on elasticity and viscoelasticity of polymer networks have been intensively studied, it remains elusive how chain entanglement affects fracture and fatigue of polymer networks. In this paper, using polyacrylamide hydrogels as a model material, we systematically compare fracture toughness and fatigue threshold of polymer networks with various levels of chain entanglement. We find that the fracture toughness and fatigue threshold of an unentangled polymer network are almost the same, although the unentangled polymer network still contains non-ideal features including topological defects (i.e., dangling chains and cyclic loops) and structural heterogeneity (i.e., non-uniform chain lengths and non-uniform functionalities). In contrast, the fracture toughness of an entangled polymer network can be over ten times (up to 16 times) higher than its fatigue threshold, indicating substantial toughness enhancement due to chain entanglement. Different from the conventional toughness enhancement due to bulk dissipation of polymer networks, the toughness enhancement by chain entanglement requires low stress-stretch hysteresis (, 23 pages, 7 figures, submitted to Extreme Mechanics Letter

Polymer networks are pervasive in biological organisms and engineering materials. Topological defects such as cyclic loops and dangling chains are ubiquitous in polymer networks. While fracture is a dominant mechanism for mechanical failures of polymer networks, existing models for fracture of polymer networks neglect the presence of topological defects. Here, we report a defect-network fracture model that accounts for the impact of various types of topological defects on fracture of polymer networks. We show that the fracture energy of polymer networks should account for the energy from multiple layers of polymer chains adjacent to the crack. We further show that the presence of topological defects tends to toughen a polymer network by increasing the effective chain length, yet to weaken the polymer network by introducing inactive polymer chains. Such competing effects can either increase or decrease the overall intrinsic fracture energy of the polymer network, depending on the types and densities of topological defects. Our model provides theoretical explanations for the experimental data on the intrinsic fracture energy of polymer networks with various types and densities of topological defects.

Mainly composed of electrical motors and sophisticated mechanical components, existing neuroprosthetic hands1,2 are typically heavy (>400 g) and expensive (>USD 10,000), and they lack the compliance and tactile feedback of human hands. These limitations hamper neuroprosthetic hands’ innovation and broad utility for amputees3-5. Here we report the design, fabrication and applications of a lightweight (292 g) and potentially low-cost (component cost below USD 500) soft neuroprosthetic hand with simultaneous myoelectric control and tactile feedback. The soft neuroprosthetic hand consists of five soft fingers and a palm to give six active degrees of freedom under pneumatic actuation, four electromyography sensors that measure the surface electromyogram signals to control the hand to deliver four common grasp types, and five hydrogel-elastomer capacitive sensors on the fingertips that measure the touch pressure and elicit electrical stimulation on the skin of the residual limb. The soft finger is made of a fiber-reinforced elastomeric structure embedded with rigid segments to mimic the soft-joint/rigid-bone anatomy of the human finger. We use a set of standardized tests6 to compare the speed and dexterity of the soft neuroprosthetic hand and a conventional rigid neuroprosthetic hand7 on two transradial amputees. The soft neuroprosthetic hand gives overall superior performances to the rigid hand. We further demonstrate that one transradial amputee wearing the soft neuroprosthetic hand can regain the versatile hand functions with primitive touch sensation and real-time closed-loop control in daily activities such as handling tools, eating, shaking hands, petting animals, and recognizing touch pressure. This work not only represents a new paradigm for designing soft neuroprosthetic devices but also opens an avenue to widespread applications of lightweight, low-cost, and compliant hand replacements for amputees.

