Strong tough hydrogels via the synergy of freeze-casting and salting out.

Natural load-bearing materials such as tendons have a high water content of about 70 per cent but are still strong and tough, even when used for over one million cycles per year, owing to the hierarchical assembly of anisotropic structures across multiple length scales1. Synthetic hydrogels have been created using methods such as electro-spinning2, extrusion3, compositing4,5, freeze-casting6,7, self-assembly8 and mechanical stretching9,10 for improved mechanical performance. However, in contrast to tendons, many hydrogels with the same high water content do not show high strength, toughness or fatigue resistance. Here we present a strategy to produce a multi-length-scale hierarchical hydrogel architecture using a freezing-assisted salting-out treatment. The produced poly(vinyl alcohol) hydrogels are highly anisotropic, comprising micrometre-scale honeycomb-like pore walls, which in turn comprise interconnected nanofibril meshes. These hydrogels have a water content of 70-95 per cent and properties that compare favourably to those of other tough hydrogels and even natural tendons; for example, an ultimate stress of 23.5 ± 2.7 megapascals, strain levels of 2,900 ± 450 per cent, toughness of 210 ± 13 megajoules per cubic metre, fracture energy of 170 ± 8 kilojoules per square metre and a fatigue threshold of 10.5 ± 1.3 kilojoules per square metre. The presented strategy is generalizable to other polymers, and could expand the applicability of structural hydrogels to conditions involving more demanding mechanical loading.

Water-assisted strong underwater adhesion via interfacial water removal and self-adaptive gelation.

In nearly all cases of underwater adhesion, water molecules typically act as a destroyer. Thus, removing interfacial water from the substrate surfaces is essential for forming super-strong underwater adhesion. However, current methods mainly rely on physical means to dislodge interfacial water, such as absorption, hydrophobic repulsion, or extrusion, which are inefficient in removing obstinate hydrated water at contact interface, resulting in poor adhesion. Herein, we present a unique means of reversing the role of water to assist in realizing a self-strengthening liquid underwater adhesive (SLU-adhesive) that can effectively remove water at contact interface. This is achieved through multiscale physical-chemical coupling methods across millimeter to molecular levels and self-adaptive strengthening of the cohesion during underwater operations. As a result, strong adhesion over 1,600 kPa (compared to ~100 to 1,000 kPa in current state of the art) can be achieved on various materials, including inorganic metal and organic plastic materials, without preloading in different environments such as pure water, a wide range of pH solutions (pH = 3 to 11), and seawater. Intriguingly, SLU-adhesive/photothermal nanoparticles (carbon nanotubes) hybrid materials can significantly reduce the time required for complete curing from 24 h to 40 min using near-infrared laser radiation due to unique thermal-response of the chemical reaction rate. The excellent adhesion property and self-adaptive adhesion procedure allow SLU-adhesive materials to demonstrate great potential for broad applications in underwater sand stabilization, underwater repair, and even adhesion failure detection as a self-reporting adhesive. This concept of "water helper" has potential to advance underwater adhesion and manufacturing strategies.

Microstructure-Reconfigured Graphene Oxide Aerogel Metamaterials for Ultrarobust Directional Sensing at Human-Machine Interfaces.

Graphene aerogels hold huge promise for the development of high-performance pressure sensors for future human-machine interfaces due to their ordered microstructure and conductive network. However, their application is hindered by the limited strain sensing range caused by the intrinsic stiffness of the porous microstructure. Herein, an anisotropic cross-linked chitosan and reduced graphene oxide (CCS-rGO) aerogel metamaterial is realized by reconfiguring the microstructure from a honeycomb to a buckling structure at the dedicated cross-section plane. The reconfigured CCS-rGO aerogel shows directional hyperelasticity with extraordinary durability (no obvious structural damage after 20 000 cycles at a directional compressive strain of ≤0.7). The CCS-rGO aerogel pressure sensor exhibits an ultrahigh sensitivity of 121.45 kPa-1, an unprecedented sensing range, and robust mechanical and electrical performance. The aerogel sensors are demonstrated to monitor human motions, control robotic hands, and even integrate into a flexible keyboard to play music, which opens a wide application potential in future human-machine interfaces.

