Ag-thiolate interactions to enable an ultrasensitive and stretchable MXene strain sensor with high temporospatial resolution.

High-sensitivity strain sensing elements with a wide strain range, fast response, high stability, and small sensing areas are desirable for constructing strain sensor arrays with high temporospatial resolution. However, current strain sensors rely on crack-based conductive materials having an inherent tradeoff between their sensing area and performance. Here, we present a molecular-level crack modulation strategy in which we use layer-by-layer assembly to introduce strong, dynamic, and reversible coordination bonds in an MXene and silver nanowire-matrixed conductive film. We use this approach to fabricate a crack-based stretchable strain sensor with a very small sensing area (0.25 mm2). It also exhibits an ultrawide working strain range (0.001-37%), high sensitivity (gauge factor ~500 at 0.001% and >150,000 at 35%), fast response time, low hysteresis, and excellent long-term stability. Based on this high-performance sensing element and facile assembly process, a stretchable strain sensor array with a device density of 100 sensors per cm2 is realized. We demonstrate the practical use of the high-density strain sensor array as a multichannel pulse sensing system for monitoring pulses in terms of their spatiotemporal resolution.

Enhancing Low-Frequency Microwave Absorption Through Structural Polarization Modulation of MXenes.

Two-dimensional carbon-based materials have shown promising electromagnetic wave absorption capabilities in mid- and high-frequency ranges, but face challenges in low-frequency absorption due to limited control over polarization response mechanisms and ambiguous resonance behavior. In this study, we propose a novel approach to enhance absorption efficiency in aligned three-dimensional (3D) MXene/CNF (cellulose nanofibers) cavities by modifying polarization properties and manipulating resonance response in the 3D MXene architecture. This controlled polarization mechanism results in a significant shift of the main absorption region from the X-band to the S-band, leading to a remarkable reflection loss value of - 47.9 dB in the low-frequency range. Furthermore, our findings revealed the importance of the oriented electromagnetic coupling in influencing electromagnetic response and microwave absorption properties. The present study inspired us to develop a generic strategy for low-frequency tuned absorption in the absence of magnetic element participation, while orientation-induced polarization and the derived magnetic resonance coupling are the key controlling factors of the method.

Mild γ-Butyrolactone/Water Pretreatment for Highly Efficient Sugar Production from Corn Stover.

In this study, γ-butyrolactone/water (GBL/H2O) was explored as a mild, efficient, and cost-effective binary solvent pretreatment to enhance hydrolyzability of corn stover (CS). Key pretreatment parameters-reaction time, temperature, and H2SO4 concentration-were systematically investigated for their effects on the physicochemical properties of CS. Specifically, increased temperature and acid concentration significantly decreased cellulose crystallinity (from 1.39 for untreated CS to 1.04 for CS pretreated by GBL/H2O with 100 mM H2SO4 at 120 °C for 1 h) and promoted lignin removal (47.3% for CS pretreated by GBL/H2O with 150 mM H2SO4 at 120 °C for 1 h). Acknowledging the cellulase's limited hydrolysis efficiency, a dual-enzyme scheme using a low cellulase dosage (10 FPU/g) supplemented with ß-glucosidase or xylanase was tested, enhancing hydrolysis of CS pretreated under low temperature-long duration and high temperature-short duration conditions, respectively. Optimum sugar release was obtained from CS pretreated with GBL/H2O and 150 mM H2SO4 at 120 °C for 1 h, achieving 98% glucan and 82.3% xylan conversion, compared with 53.9% and 17% of glucan and xylan conversion from untreated CS. GBL/H2O pretreatment outperformed other binary systems in literature, achieving the highest sugar conversions with lower enzyme loading. These results highlight the potential of GBL/H2O pretreatment for efficient biomass conversion, contributing to the goals of the green economy.

Long-cycling and High-voltage Solid State Lithium Metal Batteries Enabled by Fluorinated and Crosslinked Polyether Electrolytes.