© 2020 Elsevier Ltd As polymer networks infiltrated with water, hydrogels constitute the major components of the human body; and hydrogels have been widely used in applications that closely interact with biological organisms, such as tissue engineering, drug delivery, and biological research. More recently, owing to their superior softness, wetness, responsiveness, biocompatibility, and bioactivity, hydrogels are being intensively investigated for versatile functions in devices and machines including sensors, actuators, coatings, optics, electronics, and water harvesters. A nascent field named hydrogel machines rapidly evolves, exploiting hydrogels as key components for devices and machines. While there are reviews on individual categories of hydrogel machines in literature, a comprehensive discussion on various categories of hydrogel machines that systematically correlate hydrogels’ properties and machines’ functions is still missing in the field. This review is aimed to provide such a panoramic overview. We first classify various hydrogel machines into a number of categories according to their applications. For each category, we discuss (i) the working principles of the hydrogel machines, (ii) the specific properties of hydrogels that enable the key functions of the machines, and (iii) challenges faced by hydrogel machines and recent developments to address them. The field of hydrogel machines will not only translate fundamental understanding of hydrogels into new applications, but also shift the paradigm in machine design by integrating hydrogels that can potentially minimize physical and physiological mismatches with biological organisms.

Soft materials have enabled diverse modern technologies, but their practical deployment is usually limited by their mechanical failures. Fracture and fatigue of polymer networks are two important causes of mechanical failures of soft materials. A soft material fails by fracture when a monotonic load reaches its fracture toughness or fails by fatigue when a cyclic load reaches its fatigue threshold. The fracture toughness is usually much higher than the fatigue threshold for randomly crosslinked elastomers and gels. While fracture and fatigue have been extensively studied in randomly crosslinked elastomers and gels, they have not been comparatively studied in polymer networks with well-controlled architectures and defects. This work systematically studies the fracture and fatigue of ideal polymer networks with controlled densities of dangling-chain defects. We show that the fracture toughness and fatigue threshold of an ideal polymer network almost without defects are the same. After introducing a low density of dangling-chain defects into the ideal polymer network, its fracture toughness and fatigue threshold still maintain approximately the same. The fracture toughness of the ideal polymer network is also independent of the loading rate. We further use the recently developed defect-network model to explain the fatigue threshold (i.e., intrinsic fracture energy) of ideal polymer networks with controlled densities of dangling-chain defects.

Nature builds biological materials from limited ingredients, however, with unparalleled mechanical performances compared to artificial materials, by harnessing inherent structures across multi-length-scales. In contrast, synthetic material design overwhelmingly focuses on developing new compounds, and fails to reproduce the mechanical properties of natural counterparts, such as fatigue resistance. Here, a simple yet general strategy to engineer conventional hydrogels with a more than 100-fold increase in fatigue thresholds is reported. This strategy is proven to be universally applicable to various species of hydrogel materials, including polysaccharides (i.e., alginate, cellulose), proteins (i.e., gelatin), synthetic polymers (i.e., poly(vinyl alcohol)s), as well as corresponding polymer composites. These fatigue-resistant hydrogels exhibit a record-high fatigue threshold over most synthetic soft materials, making them low-cost, high-performance, and durable alternatives to soft materials used in those circumstances including robotics, artificial muscles, etc.

Under tension, confined elastic layers can exhibit various modes of mechanical instabilities, including cavitation, fingering and fringe instabilities. While the cavitation has been extensively studied, the fingering and fringe instabilities have not been well understood, and the relations and interactions of these instabilities have not been explored yet. In this paper, we systematically study the formation, transition, interaction and co-existence of mechanical instabilities in confined elastic layers under tension. Through combined experimental, numerical and theoretical analysis, we find that the mode of instability is determined by both geometry and mechanical properties of the elastic layer through two non-dimensional parameters: layer's lateral dimension over its thickness and elastocapillary length over the defect size. A phase diagram is calculated to quantitatively predict the occurrence of any mode of instability. We further show cavitation instability and fingering instability can coexist and interact with each other in one elastic layer. The current work can help the design of robust adhesives by rationally harnessing the desired mode of instabilities while suppressing the other modes.

