Iontronic pressure sensors hold great promise for electronic skins and related fields, yet conventional single-microstructure designs struggle to balance sensitivity and linear range, whereas ionic leakage induces signal drift. Herein, we present a highly effective anti-leakage iontronic sensor featuring a surface gradient microcone array. The design leverages the progressive deformation of multilevel microstructures and immobilizes ionic liquids within a thermoplastic polyurethane matrix via hydrogen bonding and electrostatic interactions. By optimizing additives and microstructural parameters, we achieved synergistic control over electromechanical properties and response behavior. The sensor exhibits a high sensitivity of 209 kPa-1 over a wide linear range of 10-200 kPa (R2 = 0.997), an ultralow detection limit of 2 Pa, a high-pressure resolution of 12 Pa under an 8 kPa preload, and a low signal drift rate of 4.6% over 3000 cycles. Applications demonstrated include encrypted Morse code transmission, physiological signal monitoring, joint motion recognition, and detection of 5 to 30 μm microvibrations. This work provides a mechanochemical synergistic strategy for designing high-performance flexible pressure sensors.
The incorporation of thiophene groups into photocatalytic materials has gained increasing attention as a promising strategy for enhancing catalytic performance. However, the specific role of thiophene functionalities in the catalytic process remains unclear. In this work, two isostructural Zn-based metal-organic frameworks (MOFs), ZnTtz-1 and ZnTtz-2, were synthesized on a gram scale from Zn(NO3)2 center dot 6H2O and 5-phenyl-1H-tetrazole (PhTtzH) or 5-(thiophen-2-yl)-1H-tetrazole (ThTtzH), respectively. These MOFs provide an ideal platform for a comparative investigation of the photocatalytic mechanisms in thiophene-functionalized versus thiophene-free systems. Remarkably, ZnTtz-2 exhibited superior photocatalytic activity over ZnTtz-1 in the degradation of rhodamine B (RhB), methyl orange (MO), and tetracycline (TC). Mechanistic studies revealed that the potent radicals-center dot OH play a dominant role in the photodegradation process catalyzed by ZnTtz-2, whereas center dot O2- radicals are the main active species in ZnTtz-1, accounting for the enhanced efficiency of ZnTtz-2. Further analysis indicated that the introduction of thiophene groups leads to a notable modification of the energy band structure, along with a decrease in the band gap width and improved electron-hole separation efficiency. These findings underscore the significant potential of thiophene functionalization in the rational design of MOF-based photo-catalysts with optimized electronic structures.
Laccases are widely utilized in biochemical sensing, food quality monitoring, and pollutant degradation due to their environmentally friendly nature. However, the development of non-copper-based laccase mimics remains limited, and their catalytic mechanisms and practical applications require further investigation. Herein, we incorporate non-metallic boron (B) into manganese (Mn)-based oxides (MBO), endowing the material with exceptional laccase-like activity, free from interference typically induced by extraneous metal sites. Acting as an electron modulator, B increases the electron density of Mn active centers and lowers their average valence state (Mnn-delta), thereby promoting O2 reduction through a non-radical pathway. This electronic regulation alters the catalytic mechanism and lowers the activation energy required for benzoquinone formation. As an efficient laccase mimic, MBO catalyzes the Michael addition between dopamine and resorcinol, yielding a dual-signal product with measurable absorbance and fluorescence. By exploiting the specific coordination and inhibition of MBO by ergothioneine (EGT), a dual-mode sensing detection and molecular logic operation ("AND"-"INH") system was constructed for EGT detection, which achieved high sensitivity, a low detection limit, and excellent operational stability. This work presents a novel strategy for enhancing the laccase-like performance of Mn-based nanozymes through non-metallic doping and applying it to biochemical sensing with logical analysis.
Laccase is a member of the blue multicopper oxidase family,which catalyzes the oxidation of phenolic compounds in the presence of oxygen.As a versatile biocatalyst with broad substrate specificity,laccase holds promise for various applications such as biosensing,environmental remediation,and green catalysis.However,the practical deployment of native laccase is often hindered by the limitations of high production costs and poor operational stability.In the catalytic process of natural laccase,the redox couple between monovalent and divalent copper(Cu2+/Cu+)plays a key role in transferring electrons from the reducing substrate to oxygen molecules.Inspired by this mechanism,layered potassium birnessite(KBir)with remarkable laccase-mimicking activity was synthesized in this work.By utilizing the redox characteristics of the interlayer manganese couple(Mn4+/Mn3+),active center and catalytic function of natural laccase were successfully mimicked.Steady-state kinetic analysis confirmed that KBir had excellent catalytic efficiency,along with good stability under various conditions(Temperature,pH,inorganic salts,and organic solvents),making it a promising alternative to natural laccase.Based on this,KBir was successfully applied to detection of quercetin(QUE),demonstrating great potential in the field of biosensing.This work provided new insights into the rational design of advanced laccase-mimicking enzymes and highlighted their broad application prospects.