Solid-state lithium metal batteries (LMBs), constructed through the in situ fabrication of polymer electrolytes, are considered a critical strategy for the next-generation battery systems with high energy density and enhanced safety. However, the constrained oxidation stability of polymers, such as the extensively utilized polyethers, limits their applications in high-voltage batteries and further energy density improvements. Herein, an in situ fabricated fluorinated and crosslinked polyether-based gel polymer electrolyte, FGPE, is presented, exhibiting a high oxidation potential (5.1 V). The fluorinated polyether significantly improves compatibility with both lithium metal and high-voltage cathode, attributed to the electron-withdrawing -CF3 group and the generated LiF-rich electrolyte/electrode interphase. Consequently, the solid-state Li||LiNi0.6Co0.2Mn0.2O2 batteries employing FGPE demonstrate exceptional cycling performances of 1000 cycles with 78 % retention, representing one of the best results ever reported for polymer electrolytes. Moreover, FGPE enables batteries to operate at 4.7 V, realizing the highest operating voltage of polyether-based batteries to date. Notably, our designed in situ FGPE provides the solid-state batteries with exceptional cycling stability even at practical conditions, including high cathode loading (21 mg cm-2) and industry-level 18650-type cylindrical cells (1.3 Ah, 500 cycles). This work provides critical insights into the development of oxidation-stable polymer electrolytes and the advancement of practical high-voltage LMBs.

Highly Elastic, Robust, and Efficient Hydrogel Solar Absorber against Harsh Environmental Impacts.

Solar distillation is a promising approach for addressing water scarcity, but relentless stress/strain perturbations induced by wind and waves would inevitably cause structural damage to solar absorbers. Despite notable advances in efficient solar absorbers, there have been no reports of compliant and robust solar absorbers withstanding practical mechanical impacts. Herein, an elastic and robust hydrogel absorber that exhibited a high level of evaporation performance was fabricated by introducing ion-coordinated MXene nanosheets as photothermal conversion units and mechanically enhanced fillers. The ion-coordinated MXene nanosheets acting as strong cross-linking points provided excellent elasticity and robustness to the hydrogel absorber. As a result, the evaporation rate of hydrogel absorber, with a high initial value of 2.61 kg m-2 h-1 under one sun irradiation, remained at 2.15 kg m-2 h-1 under a 100% tensile strain state and 2.40 kg m-2 h-1 after 10 000 stretching-releasing cycles. This continuous and stable water desalination approach provides a promising device for actual seawater distillation.

Biomimetic Electrochemical Sensor Based on Single-Atom Nickel Laccase Nanoenzyme for Quercetin Detection.

Laccase, a member of the copper oxidase family, has been used as a green catalyst in the environmental and biochemical industries. However, laccase nanoenzymes are limited to materials with copper as the active site, and noncopper laccase nanoenzymes have been scarcely reported. In this study, inspired by the multiple copper active sites of natural laccase and the redox Cu2+/Cu+ electron transfer pathway, a novel nitrogen/nickel single-atom nanoenzyme (N/Ni SAE) with high laccase-like activity was prepared by inducing Ni and dopamine precipitation through a controllable water/ethanol interface reaction. Compared with that of laccase, the laccase activity simulated by N/Ni SAE exhibited excellent stability and reusability. The N/Ni SAE exhibited a higher efficiency toward the degradation of 2,4-dichlorophenol, hydroquinone, bisphenol A, and p-aminobenzene. In addition, a sensitive electrochemical biosensor was constructed by leveraging the laccase-like activity of N/Ni SAE; this sensor offered unique advantages in terms of catalytic activity, selectivity, stability, and repeatability. Its detection ranges for quercetin were 0.01-0.1 and 1.0-100 µM, and the detection limit was 3.4 nM. It was also successfully used for the quantitative detection of quercetin in fruit juices. Therefore, the single-atom biomimetic nanoenzymes prepared in this study promote the development of a new electrochemical strategy for the detection of various bioactive molecules and show great potential for practical applications.

A Microphase-Separated Design toward an All-Round Ionic Hydrogel with Discriminable and Anti-Disturbance Multisensory Functions.