As polymer networks infiltrated with water, hydrogels are major constituents of animal and plant bodies and have diverse engineering applications. While natural hydrogels can robustly adhere to other biological materials, such as bonding of tendons and cartilage on bones and adhesive plaques of mussels, it is challenging to achieve such tough adhesions between synthetic hydrogels and engineering materials. Recent experiments show that chemically anchoring long-chain polymer networks of tough synthetic hydrogels on solid surfaces create adhesions tougher than their natural counterparts, but the underlying mechanism has not been well understood. It is also challenging to tune systematically the adhesion of hydrogels on solids. Here, we provide a quantitative understanding of the mechanism for tough adhesions of hydrogels on solid materials via a combination of experiments, theory, and numerical simulations. Using a coupled cohesive-zone and Mullins-effect model validated by experiments, we reveal the interplays of intrinsic work of adhesion, interfacial strength, and energy dissipation in bulk hydrogels in order to achieve tough adhesions. We further show that hydrogel adhesion can be systematically tuned by tailoring the hydrogel geometry and silanization time of solid substrates, corresponding to the control of energy dissipation zone and intrinsic work of adhesion, respectively. The current work further provides a theoretical foundation for rational design of future biocompatible and underwater adhesives., United States. Office of Naval Research (N00014-14-1-0528), National Science Foundation (U.S.) (CMMI-1253495), National Institutes of Health (U.S.) (UH3TR000505)

We present a large deformation viscoelasticity model for recently synthesized double network hydrogels which consist of a covalently-crosslinked polyacrylamide network with long chains, and an ionically-crosslinked alginate network with short chains. Such double-network gels are highly stretchable and at the same time tough, because when stretched the crosslinks in the ionically-crosslinked alginate network rupture which results in distributed internal microdamage which dissipates a substantial amount of energy, while the configurational entropy of the covalently-crosslinked polyacrylamide network allows the gel to return to its original configuration after deformation. In addition to the large hysteresis during loading and unloading, these double network hydrogels also exhibit a substantial rate-sensitive response during loading, but exhibit almost no rate-sensitivity during unloading. These features of large hysteresis and asymmetric rate-sensitivity are quite different from the response of conventional hydrogels. We limit our attention to modeling the complex viscoelastic response of such hydrogels under isothermal conditions. Our model is restricted in the sense that we have limited our attention to conditions under which one might neglect any diffusion of the water in the hydrogel — as might occur when the gel has a uniform initial value of the concentration of water, and the mobility of the water molecules in the gel is low relative to the time scale of the mechanical deformation. We also do not attempt to model the final fracture of such double-network hydrogels.

Living systems, such as bacteria, yeasts, and mammalian cells, can be genetically programmed with synthetic circuits that execute sensing, computing, memory, and response functions. Integrating these functional living components into materials and devices will provide powerful tools for scientific research and enable new technological applications. However, it has been a grand challenge to maintain the viability, functionality, and safety of living components in freestanding materials and devices, which frequently undergo deformations during applications. Here, we report the design of a set of living materials and devices based on stretchable, robust, and biocompatible hydrogel-elastomer hybrids that host various types of genetically engineered bacterial cells. The hydrogel provides sustainable supplies of water and nutrients, and the elastomer is air-permeable, maintaining long-term viability and functionality of the encapsulated cells. Communication between different bacterial strains and with the environment is achieved via diffusion of molecules in the hydrogel. The high stretchability and robustness of the hydrogel-elastomer hybrids prevent leakage of cells from the living materials and devices, even under large deformations. We show functions and applications of stretchable living sensors that are responsive to multiple chemicals in a variety of form factors, including skin patches and gloves-based sensors. We further develop a quantitative model that couples transportation of signaling molecules and cellular response to aid the design of future living materials and devices.