The bis(pyrazolyl)borate, Na[(4-EtOOC-3-CF3Pz)2BPh2] (NaL) and its Ag(I) and Cu(I) complexes – [AgL(NCCH3)]n (1) and [CuL(NCCH3)] (2) have been prepared and characterized. The single crystal X-ray diffraction analysis demonstrated that the coordination modes of L− are different in complexes 1 and 2, where the bis(pyrazolyl)borate acts as a µ2-κ2N, N′:κC bridge or a κ2N, N′ chelate, respectively. The two complexes thus adopt different structures: the Ag(I) complex exhibits a chain-like structure, featuring the strong intermolecular AgI–Cphenyl contact of 2.456 Å, while the Cu(I) complex is a discrete mononuclear complex. Furthermore, the preliminary investigations were conducted on the photocatalytic performance of the silver complex toward degradation of an organic dye – Rhodamine B.
Real-time monitoring of mechanical lubrication is essential for predictive maintenance of industrial machinery, yet conventional sensors fail to discern the weak vibration signals that herald early-stage lubrication failure. Here we report an electric double-layer (EDL) capacitive sensor built on a topologically entangled ion gel dielectric. By combining a high monomer concentration with phytic acid (PA) regulation, we obtain an ion gel that exhibits low hysteresis (6.7 +/- 0.3%), and that forms rapidly through photopolymerization without chemical crosslinkers. Simulations reveal that PA converts intramolecular hydrogen bonds into stronger intermolecular "PA-amide" bonds, enhancing segmental mobility while preserving a high entanglement density, the molecular basis for the gel's low modulus and minimal energy dissipation. Digital light processing (DLP) 3D-printed micro-cone arrays further confer exceptional sensitivity (40,000 +/- 8000 kPa(-1)), a symmetrical response time of 89 +/- 8 ms and 92 +/- 10 ms, 1 mu m spatial resolution, and durability over 10,000 cycles. The device resolves microscale vibrations (0-60 mu m) at ultra-low frequencies (2-4 Hz), a regime inaccessible to conventional pressure sensors. Integrated with machine learning, it discriminates oil-lubricated from dry-friction states with an overall accuracy of 90.0% +/- 11%, marking considerable potential for in situ tribological diagnostics and intelligent condition monitoring of industrial machinery.
To improve the durability of aerospace moving parts during sequential/alternating atmosphere conditions, a dense multilayer coating (GO-MXene)LBL10 was deposited on stainless steel substrate by spraying-assisted layerby-layer alternate assembly based on hydrogen bonding. Under different atmospheric conditions, LBL coating presents significantly different wear lives (15,000 cycles in Air, 4200 cycles in N2). Additionally, the transfer film formed after Air-1000 cycles extended wear life of nearly 7000 cycles under N2 atmosphere. And LBL coating exhibited unique dynamic response characteristics under Air-N2 alternating conditions. The outstanding performance lies in MXene's bearing capacity, interface sliding, and secondary lubrication of transfer film, offering novel insights for sustainable lubrication in reusable space-ground transportation systems.
Embodied human-machine interaction (EHMI) is predicated on the utilization of human motion signals as a medium of communication, with the objective of achieving a more natural, immersive, intuitive, and efficient interactive experience. The utilization of flexible hydrogel sensors as the EHMI core perception device remains limited due to discomfort caused by heavy loads and mechanical constraints. The present study developed a novel low-constraint wearable hydrogel sensor patch (LCWHSP) based on the remote sensing mechanism of bionic spiders. The innovative integration of a Fenton-like reaction into light-curing 3D printing technology has facilitated the collaborative optimization of the printability and performance parameters of graphene-Fe3+ dynamically coordinated sodium alginate-polyacrylamide (GFSP) double crosslinked hydrogel sensitive materials. The cross-shaped structure design of the LCWHSP enables single-point multidimensional sensing on the skin interface, thereby effectively reducing the sensation of wearing a foreign object caused by high-density sensor arrays. High-precision recognition of hand movements was achieved by utilizing a signal acquisition system and a deep learning analysis model (with an accuracy rate of 98.60%). Further using in typical EHMI scenarios, such as controlling virtual interfaces and manipulating robotic arms, fully validated its practical application potential.