Stretchable ionic hydrogels with superior all-round properties that can detect multimodal sensations with excellent discriminability and robustness against external disturbances are highly required for artificial electronic skinapplications. However, some critical material parameters exhibit intrinsic tradeoffs with each other for most ionic hydrogels. Here, a microphase-separated hydrogel is demonstrated by combining three strategies: (1) using of a low crosslinker/monomer ratio to obtain highly entangled polymer chains as the first network; (2) the introduction of zwitterions into the first network; (3) the synthesis of an ultrasoft polyelectrolyte as the second network. This all-round elastic ionic hydrogel exhibits a low Young's modulus (< 60 kPa), large stretchability (> 900%), high resilience (> 95%), unique strain-stiffening behavior, excellent fatigue tolerance, high ionic conductivity (> 2.0 S m⁻1), and anti-freezing capability, which have not been achieved before. These properties allow the ionic hydrogel to operate as a stretchable multimodal sensor that can detect and decouple multiple stimuli (temperature, pressure, and proximity) with excellent discriminability, high sensitivity, and strong sensing-robustness against strains or temperature perturbations. The ionic hydrogel sensor exhibits great potential for intelligent electronic skin applications such as reliable health monitoring and accurate object identification.

Multifunctional, Self-Adhesive MXene-Based Hydrogel Flexible Strain Sensors for Hand-Written Digit Recognition with Assistance of Deep Learning.

The conductive hydrogel as a flexible sensor not only has certain mechanical flexibility but also can be used in the field of human health detection and human-computer interaction. Herein, by introduction of tannic acid (TA) with MXene into the polyacrylamide (PAM)/carboxymethyl chitosan (CMC) double-network hydrogel, a hydrogel with high stretchability, self-adhesion, and high sensitivity was prepared. CMC and PAM form a semi-interpenetrating double-network of high toughness and durability through electrostatic interactions and multiple hydrogen bonding networks. The abundant hydrophilic functional groups on TA and MXene form multiple hydrogen bonds simultaneously with the polymer network, ensuring high stretchability and sensitivity of the hydrogel. The hydrogel can display an accurate response to a variety of stimulus signals and can monitor both human joint movements and small physiological signal changes. It can also be combined with deep learning algorithms to classify handwritten digits with an accuracy rate of 98%. This work can promote the application of hydrogel sensors with durability and high sensitivity. The combination of algorithms and flexible sensors provides important ideas for the further development of flexible devices.

Biomimetic Ultratough, Strong, and Ductile Artificial Polymer Fiber Based on Immovable and Slidable Cross-links.

It remains a challenge to artificially fabricate fibers with the macroscopic mechanical properties and characteristics of spider silk. Herein, a covalently cross-linked double-network strategy was proposed to disrupt the inverse relation of strength and toughness in the fabrication of ultratough and superstrong artificial polymer fibers. Our design utilized a strong fishnet-like structure based on immovable cellulose nanocrystal cross-links to mimic the function of the ß-sheet nanocrystallites and a slidable mechanically interlocked network based on polyrotaxane to imitate the dissipative stick-slip motion of the ß-strands in spider silk. The resultant fiber exhibited superior mechanical properties, including gigapascal tensile strength, a ductility of over 60%, and a toughness exceeding 420 MJ/m3. The fibers also showed robust biological functions similar to those of spider silks, demonstrating mechanical enhancement, energy absorption ability, and shape memory. A composite with our artificial fibers as reinforcing fibers exhibited remarkable tear and fatigue resistance.

Peak Running, Mechanical, and Physiological Demands of Professional Men's Field Hockey Matches.

