The 100 most-cited articles in ACS Applied Materials & Interfaces, 2019

For the development of next-generation lithium batteries, major research effort is made to enable a reversible lithium metal anode by the use of solid electrolytes. However, the fundamentals of the solid–solid interface and especially the processes that take place under current load are still not well characterized. By measuring pressure-dependent electrode kinetics, we explore the electrochemo-mechanical behavior of the lithium metal anode on the garnet electrolyte Li 6.25 Al 0.25 La 3 Zr 2 O 12 . Because of the stability against reduction in contact with the lithium metal, this serves as an optimal model system for kinetic studies without electrolyte degradation. We show that the interfacial resistance becomes negligibly small and converges to practically 0 Ω·cm 2 at high external pressures of several 100 MPa. To the best of our knowledge, this is the smallest reported interfacial resistance in the literature without the need for any interlayer. We interpret this observation by the concept of constriction resistance and show that the contact geometry in combination with the ionic…

Oil leakage and the discharge of oil/water mixtures by domestic and industrial consumers have caused not only severe environmental pollution and a threat to all species in the ecosystem but also a huge waste of precious resources. Therefore, the separation of oil/water mixtures, especially stable emulsion, has become an urgent global issue. Recently, materials containing a special wettability feature for oil and water have drawn immense attention because of their potential applications for oil/water separation application. In this paper, we systematically summarize the fundamental theories, separation mechanism, design strategies, and recent developments in materials with special wettability for separating stratified and emulsified oil/water mixtures. The related wetting theories that unveil the physical underlying mechanism of the oil/water separation mechanism are proposed, and the practical design criteria for oil/water separation materials are provided. Guided by the fundamental design criteria, various porous materials with special wettability characteristics, including those…

Lightweight absorption-dominated electromagnetic interference (EMI) shielding materials are more attractive than conventional reflection-dominated counterparts because they minimize the twice pollution of the reflected electromagnetic (EM) wave. Here, porous Ti 2 CT x MXene/poly(vinyl alcohol) composite foams constructed by few-layered Ti 2 CT x (f-Ti 2 CT x ) MXene and poly(vinyl alcohol) (PVA) are fabricated via a facile freeze-drying method. As superior EMI shielding materials, their calculated specific shielding effectiveness reaches up to 5136 dB cm 2 g –1 with an ultralow filler content of only 0.15 vol % and reflection effectiveness (SE R ) of less than 2 dB, representing the excellent absorption-dominated shielding performance. Contrast experiment reveals that the good impedance matching derived from the multiple porous structures, internal reflection, and polarization effect (dipole and interfacial polarization) plays a synergistic role in the improved absorption efficiency and superior EMI shielding performance. Consequently, this work provides a promising MXene-based EMI…

An ultrahigh sensitive capacitive pressure sensor based on a porous pyramid dielectric layer (PPDL) is reported. Compared to that of the conventional pyramid dielectric layer, the sensitivity was drastically increased to 44.5 kPa –1 in the pressure range <100 Pa, an unprecedented sensitivity for capacitive pressure sensors. The enhanced sensitivity is attributed to a lower compressive modulus and larger change in an effective dielectric constant under pressure. By placing the pressure sensors on islands of hard elastomer embedded in a soft elastomer substrate, the sensors exhibited insensitivity to strain. The pressure sensors were also nonresponsive to temperature. Finally, a contact resistance-based pressure sensor is also demonstrated by chemically grafting PPDL with a conductive polymer, which also showed drastically enhanced sensitivity.

Developing a facile, cost-saving, and environment-friendly method for fabricating a multifunctional humidity sensor is of great significance to expand its practical applications. However, most humidity sensors involve a complex fabrication process, resulting in their high cost and narrow application fields. Herein, a multifunctional paper-based humidity sensor with many advantages is proposed. This humidity sensor is fabricated using conventional printing paper and flexible conductive adhesive tape by a facile pasting method, in which the paper is used as both the humidity-sensing material and the substrate of the sensor. Owing to the moderate hydrophilicity of the paper and the rational structure design of the paper-based humidity sensor, the sensor exhibits an excellent humidity-sensing response of more than 10 3 as well as good linearity ( R 2 = 0.9549) within the humidity range from 41.1 to 91.5% relative humidity. Furthermore, the paper-based humidity sensor has good flexibility and compatibility, endowing it with multifunctional applications for breath rate, baby diaper…

Self-healing, adhesive conductive hydrogels are of great significance in wearable electronic devices, flexible printable electronics, and tissue engineering scaffolds. However, designing self-healing hydrogels with multifunctional properties such as high conductivity, excellent mechanical property, and high sensitivity remains a challenge. In this work, the conductive self-healing nanocomposite hydrogels based on nanoclay (laponite), multiwalled carbon nanotubes (CNTs), and N-isopropyl acrylamide are presented. The presented nanocomposite hydrogels displayed good electrical conductivity, rapid self-healing and adhesive properties, flexible and stretchable mechanical properties, and high sensitivity to near-infrared light and temperature. These excellent properties of the hydrogels are demonstrated by the three-dimensional (3D) bulky pressure-dependent device, human activity monitoring device, and 3D printed gridding scaffolds. Good cytocompatibility of the conductive hydrogels was also evaluated with L929 fibroblast cells. These nanocomposite hydrogels have great potential for…