Skeletal muscles possess the combinational properties of high fatigue resistance (1,000 J/m(2)), high strength (1 MPa), low Young’s modulus (100 kPa), and high water content (70 to 80 wt %), which have not been achieved in synthetic hydrogels. The muscle-like properties are highly desirable for hydrogels’ nascent applications in load-bearing artificial tissues and soft devices. Here, we propose a strategy of mechanical training to achieve the aligned nanofibrillar architectures of skeletal muscles in synthetic hydrogels, resulting in the combinational muscle-like properties. These properties are obtained through the training-induced alignment of nanofibrils, without additional chemical modifications or additives. In situ confocal microscopy of the hydrogels’ fracturing processes reveals that the fatigue resistance results from the crack pinning by the aligned nanofibrils, which require much higher energy to fracture than the corresponding amorphous polymer chains. This strategy is particularly applicable for 3D-printed microstructures of hydrogels, in which we can achieve isotropically fatigue-resistant, strong yet compliant properties.

Hydrogels of conducting polymers, particularly poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS), provide a promising electrical interface with biological tissues for sensing and stimulation, owing to their favorable electrical and mechanical properties. While existing methods mostly blend PEDOT:PSS with other compositions such as non-conductive polymers, the blending can compromise resultant hydrogels’ mechanical and/or electrical properties. Here, we show that designing interconnected networks of PEDOT:PSS nanofibrils via a simple method can yield high-performance pure PEDOT:PSS hydrogels. The method involves mixing volatile additive dimethyl sulfoxide (DMSO) into aqueous PEDOT:PSS solutions followed by controlled dry-annealing and rehydration. The resultant hydrogels exhibit a set of properties highly desirable for bioelectronic applications, including high electrical conductivity (~20 S cm−1 in PBS, ~40 S cm−1 in deionized water), high stretchability (> 35% strain), low Young’s modulus (~2 MPa), superior mechanical, electrical and electrochemical stability, and tunable isotropic/anisotropic swelling in wet physiological environments., Hydrogels of conducting polymers provide an electrical interface with biological tissues for sensing and stimulation, but currently have compromised mechanical and electrical properties. Here, the authors show a simple method to achieve pure PEDOT:PSS hydrogels that exhibit superior mechanical and electrical properties, stability, and tunable swelling.

The emerging applications of hydrogels in devices and machines require these soft materials to maintain robustness under cyclic mechanical loads. Whereas hydrogels have been made tough to resist fracture under a single cycle of mechanical load, these toughened gels still suffer from fatigue fracture under multiple cycles of loads. The reported fatigue threshold (i.e., the minimal fracture energy at which crack propagation occurs under cyclic loads) for synthetic hydrogels is on the order of 1-100 J/m2, which is primarily associated with the energy required to fracture a single layer of polymer chains per unit area. Here, we demonstrate that the controlled introduction of crystallinity in hydrogels can significantly enhance their fatigue thresholds, since the process of fracturing crystalline domains for fatigue-crack propagation requires much higher energy than fracturing a single layer of polymer chains. The fatigue threshold of polyvinyl alcohol (PVA) with a crystallinity of 18.9 wt.% in the swollen state can exceed 1,000 J/m2. We further develop a strategy to enhance the anti-fatigue-fracture properties of PVA hydrogels, but still maintain their high water contents and low moduli by patterning highly-crystalline regions in the hydrogels. The current work not only reveals an anti-fatigue-fracture mechanism in hydrogels but also provides a practical method to design anti-fatigue-fracture hydrogels for diverse applications., Comment: 38 pages, 14 figures

Couplants play significant roles in ultrasonography. To ensure imaging quality, it is critical to maintain conformal contact of the couplant with both the skin surface and the ultrasound probe in clinical applications. In addition, either the probe or the couplant should not deform the skin surface significantly, which will result in an overestimated modulus of the tissue for elastography imaging. However, existing liquid gel couplants cannot bear external compressive force, while existing solid gel couplants cannot maintain a conformal contact with skin surface. Especially, the nonconformal contacts and deformation become more severe on body parts of locally high curvatures such as skin tumors, fingers, and elbows. Here we report a bilayer design of couplant for ultrasonography, composing of a stiff layer and a compliant layer of hydrogels. The bilayer hydrogel pad enables it to bear external compression, allowing the probe to move smoothly, conforming high curvature parts and releasing stress concentration. Our clinical experiments further show high quality imaging of thyroid nodules, skin tumors in elbows and fingers using the bilayer hydrogel pad, which represents a promising alternative for a range of applications in ultrasonic diagnosis.