The aim of this study was to investigate the peak running, mechanical, and physiological demands of players of different positions in professional men's field hockey matches. Eighteen professional male field hockey players participated in the study, and data were collected in eleven official matches. Players wore GPS units (Vector S7, Catapult Sports) and heart rate (HR) monitors (Polar H1, Polar Electros) to collect physical and physiological data. Physical and physiological output of forwards, midfielders, and defenders in full matches and during 1-min peak periods was analysed. For all metrics and positions, the values identified for the 1-min peak periods were greater than the average values of match play (p < 0.05). In terms of 1-min peak period Player Load, all three positions were significantly different from each other. Forwards achieved the highest Player Load per minute, while defenders the lowest. The distance per minute, high-speed distance per minute, and the relative average heart rate of defenders were significantly lower than of midfielders and forwards (p < 0.05). The current study revealed the peak running, mechanical, and physiological demands of professional men's field hockey matches. It is recommended when prescribing training programmes, to consider not only match average demands, but also peak demands. Forwards and midfielders displayed similar peak demands, while defenders had the lowest demands in all metrics except the number of accelerations and decelerations per minute. Player Load per minute can be used to identify the differences in peak mechanical demands between forwards and midfielders.

Manipulation of Impedance Matching toward 3D-Printed Lightweight and Stiff MXene-Based Aerogels for Consecutive Multiband Tunable Electromagnetic Wave Absorption.

Highly conductive MXene material exhibits outstanding dissipation capability of electromagnetic (EM) waves. However, the interfacial impedance mismatch due to high reflectivity restricts the application of MXene-based EM wave absorbing materials. Herein, a direct ink writing (DIW) 3D printing strategy to construct lightweight and stiff MXene/graphene oxide aerogels (SMGAs) with controllable fret architecture is demonstrated, exhibiting tunable EM wave absorption properties by manipulating impedance matching. Noteworthy, the maximum reflection loss variation value (ΔRL) of SMGAs is -61.2 dB by accurately modulating the width of the fret architecture. The effective absorption region (fE) of SMGAs exhibits consecutive multiband tunability, and the broadest tunable fE (Δf) is 14.05 GHz, which could be continuously tuned in the whole C- (4-8 GHz), X- (8-12 GHz), and Ku-bands (12-18 GHz). Importantly, the hierarchical structures and the orderly stacking of filaments endow lightweight SMGAs (0.024 g cm-3) with a surprising compression resistance, which can withstand 36 000 times its own weight without obvious deformation. Finite element analysis (FEA) further indicates that the hierarchical structure facilitates stress dispersion. The strategy developed here provides a method for fabricating tunable MXene-based EM wave absorbers that are lightweight and stiff.

Extremely Robust and Multifunctional Nanocomposite Fibers for Strain-Unperturbed Textile Electronics.

Textile electronics are needed that can achieve strain-unaltered performance when they undergo irregular and repeated strain deformation. Such strain-unaltered textile electronics require advanced fibers that simultaneously have high functionalities and extreme robustness as fabric materials. Current synthetic nanocomposite fibers based on inorganic matrix have remarkable functionalities but often suffer from low robustness and poor tolerance against crack formation. Here, we present a design for a high-performance multifunctional nanocomposite fiber that is mechanically and electrically robust, which was realized by crosslinking titanium carbide (MXene) nanosheets with a slide-ring polyrotaxane to form an internal mechanically-interlocked network. This inorganic matrix nanocomposite fiber featured distinct strain-hardening mechanical behavior and exceptional load-bearing capability (toughness approaching 60 MJ m-3 and ductility over 27%). It retained 100% of its ductility after cyclic strain loading. Moreover, the high electrical conductivity (>1.1 × 105 S m-1 ) and electrochemical performance (>360 F cm-3 ) of the nanocomposite fiber can be well retained after subjecting the fiber to extensive (>25% strain) and long-term repeated (10 000 cycles) dimensional changes. Such superior robustness allowed for the fabrication of the nanocomposite fibers into various robust wearable devices, such as textile-based electromechanical sensors with strain-unalterable sensing performance and fiber-shaped supercapacitors with invariant electrochemical performance for 10 000 strain loading cycles.

Viscoelastic Metal-in-Water Emulsion Gel via Host-Guest Bridging for Printed and Strain-Activated Stretchable Electrodes.