Sensitivity of the sensor is of great importance in practical applications of wearable electronics or smart robotics. In the present study, a capacitive sensor enhanced by a tilted micropillar array-structured dielectric layer is developed. Because the tilted micropillars undergo bending deformation rather than compression deformation, the distance between the electrodes is easier to change, even discarding the contribution of the air gap at the interface of the structured dielectric layer and the electrode, thus resulting in high pressure sensitivity (0.42 kPa –1 ) and very small detection limit (1 Pa). In addition, eliminating the presence of uncertain air gap, the dielectric layer is strongly bonded with the electrode, which makes the structure robust and endows the sensor with high stability and reliable capacitance response. These characteristics allow the device to remain in normal use without the need for repair or replacement despite mechanical damage. Moreover, the proposed sensor can be tailored to any size and shape, which is further demonstrated in wearable application.…

Electromagnetic (EM) pollution affecting people’s normal lives and health has attracted considerable attention in the current society. In this work, a promising EM wave absorption and shielding material, MXene/Ni hybrid, composed of one-dimensional Ni nanochains and two-dimensional Ti 3 C 2 T x nanosheets (MXene), is successfully designed and developed. As expected, excellent EM wave absorption and shielding properties are obtained and controlled by only adjusting the MXene content in the hybrid. A minimum reflection loss of −49.9 dB is obtained only with a thickness of 1.75 mm at 11.9 GHz when the MXene content is 10 wt %. Upon further increasing the MXene content to 50 wt %, the optimal EM shielding effectiveness (SE) reaches 66.4 dB with an absorption effectiveness (SE A ) of 59.9 dB. Mechanism analysis reveals that the excellent EM wave absorption and shielding performances of the hybrid are contributed to the synergistic effect of conductive MXene and magnetic Ni chains, by which, the dielectric properties and electromagnetic loss can be easily controlled to obtain appropriate…

Lightweight and high-efficiency microwave attenuation are two major challenges in the exploration of carbon-based absorbers, which can be achieved simultaneously by manipulating their chemical composition, microstructure, or impedance matching. In this work, core–shell CoNi@graphitic carbon decorated on B,N-codoped hollow carbon polyhedrons has been constructed by a facile pyrolysis process using metal–organic frameworks as precursors. The B,N-codoped hollow carbon polyhedrons, originated from the calcination of Co-Ni-ZIF-67, are composed of carbon nanocages and BN domains, and CoNi alloy is encapsulated by graphitic carbon layers. With a filling loading of 30 wt %, the absorber exhibits a maximum R L of −62.8 dB at 7.2 GHz with 3 mm and the effective absorption bandwidth below −10 dB remarkably reaches as strong as 8 GHz when the thickness is only 2 mm. The outstanding microwave absorption performance stems from the hollow carbon polyhedrons and carbon nanocages with interior cavities, the synergistic coupling effect between the abundant B–C–N heteroatoms, the strong…

High-performance flexible pressure sensors are highly desirable in health monitoring, robotic tactile, and artificial intelligence. Construction of microstructures in dielectrics and electrodes is the dominating approach to improving the performance of capacitive pressure sensors. Herein, we have demonstrated a novel three-dimensional microconformal graphene electrode for ultrasensitive and tunable flexible capacitive pressure sensors. Because the fabrication process is controllable, the morphologies of the graphene that is perfectly conformal with the electrode are controllable consequently. Multiscale morphologies ranging from a few nanometers to hundreds of nanometers, even to tens of micrometers, have been systematically investigated, and the high-performance capacitive pressure sensor with high sensitivity (3.19 kPa –1 ), fast response (30 ms), ultralow detection limit (1 mg), tunable-sensitivity, high flexibility, and high stability was obtained. Furthermore, an ultrasensitivity of 7.68 kPa –1 was successfully achieved via symmetric double microconformal graphene electrodes.…

The big challenging issues in photocatalytic H 2 evolution are efficient separation of the photoinduced carriers, the stability of the catalyst, enhancing quantum efficiency, and requiring photoinduced electrons to enrich on photocatalysts’ surface. Herein, Ti 3 C 2 MXene quantum dots (QDs) possess the activity of Pt as a co-catalyst in promoting the photocatalytic H 2 evolution to form heterostructures with g-C 3 N 4 nanosheets (NSs) (denoted g-C 3 N 4 @Ti 3 C 2 QDs). The photocatalytic H 2 evolution rate of g-C 3 N 4 @Ti 3 C 2 QD composites with an optimized Ti 3 C 2 QD loading amounts (100 mL) is nearly 26, 3 and 10 times higher than pristine g-C 3 N 4 NSs, Pt/g-C 3 N 4, and Ti 3 C 2 MXene sheet/g-C 3 N 4, respectively. The Ti 3 C 2 QDs increase the specific surface area of g-C 3 N 4 and boost the density of the active site. Besides, metallic Ti 3 C 2 QDs possess excellent electronic conductivity, causing the improvement of carrier transfer efficiency.