MXene/Nitrogen-Doped Carbon Nanosheet Scaffold Electrode toward High-Performance Solid-State Zinc Ion Supercapacitor.

While MXene is widely used as an electrode material for supercapacitor, the intrinsic limitation of stacking caused by the interlayer van der Waals forces has yet to be overcome. In this work, a strategy is proposed to fabricate a composite scaffold electrode (MCN) by intercalating MXene with highly nitrogen-doped carbon nanosheets (CN). The 2D structured CN, thermally converted and pickling from Zn-hexamine (Zn-HMT), serves as a spacer that effectively prevents the stacking of MXene and contributes to a hierarchically scaffolded structure, which is conducive to ion movement; meanwhile, the high nitrogen-doping of CN tunes the electronic structure of MCN to facilitate charge transfer and providing additional pseudocapacitance. As a result, the MCN50 composite electrode achieves a high specific capacitance of 418.4 F g-1 at 1 A g-1. The assembled symmetric supercapacitor delivers a corresponding power density of 1658.9 W kg-1 and an energy density of 30.8 Wh kg-1. The all-solid-state zinc ion supercapacitor demonstrates a superior energy density of 68.4 Wh kg-1 and a power density of 403.5 W kg-1 and shows a high capacitance retention of 93% after 8000 charge-discharge cycles. This study sheds a new light on the design and development of novel MXene-based composite electrodes for high performance all-solid-state zinc ion supercapacitor.

Comparison of anesthesia methods for intra-arterial therapy of patients with acute ischemic stroke: an updated meta-analysis and systematic review.

OBJECTIVES: Currently, there remains debate regarding the optimal anesthesia approach for patients undergoing intra-arterial therapy for acute ischemic stroke. Therefore, we conducted a comparative analysis to assess the effects of general anesthesia versus non general anesthesia on patient outcomes. METHODS: The research methodology entailed comprehensive searches of prominent databases such as the Cochrane Library, PubMed, Scopus, and Web of Science, covering the period from January 1, 2010, to March 1, 2024. Data synthesis employed techniques like risk ratio or standardized mean difference, along with 95% confidence intervals. The study protocol was prospectively registered with PROSPERO (CRD42024523079). RESULTS: A total of 27 trials and 12,875 patients were included in this study. The findings indicated that opting for non-general anesthesia significantly decreased the risk of in-hospital mortality (RR, 1.98; 95% CI: 1.50 to 2.61; p<0.00001; I2 = 20%), as well as mortality within three months post-procedure (RR, 1.24; 95% CI: 1.15 to 1.34; p<0.00001; I2 = 26%), while also leading to a shorter hospitalization duration (SMD, 0.24; 95% CI: 0.15 to 0.33; p<0.00001; I2 = 44%). CONCLUSION: Ischemic stroke patients who undergo intra-arterial treatment without general anesthesia have a lower risk of postoperative adverse events and less short-term neurological damage. In routine and non-emergency situations, non-general anesthetic options may be more suitable for intra-arterial treatment, offering greater benefits to patients. In addition to this, the neuroprotective effects of anesthetic drugs should be considered more preoperatively and postoperatively.

Solar anti-icing surface with enhanced condensate self-removing at extreme environmental conditions.

The inhibition of condensation freezing under extreme conditions (i.e., ultra-low temperature and high humidity) remains a daunting challenge in the field of anti-icing. As water vapor easily condensates or desublimates and melted water refreezes instantly, these cause significant performance decrease of most anti-icing surfaces at such extreme conditions. Herein, inspired by wheat leaves, an effective condensate self-removing solar anti-icing/frosting surface (CR-SAS) is fabricated using ultrafast pulsed laser deposition technology, which exhibits synergistic effects of enhanced condensate self-removal and efficient solar anti-icing. The superblack CR-SAS displays superior anti-reflection and photothermal conversion performance, benefiting from the light trapping effect in the micro/nano hierarchical structures and the thermoplasmonic effect of the iron oxide nanoparticles. Meanwhile, the CR-SAS displays superhydrophobicity to condensed water, which can be instantly shed off from the surface before freezing through self-propelled droplet jumping, thus leading to a continuously refreshed dry area available for sunlight absorption and photothermal conversion. Under one-sun illumination, the CR-SAS can be maintained ice free even under an ambient environment of -50 °C ultra-low temperature and extremely high humidity (ice supersaturation degree of ∼260). The excellent environmental versatility, mechanical durability, and material adaptability make CR-SAS a promising anti-icing candidate for broad practical applications even in harsh environments.