To address the need for friction-controllable interfaces in intelligent equipment and engineering, an anisotropic graphene oxide (GO) aerogel/epoxy resin composite (GA/EP) was developed in this study, which exhibits anisotropic trends in thermal conductivity, mechanical and tribological properties. The top side (T) of the GA/EP composite exhibits optimal tribological performance with a low coefficient of friction (COF) of 0.063 due to its higher thermal conductivity and elastic modulus than lateral side. The COF of lateral axis (LA) direction is 0.095, while that of lateral radial (LR) direction is 0.660. Molecular dynamics simulation results indicate that the low friction stress remains stable at 20-40 atmospheres (atm) in the LA direction that favors the formation of shear-friendly interfaces by reducing interactions between GA/EP and the counterpart, whereas LR's abrupt stress (50,000-100,000 atm) increase disrupts lubrication. This research meets the demand for differentiated dynamic COF, enhancing the potential of intelligent precision equipment in practical engineering applications.
The cyclic triangular complex - silver (I) 4-nitro-3,5-bis(trifluoromethyl)pyrazolate (Ag3pz3) with super π-acidity shows great potential in adsorptive desulfurization (ADS) as a novel adsorbent, however, it fails to work well in the continue flow adsorption study. In order to improve its dynamic adsorption performance, a composite has been prepared by mixing Ag3pz3 and multilayer graphene (MG) in methanol. Based on the results of characterization by FT-IR, XPS, SEM, and so on, the optimal mass ratio of Ag3pz3:MG in the synthesis is 0.14, so composite obtained under this condition is labeled as Ag3pz3/MG-0.14, in which the molecules of Ag3pz3 are uniformly distributed on the surface of MG via Ag∙∙∙C interactions and π-π stacking. The composite exhibits higher specific surface area than that of Ag3pz3. Importantly, the column test proves the practicality of the composite - Ag3pz3/MG-0.14 in continuous flow desulfurization with the enhanced dynamic capacity (4.0 mg S/g), in comparison with 1.9 mg S/g for graphene (C0 = 200 mg S/L for dibenzothiophene in iso-octane, madsorbent = 0.5 g, T = 298 K, v = 0.1 mL∙min-1). This work confirms the importance and advantage of the integration of functional coordination compound and suitable supporting materials for designing new type of high-performance ADS adsorbents.
The piezoresistive effect serves as a key mechanical sensing mechanism extensively utilized across diverse sensing applications. Piezoresistive stress-strain sensors stand out due to their straightforward design, high sensitivity, low energy requirements, and versatile functionality, making them particularly promising for the advancement of wearable flexible electronics. These sensors are poised to become a foundational technology in the evolution of digital healthcare. In this Perspective, we comprehensively summarize recent advancements and innovative uses of flexible piezoresistive sensing technologies. First, we theoretically characterize the charge transport models of the piezoresistive effect in flexible substrates, including the quantum tunneling effect, microcrack propagation mechanism, and contact resistance theory. We then comprehensively elucidate the structure-performance relationships of five major material systems: micro/nanoarchitectured materials, flexible conductive aerogels, biocompatible soft hydrogels, smart responsive fabrics, and conductive paper-based devices. Furthermore, we highlight the breakthrough applications of this technology in digital healthcare, exemplified by high-precision wearable physiological signal monitoring systems, intelligent prosthetic tactile feedback devices, and advanced postoperative rehabilitation assessment platforms. Finally, we discuss future directions, emphasizing the integration of machine learning to enhance flexible sensing systems for personalized precision medicine and remote intelligent healthcare solutions.
Graphene aerogel (GA) has attracted wide attention for its potential applications in various fields. However, the graphene nanosheets in the GA framework often exhibit insufficient adhesion and interfacial contact due to weak interactions, resulting in fragile cell walls and poor structural stability. Here, inspired by the principle of "soft-hard" compounding, a class of GA with extraordinary structural stability and mechanical property was prepared based on the in-situ bonding interfacial engineering between different phases in Pickering emulsion. Through interfacial engineering, the fatal compounding drawback between fusing oily polymer soft chains and water-soluble hard graphene oxide (GO) nanosheets is resolved, which enables polydimethylsiloxane (PDMS) chains to in-situ adhere onto GO nanosheets, eventually resulting in compelling structural-stable PDMS/GO aerogel (PGOA) backbone. Later, PDMS/GA (PGA) can be easily obtained by simple reduction of PGOA. The obtained PGA achieves excellent structural stability, 97.5 % elasticity, 1.7 MPa compressive capacity, and unprecedented isotropic characteristics. The assembled flexible sensor based on PGA has a high sensitivity of 17.08 kPa(-1). Additionally, PGA has low thermal conductivity (0.0245-0.0301 W/(m center dot K)) and good flame retardancy (similar to 1000 degrees C). Because of these excellent properties, PGA has a wide range of potential applications in areas such as flexible sensing, thermal protection, and fire detection.