With the rapid development of flexible wearable electronics, a piezoresistive sensor with low detection limit and wide strain sensing range turns out to be a great challenge for its application in this field. Here, a cracked cellulose nanofibril/silver nanowire (CA) layer-coated polyurethane (PU) sponge was acquired through a simple dip-coating process followed by precompression treatment. The electrical conductivity and mechanical property of the conductive CA@PU sponge could be effectively tuned through changing the dip-coating number. As a piezoresistive sensor, the sponge exhibited the capability of detecting both small and large motions over a wide compression strain range of 0–80%. Based on the “crack effect”, the sensor possessed a detection limit as low as 0.2% and the gauge factor [GF, GF = (Δ R / R 0 )/ε, where Δ R, R 0, and ε represent the instantaneous resistance change, original resistance, and strain applied, respectively] was as high as 26.07 in the strain range of 0–0.6%. Moreover, the “contact effect” enabled the sensor to be applicable for larger strain, and the GF…

Flexible, stretchable, and bendable materials, including inorganic semiconductors, organic polymers, graphene, and transition metal dichalcogenides (TMDs), are attracting great attention in such areas as wearable electronics, biomedical technologies, foldable displays, and wearable point-of-care biosensors for healthcare. Among a broad range of layered TMDs, atomically thin layered molybdenum disulfide (MoS 2 ) has been of particular interest, due to its exceptional electronic properties, including tunable bandgap and charge carrier mobility. MoS 2 atomic layers can be used as a channel or a gate dielectric for fabricating atomically thin field-effect transistors (FETs) for electronic and optoelectronic devices. This review briefly introduces the processing and spectroscopic characterization of large-area MoS 2 atomically thin layers. The review summarizes the different strategies in enhancing the charge carrier mobility and switching speed of MoS 2 FETs by integrating high-κ dielectrics, encapsulating layers, and other 2D van der Waals layered materials into flexible MoS 2 device…

Ambient particulate matter pollution has posed serious threats to global environment and public health. However, highly efficient filtration of submicron particles, the so-named “secondary pollution” caused by, e.g., bacterial growth in filters and the use of nondegradable filter materials, remains a serious challenge. In this study, poly(vinyl alcohol) (PVA) and konjac glucomannan (KGM)-based nanofiber membranes, loaded with ZnO nanoparticles, were prepared through green electrospinning and ecofriendly thermal cross-linking. Thus obtained fibrous membranes not only show highly efficient air-filtration performance but also show superior photocatalytic activity and antibacterial activity. The filtration efficiency of the ZnO@PVA/KGM membranes for ultrafine particles (300 nm) was higher than 99.99%, being superior to that of commercial HEPA filters. By virtue of the high photocatalytic activity, methyl orange was efficiently decolorized with a removal efficiency of more than 98% at an initial concentration of 20 mg L –1 under 120 min of solar irradiation. A multifunctional membrane…

Nanozyme/natural enzyme hybrid plays a vital role in biosensing, therapy, and catalysis owing to the integrated advantages in the selectivity of natural enzymes and controllable catalytic activity of nanozymes. Herein, Fe-MIL-88B-NH 2 [(Fe-metal–organic framework (MOF)] with remarkable peroxidase-like activity, ultrahigh stability, and high biocompatibility was utilized for immobilization of glucose oxidase (GOx) via an amidation coupling reaction. On the basis of the excellent selectivity and catalytic activity of Fe-MOF-GOx, a cascade catalysis was performed for the colorimetric detection of glucose. The integrated Fe-MOF-GOx not only exhibited higher stability and reusability than their mixtures including Fe-MOF and free GOx system but also possessed a wide linear range (1–500 μM), with a low detection limit of 0.487 μM for glucose detection.

Environmental contamination is a major global challenge and the effects of contamination are found in most habitats. In recent times, the pollution by microplastics has come to the global attention and their removal displays an extraordinary challenge with no reasonable solutions presented so far. One of the new technologies holding many promises for environmental remediation on the microscale are self-propelled micromotors. They present several properties that are of academic and technical interest, such as the ability to overcome the diffusion limitation in catalytic processes and their phoretic interaction with their environment. Here, we present two novel strategies for the elimination of microplastics using photocatalytic Au@Ni@TiO2 -based micromotors. We show that individual catalytic particles as well as assembled chains show excellent collection and removal of suspended matter and microplastics from natural water samples.

Making full use of the interface modulation-induced interface polarization is an effective strategy to achieve excellent microwave absorption (MA). In this study, we develop an interfacial modulation strategy for achieving this goal in the commonly reported dielectric carbon nanotubes@polyaniline (CNTs@PANi) hybrid microwave absorber by optimizing the CNT nanocore structure. The heterogeneous interfaces from PANi and CNTs can be well regulated by longitudinal unzipping of the walls of CNTs to form 1D CNT- and 3D CNT-bridged graphene nanoribbons and 2D graphene nanoribbons. By controlling the oxidation peeling degree of CNTs, their interface area and defects are enhanced, thus producing more polarization centers to generate interfacial polarization and polarization relaxation, and also introducing more PANi loadings. Furthermore, more interface contact area can be produced between CNTs and PANi. This could induce a strong dielectric resonant and further improve the impedance matching, leading to significant enhancement of MA performance. With filler loading of only 10 wt % and a…