Investigation of reversible metal ion (Li+, Na+, Mg2+, Al3+) insertion in MoTe2 for rechargeable aqueous batteries.

In this work, we report the electrochemical reactivity of MoTe2 for various metal ions with special emphasis on Al3+ ion storage in aqueous electrolytes for the first time. A stable discharge capacity of 100 mA h g-1 over 250 cycles at a current density of 1 Ag-1 could be obtained for the Al3+ ion, whereas inferior storage capacities were shown for other metal ions.

Superhydrophobic photothermal icephobic surfaces based on candle soot.

Ice accumulation causes various problems in our daily life for human society. The daunting challenges in ice prevention and removal call for novel efficient antiicing strategies. Recently, photothermal materials have gained attention for creating icephobic surfaces owing to their merits of energy conservation and environmental friendliness. However, it is always challenging to get an ideal photothermal material which is cheap, easily fabricating, and highly photothermally efficient. Here, we demonstrate a low-cost, high-efficiency superhydrophobic photothermal surface, uniquely based on inexpensive commonly seen candle soot. It consists of three components: candle soot, silica shell, and polydimethylsiloxane (PDMS) brushes. The candle soot provides hierarchical nano/microstructures and photothermal ability, the silica shell strengthens the hierarchical candle soot, and the grafted low-surface-energy PDMS brushes endow the surface with superhydrophobicity. Upon illumination under 1 sun, the surface temperature can increase by 53 °C, so that no ice can form at an environmental temperature as low as -50 °C and it can also rapidly melt the accumulated frost and ice in 300 s. The superhydrophobicity enables the melted water to slide away immediately, leaving a clean and dry surface. The surface can also self-clean, which further enhances its effectiveness by removing dust and other contaminants which absorb and scatter sunlight. In addition, after oxygen plasma treatment, the surface can restore superhydrophobicity with sunlight illumination. The presented icephobic surface shows great potential and broad impacts owing to its inexpensive component materials, simplicity, ecofriendliness, and high energy efficiency.

Photoinduced Dual Shape Programmability of Covalent Adaptable Networks with Remarkable Mechanical Properties.

As classic shape memory polymers featuring shape reconfiguration of temporary state, covalent adaptable networks containing reversible bonds can enable permanent-state reconfigurability through topological rearrangement via dynamic bond exchange. Yet, such an attractive dual shape programmability is limited by the actuation mode of direct heat transfer and poor mechanical properties, restricting its control precision and functionality. Herein, we presented a method to create nanocomposites with photomodulated dual shape programmability and remarkable mechanical properties leading the fields of covalent adaptable networks. MXene, whose photothermal efficiency was revealed to be regulated by the etching method and delamination, was introduced into polyurethane networks. Upon adjusting the light intensity, the dual shape programmability of both permanent and temporary states could be accomplished, which exhibited potential in information recognition, photowriting paper, etc. Furthermore, owing to the dynamic transcarbamoylation at elevated temperatures, such a phototriggered dual shape programmability could be maintained after the self-healing and reprocessing.

Inorganic Photonic Microspheres with Localized Concentric Ordering for Deep Pattern Encoding and Triple Sensory Microsensor.