Stretchable conductive electrodes that can be made by printing technology with high resolution is desired for preparing wearable electronics. Printable inks composed of liquid metals are ideal candidates for these applications, but their practical applications are limited by their low stability, poor printability, and low conductivity. Here, thixotropic metal-in-water (M/W) emulsion gels (MWEGs) were designed and developed by stabilizing and bridging liquid metal droplets (LMDs) via a host-guest polymer. In the MWEGs, the hydrophilic main chain of the host-guest polymers emulsified and stabilized LMDs via coordination bonds. The grafted cyclodextrin and adamantane groups formed dynamic inclusion complexes to bridge two neighboring LMDs, leading to the formation of a dynamically cross-linked network of LMDs in the aqueous phase. The MWEGs exhibited viscoelastic and shear-thinning behavior, making them ideal for direct three-dimensional (3D) and screen printing with a high resolution (∼65 µm) to assemble complex patterns consisting of ∼95 wt % liquid metal. When stretching the printed patterns, strong host-guest interactions guaranteed that the entire droplet network was cross-linked, while the brittle oxide shell of the droplets ruptured, releasing the liquid metal core and allowing it to fuse into continuous conductive pathways under an ultralow critical strain (<1.5%). This strain-activated conductivity exceeded 15800 S/cm under a large strain of 800% and exhibited long-term cyclic stability and robustness.

Highly Sensitive Temperature-Pressure Bimodal Aerogel with Stimulus Discriminability for Human Physiological Monitoring.

Multimodal sensor with high sensitivity, accurate sensing resolution, and stimuli discriminability is very desirable for human physiological state monitoring. A dual-sensing aerogel is fabricated with independent pyro-piezoresistive behavior by leveraging MXene and semicrystalline polymer to assemble shrinkable nanochannel structures inside multilevel cellular walls of aerogel for discriminable temperature and pressure sensing. The shrinkable nanochannels, controlled by the melt flow-triggered volume change of semicrystalline polymer, act as thermoresponsive conductive channels to endow the pyroresistive aerogel with negative temperature coefficient of resistance of -10.0% °C-1 and high accuracy within 0.2 °C in human physiological temperature range of 30-40 °C. The flexible cellular walls, working as pressure-responsive conductive channels, enable the piezoresistive aerogel to exhibit a pressure sensitivity up to 777 kPa-1 with a detectable pressure limit of 0.05 Pa. The pyro-piezoresistive aerogel can detect the temperature-dependent characteristics of pulse pressure waveforms from artery vessels under different human body temperature states.

Tailoring Silver Nanowire Nanocomposite Interfaces to Achieve Superior Stretchability, Durability, and Stability in Transparent Conductors.

Silver nanowires (AgNWs) have been considered as a promising candidate for transparent stretchable conductors (TSCs). However, the strong interface mismatch of stiff AgNWs and elastic substrates leads to the stress concentration at their interface and ultimately the low stretchability and poor durability of TSCs. Here, to address the interfacial mismatch of AgNWs-based TSCs we put forward a universal interface tailoring strategy that introduces the mercapto compound as the intermediate cross-linked layer. The mercapto compound strongly interacts with the AgNWs, forming a dense protective layer on their surface to improve their corrosion resistance, and reacts with the polymer substrate, forming a buffer layer to release the concentrated stress. As a result, the optimized TSCs showed superior stretchability (160%), exceptional durability (230 000 cycles), competent optoelectrical performance (18.0 ohm·sq-1 with a transmittance of 86.5%), and prominent stability. This work provides clear guidance and a strong impetus for the development of transparent stretchable electronics.

Pushing detectability and sensitivity for subtle force to new limits with shrinkable nanochannel structured aerogel.