Designing of an efficient heterostructure photocatalyst for photocatalytic organic pollutant removal and H 2 production has been a subject of rigorous research intended to solve the related environmental aggravation and enormous energy crises. Z-scheme-based charge-transfer dynamics in a p–n heterostructure could significantly replicate the inherent power of natural photosynthesis, which is the key point to affect the transportation of photoinduced exciton pairs. In this finding, a series of p-type MoS 2 loaded with n-type NiFe-layered double hydroxide (LDH) forming a heterostructure MoS 2 /NiFe LDH were designed by electrostatic self-assembled chemistry and an in situ hydrothermal strategy for photocatalytic rhodamine B (RhB) dye degradation and H 2 production. The creation of p–n heterojunctions of type-II and Z-scheme mode of charge transfer modified the optical and electronic property of the as-synthesized MSLDH3, thereafter promoting the generation, separation, and migration of photoinduced electron–hole pairs. The as-synthesized MSLDH3 showed superior photocatalytic activities…

Aramid nanofiber (ANF) paper has shown potential applications in flexible electronics. However, its inherent low thermal conductivity coefficient (λ) values might threaten the safety of devices under a high-power working condition. In this work, polydopamine-functionalized boron nitride nanosheet (BNNS@PDA)/ANF thermally conductive composite papers with nacre-mimetic layered structures were prepared via highly efficient vacuum-assisted filtration followed by hot pressing. For a given BNNS loading, the surface functionalization of BNNS could further enhance the thermal conductivities and mechanical properties of BNNS@PDA/ANF composite papers. BNNS@PDA/ANF composite papers presented anisotropic thermal conductivities, and the through-plane (λ ⊥ ) and in-plane (λ ∥ ) values of the 50 wt % BNNS@PDA/ANF composite papers reached 0.62 and 3.94 W/mK, 181.8 and 196.2% higher than those of original ANF paper, respectively, which were also higher than those of 50 wt % BNNS/ANF composite papers (λ ⊥ = 0.52 W/mK and λ ∥ = 3.33 W/mK). The tensile strength of the 50 wt % BNNS@PDA/ANF composite…

High-performance flexible strain and pressure sensors are important components of the systems for human motion detection, human-machine interaction, soft robotics, electronic skin, etc., which are envisioned as the key technologies for applications in future human healthcare monitoring and artificial intelligence. In recent years, highly flexible and wearable strain/pressure sensors have been developed based on various materials/structures and transduction mechanisms. Piezoresistive three-dimensional (3D) monolithic conductive sponge, the resistance of which changes upon external pressure or stimuli, has emerged as a forefront material for flexible and wearable pressure sensor due to its excellent sensor performance, facile fabrication, and simple circuit integration. This review focuses on the rapid development of the piezoresistive pressure sensors based on 3D conductive sponges. Various piezoresistive conductive sponges are categorized into four different types and their material and structural characteristics are summarized. Methods for preparation of the 3D conductive sponges…

Flexible and wearable pressure sensors are of paramount importance for the development of personalized medicine and electronic skin. However, the preparation of easily disposable pressure sensors is still facing pressing challenges. Herein, we have developed an all paper-based piezoresistive (APBP) pressure sensor through a facile, cost-effective, and environmentally friendly method. This pressure sensor was based on a tissue paper coated with silver nanowires (AgNWs) as a sensing material, a nanocellulose paper (NCP) as a bottom substrate for printing electrodes, and NCP as a top encapsulating layer. The APBP pressure sensor showed a high sensitivity of 1.5 kPa –1 in the range of 0.03–30.2 kPa and retained excellent performance in the bending state. Furthermore, the APBP sensor has been mounted on the human skin to monitor physiological signals (such as arterial heart pulse and pronunciation from throat) and successfully applied as a soft electronic skin to respond to the external pressure. Due to the use of the common tissue paper, NCP, AgNWs, and conductive nanosilver ink only,…

Lightweight materials with high electrical conductivity and robust mechanical properties are highly desirable for electromagnetic interference (EMI) shielding in modern portable and highly integrated electronics. Herein, a three-dimensional (3D) porous Ti 3 C 2 T x /carbon nanotube (CNT) hybrid aerogel was fabricated via a bidirectional freezing method for lightweight EMI shielding application. The synergism of the lamellar and porous structure of the MXene/CNT hybrid aerogels contributed extensively to their excellent electrical conductivity (9.43 S cm –1 ) and superior electromagnetic shielding effectiveness (EMI SE) value of 103.9 dB at 3 mm thickness at the X-band frequency, the latter of which is the best value reported for synthetic porous nanomaterials. The CNT reinforcement in the MXene/CNT hybrid aerogels enhanced the mechanical robustness and increased the compressional modulus by 9661% relative to that of the pristine MXene aerogel. The hybrid aerogel with high electrical conductivity, good mechanical strength, and superior EMI shielding performance is a promising…

Wearable pressure sensors are in great demand with the rapid development of intelligent electronic devices. However, it is still a huge challenge to obtain high-performance pressure sensors with high sensitivity, wide response range, and low detection limit simultaneously. Here, a polyimide (PI)/carbon nanotube (CNT) composite aerogel with the merits of superelastic, high porosity, robust, and high-temperature resistance was successfully prepared through the freeze drying plus thermal imidization process. Benefiting from the strong chemical interactions between PI and CNT and stable electrical property, the composite aerogel exhibits versatile and superior brilliant sensing performance, which includes wide sensing range (80% strain, 61 kPa), ultrahigh sensitivity (11.28 kPa –1 ), ultralow detection limit (0.1% strain, <10 Pa), fast response time (50 ms) and recovery time (70 ms), remarkable long-term stability (1000 cycles), and exceptional detection ability toward different deformations (compression, distortion, and bending). Furthermore, the composite aerogel also shows stable…