Photonic microspheres offer building units with unique topological structures and specific optical functions for diverse applications. Here, a new class of inorganic photonic microspheres with superior robustness, optical and electrical properties is reported by introducing a unique localized concentric ordering architecture and chemical interaction, which further serve as building blocks for deep pattern encoding and multiple sensory optoelectronic devices. Benefiting from localized concentric ordering architecture, the resultant photonic microspheres demonstrate orientation- and angle-independent structural colors. Notably, the formation of well-combined lamellae inorganic layers by chemical interaction grants the microspheres superior mechanical robustness, excellent solvent resistance, thermal stability, and multiple optoelectronic properties simultaneously, rarely seen in previous reports. Owing to these merits, such microspheres are used to construct diverse encoded photonic patterns for anti-counterfeiting applications. Interestingly, cross-communication among neighboring microspheres creates complex photonic sub-patterns, which provide "fingerprint information" with deep encryption security. Moreover, a single photonic microsphere-based optoelectronic microsensor is demonstrated for the first time, which achieves appealing application for real-time health monitoring and safety warning toward triple environmental stimuli. This work not only provides a new kind of robust, multifunctional photonic material, but also opens a new avenue for their uses as complexed pattern encoding and multi-parametric sensing platforms.

Synthetic homeostatic materials with chemo-mechano-chemical self-regulation.

Living organisms have unique homeostatic abilities, maintaining tight control of their local environment through interconversions of chemical and mechanical energy and self-regulating feedback loops organized hierarchically across many length scales. In contrast, most synthetic materials are incapable of continuous self-monitoring and self-regulating behaviour owing to their limited single-directional chemomechanical or mechanochemical modes. Applying the concept of homeostasis to the design of autonomous materials would have substantial impacts in areas ranging from medical implants that help stabilize bodily functions to 'smart' materials that regulate energy usage. Here we present a versatile strategy for creating self-regulating, self-powered, homeostatic materials capable of precisely tailored chemo-mechano-chemical feedback loops on the nano- or microscale. We design a bilayer system with hydrogel-supported, catalyst-bearing microstructures, which are separated from a reactant-containing 'nutrient' layer. Reconfiguration of the gel in response to a stimulus induces the reversible actuation of the microstructures into and out of the nutrient layer, and serves as a highly precise 'on/off' switch for chemical reactions. We apply this design to trigger organic, inorganic and biochemical reactions that undergo reversible, repeatable cycles synchronized with the motion of the microstructures and the driving external chemical stimulus. By exploiting a continuous feedback loop between various exothermic catalytic reactions in the nutrient layer and the mechanical action of the temperature-responsive gel, we then create exemplary autonomous, self-sustained homeostatic systems that maintain a user-defined parameter--temperature--in a narrow range. The experimental results are validated using computational modelling that qualitatively captures the essential features of the self-regulating behaviour and provides additional criteria for the optimization of the homeostatic function, subsequently confirmed experimentally. This design is highly customizable owing to the broad choice of chemistries, tunable mechanics and its physical simplicity, and may lead to a variety of applications in autonomous systems with chemo-mechano-chemical transduction at their core.

Microscale Silicon Origami.

A new methodology to create 3D origami patterns out of Si nanomembranes using pre-stretched and pre-patterned polydimethylsiloxane substrates is reported. It is shown this approach is able to mimic paper-based origami patterns. The combination of origami-based microscale 3D architectures and stretchable devices will lead to a breakthrough on reconfigurable systems.

Computational modeling of oscillating fins that "catch and release" targeted nanoparticles in bilayer flows.

A number of physiological processes in living organisms involve the selective "catch and release" of biomolecules. Inspired by these biological processes, we use computational modeling to design synthetic systems that can controllably catch, transport, and release specific molecules within the surrounding solution, and, thus, could be harnessed for effective separation processes within microfluidic devices. Our system consists of an array of oscillating, microscopic fins that are anchored onto the floor of a microchannel and immersed in a flowing bilayer fluid. The oscillations drive the fins to repeatedly extend into the upper fluid and then tilt into the lower stream. The fins exhibit a specified wetting interaction with the fluids and specific adhesive interactions with nanoparticles in the solution. With this setup, we determine conditions where the oscillating fins can selectively bind, and thus, "catch" target nanoparticles within the upper fluid stream and then release these particles into the lower stream. We isolate the effects of varying the wetting interaction and the fins' oscillation modes on the effective extraction of target species from the upper stream. Our findings provide fundamental insights into the system's complex dynamics and yield guidelines for fabricating devices for the detection and separation of target molecules from complex fluids.