Hydrogels, owing to their excellent biocompatibility, high water content, and adjustable physicochemical properties, have become indispensable biomaterials in the field of 3D printing. The dynamic boronic ester bond is a reversible covalent bond that can form and dissociate under specific conditions, endowing materials with robust self-healing capabilities and high sensitivity to external stimuli. By carefully designing materials utilizing dynamic boronic ester bonding, we developed an innovative polymer hydrogel that combines high stability and dynamic characteristics. Specifically, 3-aminophenylboronic acid (PBA) was successfully grafted onto the natural polysaccharide sodium alginate (SA), resulting in the SA-PBA moiety. Dynamic boronic ester bonds were then formed by combining SA-PBA with polyvinyl alcohol (PVA) and MXene (Ti3C2Tx), ultimately yielding SA-PBA/PVA/MXene 3D printable hydrogel ink (SPPM-h). The incorporation of MXene was intended to enhance the conductivity of the hydrogel. After thoroughly characterizing the composition and structure of SPPM-h, we conducted an in-depth evaluation of its key properties, including rheological behavior, self-healing ability, and tensile performance. SPPM-h exhibited remarkable self-healing properties, achieving complete self-repair within just 30 s after fracture-significantly faster than some hydrogels reported in the literature, which require up to 24 h for repair. The conductivity of SPPM-h 3D printing hydrogel ink is approximately 0.034 S/m. Additionally, it demonstrates good adhesion on various types of surfaces, offering broad prospects for applications in direct ink writing 3D printing.
Pure epoxy resin (EP) coating exhibits poor wear resistance and weak corrosion protection capability, resulting in short service life. In this work, MoS2@polymethyl methacrylate (MoS2@PMMA) core-shell hybrid was firstly synthesized by emulsion polymerization, which demonstrated stability in high humidity conditions attributing to reduced MoS2 oxidation. As an additive, the tribological performances of MoS2@PMMA/EP coating at different humidity and its anti-corrosive property were explored. Under high humidity, the MoS2@PMMA/EP coating exhibited the lowest friction coefficient (0.36) compared with EP coating (0.49) and MoS2/EP coating (0.56). Especially, the wear rate of the MoS2@PMMA/EP reduced by 95.07 % and 93.22 % as to EP coating and MoS2/ EP coating, respectively. Furthermore, electrochemical tests showed the MoS2@PMMA could enhanced the corrosion resistance of the EP matrix.
To advance the performance of electrocatalysts for the oxygen evolution reaction (OER), it is crucial to improve reactive site accessibility, conductivity, and reaction kinetics through the incorporation of heteroatom and optimizing pore architectures. In this study, we present a scalable synthesis strategy to fabricate nitrogen and chalcogens containing porous MOFs for OER electrocatalysts. The two-dimensional MOF with optimized chalcogens-based 3,5-di-substituted-1,2,4-triazole ligands exhibits strong synergistic effects, resulting in improved OER accomplishment with a low overpotential (eta) of 107 mV at 10 mA cm-2 and remarkable durability extending up to 100 h in alkaline conditions. The optimization of thiophene content within the framework, confirmed by comprehensive physical and electrochemical characterization, enhances conductivity and increases active sites, driving remarkable catalytic activity. Density functional theory (DFT) calculations further elucidate the impact of thiophene on the OER reaction, underscoring the potential of thiophene-based triazolate MOFs as promising candidates for sustainable and efficient water oxidation.
Non-metallic pipelines have been widely used in various fields due to their numerous advantages. However, long-term use can lead to aging, cracking, or internal defects, which pose threats to the safe operation of the pipelines. In this paper, a square ring resonator is designed and integrated with the conventional microwave reflection detection method. The effectiveness of the square ring resonator in detecting pipeline defects is verified through simulation by setting the relative permittivity of the pipeline to different values to simulate defects. The simulation results demonstrate that the average sensitivity of the resonator is approximately 8.5% higher than that without a resonator, and it can effectively identify pipeline defects.