Lightweight and flexible supercapacitors with high volumetric capacitance are vitally required for wearable and portable energy storage devices. We propose an eco-friendly, simple-to-fabricate high performance supercapacitor, which consists of a solid state material based on nitrogen-doped graphene flake electrodes distributed in the NaCl-containing hydrogel electrolyte, achieving a large surface area interface. Stretchability is achieved by sandwiching this structure between two single-walled carbon nanotube film current collectors. The as-prepared quasi-solid material exhibits outstanding volumetric capacitive performance, high energy density and power density values, attaining corresponding values of 806 F cm−3, 112 mW h cm−3 and 294 W cm−3 at 0.3 A g−1. This superior capacitive behavior is due to the excellent network comprising NaCl-containing hydrogel, N-Graphene powder and carbon nanotube film, offering new strategy for developing of sustainable high-performance supercapacitors.

Coupling between solution salinity and the mechanics of charged hydrogels presents an opportunity to harvest osmotic energy in a clean and sustainable way. By applying mechanical pressure to retard the swelling or deswelling of hydrogels in saline solutions, the free energy of mixing is converted into mechanical work. This study developed a theoretical framework and experimentally investigated the potential of hydrogels for energy production from salinity gradients. Mathematical modeling revealed the effect of parameters including the charge and elastic modulus of hydrogels, applied pressure, and the solution salinity on energy conversion using different thermodynamic cycles. With proper material design and process control, the thermodynamic efficiency of an ideal process was predicted to exceed 5% with 10 mM and 600 mM NaCl solutions. Experiments with poly (styrene sulfonate) hydrogels verified the theoretically predicted trends and demonstrated more than 10% thermodynamic efficiency for moderate-salinity sources, due to the unique swelling-strengthened mechanical properties of the gels. The study suggests the potential of polyelectrolyte hydrogels in the extraction of energy from low- to moderate-salinity sources and provides a framework for their design.

In many normal and abnormal physiological processes, including cellular migration during normal development and invasion in cancer metastasis, cells are required to withstand severe deformations. The structural integrity of eukaryotic cells under small deformations has been known to depend on the cytoskeleton including actin filaments (F-actin), microtubules and intermediate filaments (IFs). However, it remains unclear how cells resist severe deformations since both F-actin and microtubules fluidize or disassemble under moderate strains. Here, we demonstrate that vimentin intermediate filaments (VIFs), a marker of mesenchymal cells, dominate cytoplasmic mechanics at large deformations. Our results show that cytoskeletal VIFs form a stretchable, hyperelastic network. This network works synergistically with other dissipative cytoplasmic components, substantially enhancing the strength, stretchability, resilience and toughness of the living cytoplasm.

Electrically conductive hydrogels (ECHs) are attracting much interest in the field of biomaterials science because of their unique properties. However, effective incorporation and dispersion of conductive materials in the matrices of polymeric hydrogels for improved conductivity remains a great challenge. Here, we demonstrate highly transparent, electrically conductive, stretchable tough hydrogels modified by single-walled carbon nanotubes (SWCNTs). Two different approaches for the fabrication of SWCNT/hydrogel structures are examined: a simple SWCNT film transfer onto the as-prepared hydrogel and the film deposition onto the pre-stretched hydrogel. Functionality of our method is confirmed by scanning electron microscopy along with optical and electrical measurements of our structures while subjecting them to different strains. Since the hydrogel-based structures are intrinsically soft, stretchable, wet, and sticky, they conform well to a human skin. We demonstrate applications of our material as skin-like passive electrodes and active finger-mounted joint motion sensors. Our technique shows promise to accelerate the development of biointegrated wearable electronics.