Metal-organic framework (MOF)-derived composites on the microwave absorption have received extensive attention. However, which kind of organic ligand corresponding MOF derivative has better electromagnetic wave absorption performance is an urgent problem to be solved. In this work, two kinds of Ni@C derived from the Ni-based MOFs with two kinds of organic ligands (dimethylimidazole as a ligand named as Ni-ZIF and trimesic acid as a ligand named as Ni-BTC) were successfully obtained. The compositions, morphologies, and electromagnetic properties of two composites were well controlled. As a result, both kinds of Ni@C exhibited the good microwave absorption properties. Comparatively speaking, the Ni@C derived from Ni-ZIF performs better. The Ni@C-ZIF microspheres with a 40% mass filling ratio exhibited a strong reflection loss of -86.8 dB at 13.2 GHz when the matching thickness was 2.7 mm, and the corresponding effective absorption bandwidth was 7.4 GHz (4-11.4 GHz) with the thickness ranging from 1.5 to 4.0 mm. The impedance matching, multiple reflection, and interfacial polarization…

A recent report from the United Nations has warned about the excessive CO 2 emissions and the necessity of making efforts to keep the increase in global temperature below 2 °C. Current CO 2 capture technologies are inadequate for reaching that goal, and effective mitigation strategies must be pursued. In this work, we summarize trends in materials development for CO 2 adsorption with focus on recent studies. We put adsorbent materials into four main groups: (I) carbon-based materials, (II) silica/alumina/zeolites, (III) porous crystalline solids, and (IV) metal oxides. Trends in computational investigations along with experimental findings are covered to find promising candidates in light of practical challenges imposed by process economics.

Organic ligands and metal ions in the metal-organic frameworks (MOFs, a type of porous magnetic metal/carbon nanocomposites obtained through high-temperature carbonization) have caused widespread concerns in the field of microwave absorption because of the existence of various microwave loss mechanisms in these materials. However, MOF-driven microwave absorbing materials with high absorption intensity and wide absorption band still require further research and development. In this work, hollow sphere trimetallic FeCoNi@C microwave absorbing materials via high-temperature carbonization were obtained using FeCoNi-based MOF-74 (FeCoNi-MOF) as the precursor. The effects of different carbonization conditions on the microwave absorption properties of the materials were studied. FeCoNi-MOF-74 annealed at 700 °C showed superior microwave absorption capacity, where the RL value reached -64.75 dB at 15.44 GHz corresponding to the actual application thickness of the absorber (only 2.1 mm), and the minimum RL values reached -69.03 dB at 5.52 GHz. Furthermore, the as-prepared sample can fully…

Flexible strain sensors have attracted tremendous interest due to their potential application as intelligent wearable sensing devices. Among them, crack-based flexible strain sensors have been studied extensively owing to their ultrahigh sensitivity. Nevertheless, the detection range of a crack-based sensor is quite narrow, limiting its application. In this work, a stretchable strain sensor based on a designed crack structure was fabricated by spray-coating carbon nanotube (CNT) ink onto an electrospun thermoplastic polyurethane (TPU) fibrous mat and prestretching treatment to overcome the trade-off relationship. Our sensor exhibited combined features of high sensitivity in a greatly widened workable sensing range [a gauge factor of 428.5 within 100% strain, 9268.8 for a strain of 100-220%, and larger than 83982.8 for a strain of 220-300%], a fast response time (about 70 ms), superior durability (>10 000 stretching-releasing cycles), and excellent response toward bending. The microstructural evolution of CNT branches extending from two edges of the cracks and the excellent…

Conductive inks for the future printed electronics should have the following merits: high conductivity, flexibility, low cost, and compatibility with wide range of substrates. However, the state-of-the-art conductive inks based on metal nanoparticles are high in cost and poor in flexibility. Herein, we reported a highly conductive, low cost, and super flexible ink based on graphene nanoplatelets. The graphene ink has been screen-printed on plastic and paper substrates. Combined with postprinting treatments including thermal annealing and compression rolling, the printed graphene pattern shows a high conductivity of 8.81 × 10 4 S m –1 and good flexibility without significant conductivity loss after 1000 bending cycles. We further demonstrate that the printed highly conductive graphene patterns can act as current collectors for supercapacitors. The supercapacitor with the printed graphene pattern as the current collector and printed activated carbon as the active material shows a good rate capability of up to 200 mV s –1 . This work potentially provides a promising route toward the…

As a promising functional material, hydrogels have attracted extensive attention, especially in flexible wearable sensor fields, but it remains a great challenge to facilely integrate excellent mechanical properties, self-adhesion, and strain sensitivity into a single hydrogel. In this work, we present high in strength, stretchable, conformable, and self-adhesive chitosan/poly(acrylic acid) double-network nanocomposite hydrogels for application in epidermal strain sensor via in situ polymerization of acrylic acid in chitosan acid aqueous solution with tannic acid-coated cellulose nanocrystal (TA@CNC) acting as nanofillers to reinforce tensile properties, followed by a soaking process in a saturated NaCl solution to cross-link chitosan chains. With addition of a small amount of TA@CNC, the double-network nanocomposite hydrogels became highly adhesive and mechanically compliant, which were critical factors for the development of conformable and resilient wearable epidermal sensors. The salt-soaking process was applied to cross-link chitosan chains by shielded electrostatic repulsions…