Adsorptive desulfurization (ADS) is a promising technique for producing clean fuels with ultra-low sulfur, and various metal-functionalized adsorbents for desulfurization have been successively investigated. Unfortunately, ADS usually suffers from the low adsorptive selectivity in the presence of organic competitors. Herein, we report the triangular copper(I) 4-nitro-3,5-di(trifluoromethyl)pyrazolate (Cu(3)pz(3)) as a novel adsorbent to achieve a high selectivity via short Cu(I) - sulfur bond, the S-content (as DBT) can be reduced from 100 mg S/L to similar to 9 mg S/L in the toluene-iso-octane model oil (v:v = 15:85) after a static adsorption at 298 K under the adsorbent dose of 3.65 g/L, which is much better than the adsorption performance exhibited by a structurally similar adsorbent - Ag(3)pz(3) (reduced from 100 mg S/L to similar to 56 mg S/L at the same condition). Furthermore, the adsorption mechanism has been investigated at the molecular level, unveiling a correlation between the ADS selectivity and the strength of Cu(I) - S bonding. Finally, some molecular design strategies have been proposed for further improvement of the performance of ADS adsorbent.
Polydimethylsiloxane (PDMS) is known for its exceptional mechanical stability, chemical resistance, and biocompatibility, making it highly suitable for flexible sensors. However, its inherently insulating properties limit its direct application as a sensing material, and its hydrophobic nature poses challenges for effective integration with conductive materials. To overcome these challenges, the present study proposes an innovative strategy that utilizes PDMS as the matrix material while MXene as a conductive filler, aiming to fabricate PDMS aerogels through a Pickering emulsion method. In this process, MXene nanosheets are first functionalized with sodium carboxymethyl cellulose (CMC), enhancing both emulsification and gelation to stabilize the Pickering emulsion composed of PDMS and MXene. Simultaneously, the modified MXene nanosheets act as precursors for constructing the aerogel framework. This method not only promotes the formation of a robust 3D PDMS network but also creates a stable, efficient conductive pathway using MXene nanosheets. The resulting aerogels exhibit remarkable flexibility, elasticity (>90 %), and compressive strength (9.3 MPa). Therefore, with a high sensitivity of 28.7 kPa(-1 )and exceptional electromechanical performance, the PCM sensor is well-suited for applications in human health detection and mechanical equipment monitoring. Furthermore, the PCM sensor can also be integrated with robotic arm for intelligent sensing tasks, showcasing significant potential for next-generation smart devices.
Efficiently enhancing the activity and selectivity of targeted nanozymes is a challenging task, primarily due to the inherent structural stability and heterogeneous atomic composition of traditional nanozymes. Herein, theoretical design is carried out to select Fe-based oxides (FO) nanozymes with high peroxidase (POD)-like activity by incorporating different nonmetallic atoms (N, P, S, and B). Among these dopants, B emerged as a superior candidate because it could effectively tune the adsorption energies of *OH intermediates and *H2O2, thereby endowing the nanozymes with superior POD-like performance. Leveraging this insight, Bdoped Fe-based oxides (FOB) is successfully synthesized, demonstrating remarkable POD-like activity and ultrafast reaction kinetics. Mechanistic investigations revealed that B doping enhances electron transfer and intermediate adsorption by increasing the electron density and reducing the coordination number of the Fe center, concomitantly lowering the energy barrier for hydroxyl radical (·OH) formation and the rate-determining step. As a proof of concept, a three-enzyme cascade colorimetric biosensor integrating acetylcholinesterase (AChE)-choline oxidase (ChOx)-POD is constructed to perform ultrasensitive and selective detection of AChE activity and inhibitors. This study establishes a novel framework for designing high enzyme-mimicking performance transition-metal oxide nanozymes with doping nonmetallic atoms, provoking an inspiration for the rational design of nanozymes by regulating the electronic and coordination environment.
This paper presents an ultra-wideband plasmonic metamaterial absorber (MA) based on a patterned transparent resistive film. The absorber adopts a four-layer structure: a transparent compensating layer, a patterned transparent resistive film, a transparent dielectric layer, and a transparent reflective base plate. Simulation results indicate that the absorber achieves over 80% microwave absorption in the frequency ranges of 11.8–22.7 GHz and 23.9–41 GHz, with a working bandwidth of 28 GHz. It also maintains good broadband absorption under oblique electromagnetic wave incidence (at a 45° incidence angle). Experimental results show a good match with the simulations. This work is significant for designing ultra-wideband plasmonic metamaterial absorbers and applying them in electromagnetic shielding.