Biomimetic Hydrogel Composites for Soil Stabilization and Contaminant Mitigation.

We have developed a novel method to synthesize a hyper-branched biomimetic hydrogel network across a soil matrix to improve the mechanical strength of the loose soil and simultaneously mitigate potential contamination due to excessive ammonium. This method successfully yielded a hierarchical structure that possesses the water retention, ion absorption, and soil aggregation capabilities of plant root systems in a chemically controllable manner. Inspired by the robust organic-inorganic composites found in many living organisms, we have combined this hydrogel network with a calcite biomineralization process to stabilize soil. Our experiments demonstrate that poly(acrylic acid) (PAA) can work synergistically with enzyme-induced carbonate precipitation (EICP) to render a versatile, high-performance soil stabilization method. PAA-enhanced EICP provides multiple benefits including lengthening of water supply time, localization of cementation reactions, reduction of harmful byproduct ammonium, and achievement of ultrahigh soil strength. Soil crusts we have obtained can sustain up to 4.8 × 103 kPa pressure, a level comparable to cementitious materials. An ammonium removal rate of 96% has also been achieved. These results demonstrate the potential for hydrogel-assisted EICP to provide effective soil improvement and ammonium mitigation for wind erosion control and other applications.

Fast and Facile Liquid Metal Printing via Projection Lithography for Highly Stretchable Electronic Circuits.

Soft electronic circuits are crucial for wearable electronics, biomedical technologies, and soft robotics, requiring soft conductive materials with high conductivity, high strain limit, and stable electrical performance under deformation. Liquid metals (LMs) have become attractive candidates with high conductivity and fluidic compliance, while effective manufacturing methods are demanded. Digital light processing (DLP)-based projection lithography is a high-resolution and high-throughput printing technique for primarily polymers and some metals. If LMs can be printed with DLP as well, the entire soft devices can be fabricated by one printer in a streamlined and highly efficient process. Herein, fast and facile DLP-based LM printing is achieved. Simply with 5-10 s of patterned ultraviolet (UV)-light exposure, a highly conductive and stretchable pattern can be printed using a photo-crosslinkable LM particle ink. The printed eutectic gallium indium traces feature high resolution (≈20 µm), conductivity (3 × 106 S m-1), stretchability (≈2500%), and excellent stability (consistent performance at different deformation). Various patterns are printed in diverse material systems for broad applications including stretchable displays, epidermal strain sensors, heaters, humidity sensors, conformal electrodes for electrography, and multi-layer actuators. The facile and scalable process, excellent performance, and diverse applications ensure its broad impact on soft electronic manufacturing.

Advances and Challenges in Wearable Glaucoma Diagnostics and Therapeutics.

Glaucoma is a leading cause of irreversible blindness, and early detection and treatment are crucial for preventing vision loss. This review aims to provide an overview of current diagnostic and treatment standards, recent medical and technological advances, and current challenges and future outlook for wearable glaucoma diagnostics and therapeutics. Conventional diagnostic techniques, including the rebound tonometer and Goldmann Applanation Tonometer, provide reliable intraocular pressure (IOP) measurement data at single-interval visits. The Sensimed Triggerfish and other emerging contact lenses provide continuous IOP tracking, which can improve diagnostic IOP monitoring for glaucoma. Conventional therapeutic techniques include eye drops and laser therapies, while emerging drug-eluting contact lenses can solve patient noncompliance with eye medications. Theranostic platforms combine diagnostic and therapeutic capabilities into a single device. Advantages of these platforms include real-time monitoring and personalized medication dosing. While there are many challenges to the development of wearable glaucoma diagnostics and therapeutics, wearable technologies hold great potential for enhancing glaucoma management by providing continuous monitoring, improving medication adherence, and reducing the disease burden on patients and healthcare systems. Further research and development of these technologies will be essential to optimizing patient outcomes.