Polyimide (PI) aerogels have attracted great attention owing to their low density and excellent thermal stability. However, hydrophobic surface modification is required for PI aerogels to improve their ability in oil/water separation due to their amphiphilic characteristic. Two-dimensional MXenes (transition metal carbides/nitrides) can be utilized as nanofillers to enhance the properties of polymers because of their unique layered structure and versatile interface chemistry. Herein, the robust, lightweight, and hydrophobic PI/MXene three-dimensional architectures were fabricated via freeze-drying of polyamide acid/MXene suspensions and thermal imidization. Polyamide acid was synthesized using N - N -dimethylacetamide and 4,4′-oxydianiline. MXene (Ti 3 C 2 T x ) dispersion was obtained via the etching of Ti 3 AlC 2 and ultrasonic exfoliation. Taking advantage of the strong interaction between PI chains and MXene nanosheets, the interconnected, highly porous, and hydrophobic PI/MXene aerogels with low density were fabricated, resulting in the improved compressive performance,…

Herein, we demonstrate a ternary ionic hydrogel sensor consisting of tannic acid, sodium alginate, and covalent cross-linked polyacrylamide as skin-mountable and wearable sensors. Based on the multiple weak H-bonds and synergistic effects between the three components, the as-prepared hybrid hydrogel exhibits ultrastretchability with high elasticity, good self-healing, excellent conformability, and high self-adhesiveness to diverse substrates both in air and underwater. More importantly, the ternary hydrogel exhibits high strain sensitivity especially under subtle strains with a gauge factor of 2.0, which is close to the theoretical value of the ionic hydrogel sensors; an extremely large workable range of strain (0.05-2100%); and a low operating voltage 0.07 V. Consequently, the sensor demonstrates superior sensing performance for real-time monitoring of the large and subtle human motions, including limb motions, swallowing, smiling, and wrist pulse. Therefore, it is believed that the STP hydrogel has great potential applications in health monitoring, smart wearable devices, and soft…

Ionic hydrogels, a class of intrinsically stretchable and conductive materials, are widely used in soft electronics. However, the easy freezing and drying of water-based hydrogels significantly limit their long-term stability. Here, a facile solvent-replacement strategy is developed to fabricate ethylene glycol (Eg)/glycerol (Gl)-water binary antifreezing and antidrying organohydrogels for ultrastretchable and sensitive strain sensing within a wide temperature range. Because of the ready formation of strong hydrogen bonds between Eg/Gl and water molecules, the organohydrogels gain exceptional freezing and drying tolerance with retained deformability, conductivity, and self-healing ability even stay at extreme temperature for a long time. Thus, the fabricated strain sensor displays a gauge factor of 6, which is much higher than previously reported values for hydrogel-based strain sensors. Furthermore, the strain sensor exhibits a relatively wide strain range (0.5-950%) even at -18 °C. Various human motions with different strain levels are monitored by the strain sensor with good…

Barium titanate-based energy-storage dielectric ceramics have attracted great attention due to their environmental friendliness and outstanding ferroelectric properties. Here, we demonstrate that a recoverable energy density of 2.51 J cm –3 and a giant energy efficiency of 86.89% can be simultaneously achieved in 0.92BaTiO 3 -0.08K 0.73 Bi 0.09 NbO 3 ceramics. In addition, excellent thermal stability (25–100 °C) and superior frequency stability (1–100 Hz) have been obtained under 180 kV cm –1 . The first-order reversal curve method and transmission electron microscopy measurement show that the introduction of K 0.73 Bi 0.09 NbO 3 makes ferroelectric domains to transform into highly dynamic polar nanoregions (PNRs), leading to the concurrently enhanced energy-storage properties by the transition from ferroelectric to relaxor ferroelectric (RFE). Furthermore, it is confirmed by piezoresponse force microscopy that the appearance of PNRs breaks the long-range order to some extent and reduces the stability of the microstructure, which explains the excellent energy-storage performance of…

Graphene presents an extremely ultra-high thermal conductivity, well above other known thermally conductive fillers. However, graphene tends to aggregate easily due to its strong intermolecular π–π interaction, resulting in poor dispersion in the polymer matrix. In this study, silver nanoparticles anchored reduced graphene oxide (Ag/rGO) were first prepared using one-pot synchronous reduction of Ag + and GO solution via glucose. The thermally conductive (Ag/rGO)/polyimide ((Ag/rGO)/PI) nanocomposites were then obtained via electrospinning the in situ polymerized (Ag/rGO)/polyamide electrospun suspension followed by a hot-press technique. The thermal conductivity (λ), glass transition temperature ( T g ), and heat resistance index ( T HRI ) of the (Ag/rGO)/PI nanocomposites all increased with increasing the loading of Ag/rGO fillers. When the mass fraction of Ag/rGO (the weight ratio of rGO to Ag was 4:1) fillers was 15%, the corresponding (Ag/rGO)/PI nanocomposites showed a maximum λ of 2.12 W/(m K). The corresponding T g and T HRI values were also enhanced to 216.1 and 298.6 °C,…