There is an urgent need for developing electromechanical sensor with both ultralow detection limits and ultrahigh sensitivity to promote the progress of intelligent technology. Here we propose a strategy for fabricating a soft polysiloxane crosslinked MXene aerogel with multilevel nanochannels inside its cellular walls for ultrasensitive pressure detection. The easily shrinkable nanochannels and optimized material synergism endow the piezoresistive aerogel with an ultralow Young's modulus (140 Pa), numerous variable conductive pathways, and mechanical robustness. This aerogel can detect extremely subtle pressure signals of 0.0063 Pa, deliver a high pressure sensitivity over 1900 kPa-1, and exhibit extraordinarily sensing robustness. These sensing properties make the MXene aerogel feasible for monitoring ultra-weak force signals arising from a human's deep-lying internal jugular venous pulses in a non-invasive manner, detecting the dynamic impacts associated with the landing and take-off of a mosquito, and performing static pressure mapping of a hair.

An in situ and rapid self-healing strategy enabling a stretchable nanocomposite with extremely durable and highly sensitive sensing features.

Progress toward the development of wearable electromechanical sensors with durable and reliable sensing performance is critical for emerging wearable integrated electronic applications. However, it remains a long-standing challenge to realize mechanically stretchable sensing materials with extremely durable and high-performing sensing ability due to the fundamental dilemma lying in the sensing mechanism. In this work, we proposed an in situ and rapid self-healing strategy through nano-confining a dynamic host-guest supramolecular polymer network in a graphene-based multilevel nanocomposite matrix to fabricate a mechanically stretchable and structurally healable sensing nanocomposite which is provided with intriguing sensing durability and sensitivity simultaneously. When repeatedly stretching and releasing the nanocomposite sensing film, the fast association kinetics of cyclodextrin and adamantane host-guest inclusion complexes and good polymer chain dynamics in the supramolecular polymer network endowed by the nanoconfinement effect enable autonomous and rapid repair of the micro-cracks in situ generated in the sensing material. As a result, our strain sensing devices can achieve an extremely high durability and retain stable sensing performance even after over 100 000 stretching-releasing cycles at large strain of 50%. Moreover, the brittle nature originated from the inorganically dominated structure in conjunction with the thermodynamically stable host-guest interactions and dynamic hydrogen bonds inside the multilevel nanocomposite allow the sensing material to exhibit an ultrahigh gauge factor over 1500 with a large working strain of 58%. This work presents a reliable approach for the construction of ultradurable and high-performing wearable electronics.

Detection of RAGE expression and its application to diabetic wound age estimation.

With the prevalence of diabetes, it is becoming important to analyze the diabetic wound age in forensic practice. The present study investigated the time-dependent expression of receptor for advanced glycation end products (RAGE) during diabetic wound healing in mice and its applicability to wound age determination by immunohistochemistry, double immunofluorescence, and Western blotting. After an incision was created in genetically diabetic db/db mice and control mice, mice were killed at posttraumatic intervals ranging from 6 h to 14 days, followed by the sampling of wound margin. Compared with control mice, diabetic mice showed the delayed wound healing. In control and diabetic wound specimens, RAGE immunoreactivity was observed in a small number of polymorphonuclear cells (PMNs), a number of macrophages, and fibroblasts. Morphometrically, the positive ratios of RAGE in macrophages or fibroblasts considerably increased in diabetic wounds during late repair, which exceeded 60% at 7 and 10 days post-injury. There were no control wound specimens to show a ratio of >60% in macrophages or fibroblasts. By Western blotting analysis, the ratios of RAGE to GAPDH were >1.4 in all diabetic wound samples from 7 to 10 days post-injury, which were >1.8 at 10 days after injury. By comparison, no control wound specimens indicated a ratio of >1.4. In conclusion, the expression of RAGE is upregulated and temporally distributed in macrophages and fibroblasts during diabetic wound healing, which might be closely involved in prolonged inflammation and deficient healing. Moreover, RAGE is promising as a useful marker for diabetic wound age determination.

Construction of unique six-coordinated titanium species with an organic amine ligand in titanosilicate and their unprecedented high efficiency for alkene epoxidation.

A novel organic-inorganic layered titanosilicate consisting of Ti-containing MWW-type nanosheets and piperidine ligands was constructed. It exhibited an unprecedented high catalytic activity and recyclability in alkene epoxidation.