Sunlight-powered self-excited oscillators for sustainable autonomous soft robotics.

As the field of soft robotics advances, full autonomy becomes highly sought after, especially if robot motion can be powered by environmental energy. This would present a self-sustained approach in terms of both energy supply and motion control. Now, autonomous movement can be realized by leveraging out-of-equilibrium oscillatory motion of stimuli-responsive polymers under a constant light source. It would be more advantageous if environmental energy could be scavenged to power robots. However, generating oscillation becomes challenging under the limited power density of available environmental energy sources. Here, we developed fully autonomous soft robots with self-sustainability based on self-excited oscillation. Aided by modeling, we have successfully reduced the required input power density to around one-Sun level through a liquid crystal elastomer (LCE)-based bilayer structure. The autonomous motion of the low-intensity LCE/elastomer bilayer oscillator "LiLBot" under low energy supply was achieved by high photothermal conversion, low modulus, and high material responsiveness simultaneously. The LiLBot features tunable peak-to-peak amplitudes from 4 to 72 degrees and frequencies from 0.3 to 11 hertz. The oscillation approach offers a strategy for designing autonomous, untethered, and sustainable small-scale soft robots, such as a sailboat, walker, roller, and synchronized flapping wings.

All-Fabric Capacitive Pressure Sensors with Piezoelectric Nanofibers for Wearable Electronics and Robotic Sensing.

Flexible pressure sensors are increasingly sought after for applications ranging from physiological signal monitoring to robotic sensing; however, the challenges associated with fabricating highly sensitive, comfortable, and cost-effective sensors remain formidable. This study presents a high-performance, all-fabric capacitive pressure sensor (AFCPS) that incorporates piezoelectric nanofibers. Through the meticulous optimization of conductive fiber electrodes and P(VDF-TrFE) nanofiber dielectric layers, the AFCPS exhibits exceptional attributes such as high sensitivity (4.05 kPa-1), an ultralow detection limit (0.6 Pa), an extensive detection range (∼100 kPa), rapid response time (<26 ms), and robust stability (>14,000 cycles). The sensor's porous structure enhances its compressibility, while its piezoelectric properties expedite charge separation, thereby increasing the interface capacitance and augmenting overall performance. These features are elucidated further through multiphysical field-coupling simulations and experimental testing. Owing to its comprehensive superior performance, the AFCPS has demonstrated its efficacy in monitoring human activity and physiological signals, as well as in discerning soft robotic grasping movements. Additionally, we have successfully implemented multiple AFCPS units as pressure sensor arrays to ascertain spatial pressure distribution and enable intelligent robotic gripping. Our research underscores the promising potential of the AFCPS device in wearable electronics and robotic sensing, thereby contributing significantly to the advancement of high-performance fabric-based sensors.

Tough Hydrogel Electrolytes for Anti-Freezing Zinc-Ion Batteries.

As the soaring demand for energy storage continues to grow, batteries that can cope with extreme conditions are highly desired. Yet, existing battery materials are limited by weak mechanical properties and freeze-vulnerability, prohibiting safe energy storage in devices that are exposed to low temperature and unusual mechanical impacts. Herein, a fabrication method harnessing the synergistic effect of co-nonsolvency and "salting-out" that can produce poly(vinyl alcohol) hydrogel electrolytes with unique open-cell porous structures, composed of strongly aggregated polymer chains, and containing disrupted hydrogen bonds among free water molecules, is introduced. The hydrogel electrolyte simultaneously combines high strength (tensile strength 15.6 MPa), freeze-tolerance (< -77 °C), high mass transport (10× lower overpotential), and dendrite and parasitic reactions suppression for stable performance (30 000 cycles). The high generality of this method is further demonstrated with poly(N-isopropylacrylamide) and poly(N-tertbutylacrylamide-co-acrylamide) hydrogels. This work takes a further step toward flexible battery development for harsh environments.