Amorphous InGaZnO x (a-IGZO) thin-film transistors (TFTs) are currently used in flat-panel displays due to their beneficial properties. However, the mobility of ∼10 cm 2 /(V s) for the a-IGZO TFTs used in commercial organic light-emitting diode TVs is not satisfactory for high-resolution display applications such as virtual and augmented reality applications. In general, the electrical properties of amorphous oxide semiconductors are strongly dependent on their chemical composition; the indium (In)-rich IGZO achieves a high mobility of 50 cm 2 /(V s). However, the In-rich IGZO TFTs possess another issue of negative threshold voltage owing to intrinsically high carrier density. Therefore, the development of an effective way of carrier density suppression in In-rich IGZO will be a key strategy to the realization of practical high-mobility a-IGZO TFTs. In this study, we report that In-rich IGZO TFTs with vertically stacked InO x, ZnO x, and GaO x atomic layers exhibit excellent performances such as saturation mobilities of ∼74 cm 2 /(V s), threshold voltage of −1.3 V, on/off ratio of…

Silicon has been developed as the exceptionally desirable anode candidate for lithium-ion batteries (LIBs), attributing to its highest theoretical capacity, low working potential, and abundant resource. However, large volume expansion and poor conductivity hinder its practical application. Herein, we fabricate flexible, freestanding, and binder-free silicon/MXene composite papers directly as anodes for LIBs. The Silicon/MXene composite papers are synthesized via covalently anchoring silicon nanospheres on the highly conductive networks based on MXene sheets by vacuum filtration. This unique architecture can accommodate large volume expansion, enhance conductivity of composites, prevent restacking of MXene sheets, offer additional active sites, and facilitate efficient ion transport, which exhibits superior electrochemical performance with a high capacity of 2118 mAh·g –1 at 200 mA·g –1 current density after 100 cycles, a steady cycling ability of 1672 mAh·g –1 at 1000 mA·g –1 after 200 cycles, and a rate performance of 890 mAh·g –1 at 5000 mA·g –1 . This work may shed lights on the…

Methotrexate (MTX) is one of the first-line treatments for moderate to severe psoriasis, while the side effects caused by injection and oral administration of MTX greatly restrict its clinical application. Transdermal drug delivery offers a desirable alternative to the conventional approaches, but the performances of the currently available skin penetration enhancement techniques are not so satisfactory. To address these limitations, we developed a dissolving microneedle (MN) patch made of hyaluronic acid (HA) with excellent water solubility, biocompatibility, biodegradability, and mechanical properties. The amount of MTX encapsulated in the needles of the patch could be controlled during the fabrication process for precise dosage. Interestingly, the MTX-loaded MNs successfully penetrated imiquimod (IMQ)-induced thickened epidermis in mice and delivered the drug intralesionally. Meanwhile, fast dissolution of HA endowed the MNs with operability for patients. We found that the MTX-loaded MNs not only showed well-maintained inhibitory effect in vitro but also alleviated the…

The formation of dendrites on a zinc (Zn) metal anode has limited its practical applications on aqueous batteries. Herein, an artificial composite protective layer consisting of nanosized metal–organic frameworks (MOFs) to improve the poor wetting effect of aqueous electrolytes on the Zn anode is proposed to reconstruct the Zn/electrolyte interface. In this layer, hydrophilic MOF nanoparticles serve as interconnecting electrolyte reservoirs enabling nanolevel wetting effect as well as regulating an electrolyte flux on Zn anode. This zincophilic interface exhibits significantly reduced charge-transfer resistance. As a result, stable and dendrite-free Zn plating/stripping cycling performance is achieved for over 500 cycles. In addition, especially at higher C-rates, the coating layer significantly reduces the overpotentials in a Zn/MnO 2 aqueous battery during cycling. The proposed principle and method in this work demonstrate an effective way to reconstruct a stable interface on metal anodes (e.g., Zn) where a conventional solid-electrolyte interface (SEI) cannot be formed.

The latest generation flexible devices feature materials that are conductive, highly stretchable, and transparent to meet the requirements of a reliable performance. However, the existing conductors are mostly electronic conductors, which cannot satisfy these high-performance challenges. A robust hydrogel ionic conductor was rapidly fabricated with a facile one-pot approach by employing bioinspired agar with a physically cross-linked network, polyacrylamide (PAM) with a photoinitiated cross-linked network under appropriate UV intensity, and Li + as conductive ions. The resulting Li + /agar/PAM ionic double-network hydrogels could be fabricated into various shapes through injection. The unique ionic hydrogel showed a remarkable stretchability with over 1600% extension, high tension/compression strength (0.22 MPa/3.5 MPa), and toughness (2.2 MJ/m 3 ). Furthermore, it was demonstrated to possess dual sensory capabilities through the combination of both temperature and mechanical deformation. This hydrogel ionic conductor exhibited high stretching sensitivity with a gauge factor of 1.8…

A method for fabricating long, soft, and reversibly actuatable liquid crystal elastomer (LCE) fibers by using direct ink write (DIW) printing was developed. Here, the LCE was produced based on a two-stage thermal-photo curing reaction between a difunctional acrylate monomer and thiol. The LCE ink, mixed with nanoclay to increase the viscosity, was extruded through a nozzle onto a rotating mandrel to obtain a long fiber. After printing, the fiber was first thermally cured on the mandrel, then mechanically stretched, and photocured to achieve liquid crystal chain alignment for stress-free reversible activation. Upon optimizing the ink viscosity and DIW printing parameters, long fibers (up to 1.5 m long from the laboratory) were obtained. The resulting fiber had a modulus of 2 MPa, 51% actuation strain, and a failure strain of well over 100%. The potential of these fibers for applications was demonstrated. The LCE fibers were knit, sewn, and woven to form a variety of smart textiles. The fiber was also used to mimic bicep muscles with both large activation force and activation strain.…

Surface contamination by microbes leads to several detrimental consequences like hospital- and device-associated infections. One measure to inhibit surface contamination is to confer the surfaces with antimicrobial properties. Copper's antimicrobial properties have been known since ancient times, and the recent resurgence in exploiting copper for application as antimicrobial materials or coatings is motivated by the growing concern about antibiotic resistance and the pressure to reduce antibiotic use. Copper, unlike silver, demonstrates rapid and high microbicidal efficacy against pathogens that are in close contact under ambient indoor conditions, which enhances its range of applicability. This review highlights the mechanisms behind copper's potent antimicrobial property, the design and fabrication of different copper-based antimicrobial materials and coatings comprising metallic copper/copper alloys, copper nanoparticles or ions, and their potential for practical applications. Finally, as the antimicrobial coatings market is expected to grow, we offer our perspectives on the…

Cathode electrolyte interphase (CEI) layer plays an essential role in determining the electrochemical performance of Li-ion batteries (LIBs), but the detailed mechanisms of CEI formation and evolution are not yet fully understood. With the pursuit of LIBs possessing a high energy density, fundamental investigations on the CEI have become increasingly important. Herein, X-ray photoelectron spectroscopy (XPS) is employed to fingerprint CEI formation and evolution on three of the most prevailing high-voltage cathodes including layered Li 1.144 Ni 0.136 Co 0.136 Mn 0.544 O 2 (LR-NCM), Li 2 Ru 0.5 Mn 0.5 O 3 (LRMO), and spinel LiNi 0.5 Mn 1.5 O 4 (LNMO). The influences of crystal structure, chemical constitution and cut-off voltage on CEI composition are clarified. Among these cathodes, the spinel cathode exhibits the most stable CEI layer throughout the battery cycle. While the layered cathodes based on the 4d transition metal Ru favor CEI formation upon contacting the electrolyte. Most importantly, anionic redox reaction (ARR) activation at high voltages is verified to dominate CEI…

High Resolution Image Download MS PowerPoint Slide Therapeutic options for the highly pathogenic human coronavirus (HCoV) infections are urgently needed. Anticoronavirus therapy is however challenging, as coronaviruses are biologically diverse and rapidly mutating. In this work, the antiviral activity of seven different carbon quantum dots (CQDs) for the treatment of human coronavirus HCoV-229E infections was investigated. The first generation of antiviral CQDs was derived from hydrothermal carbonization of ethylenediamine/citric acid as carbon precursors and postmodified with boronic acid ligands. These nanostructures showed a concentration-dependent virus inactivation with an estimated EC 50 of 52 ± 8 μg mL –1 . CQDs derived from 4-aminophenylboronic acid without any further modification resulted in the second-generation of anti-HCoV nanomaterials with an EC 50 lowered to 5.2 ± 0.7 μg mL –1 . The underlying mechanism of action of these CQDs was revealed to be inhibition of HCoV-229E entry that could be due to interaction of the functional groups of the CQDs with HCoV-229E entry…

A triple-layered TFC nanofiltration (NF) membrane consisting of a polyamide (PA) top layer covered on a poly(ether sulfone) microfiltration membrane with a carbon nanotube (CNT) interlayer was fabricated via interfacial polymerization. The structure and properties of the PA active layer could be finely tailored by tuning the interfacial properties and pore structure of the CNT interlayer, including its surface pore size and thickness, thus improving its NF performance. This TFC NF membrane exhibited a high divalent salt rejection (the rejection of Na 2 SO 4 and MgSO 4 solution >98.3%) and dye rejection (the rejection of methyl violet (MV) >99.5%) with a high pure water flux of around 21 L m –2 h –1 bar –1 . Excitingly, this membrane also showed excellent selectivity to both mono/divalent salt ion (the selectivity of Cl – /SO 4 2– is as high as 85.5) and NaCl/dye solution (the selectivity of NaCl/MV is more than 123.5), which are much higher than most of other commercial and reported NF membranes. Moreover, this membrane also showed a good separation performance and long-term…

One-dimensional microstructure has been regarded as one of the most desirable configurations for magnetic carbon-based microwave absorbing materials (MAMs). Herein, pea-like Fe/Fe 3 C nanoparticles embedded in nitrogen-doped carbon nanotubes (Fe/Fe 3 C@NCNTs) are successfully prepared through a direct pyrolysis of the mixture of FeCl 3 ·6H 2 O and melamine under inert atmosphere. The chemical composition and microstructural feature of these Fe/Fe 3 C@NCNTs composites are highly dependent on the pyrolysis temperature. As a result, their electromagnetic properties can be also manipulated, where dielectric loss gradually decreases with the increasing pyrolysis temperature and magnetic loss presents a reverse variation trend. When the pyrolysis temperature reaches 600 °C, the as-obtained composite, Fe/Fe 3 C@NCNTs-600 can perform a maximum reflection loss of −46.0 dB at 3.6 GHz with a thickness of 4.97 mm and a qualified bandwidth of 14.8 GHz with the integrated thickness from 1.00 to 5.00 mm. It is very interesting that the microwave absorption performance of this new kind of…

Cell designs that integrate membrane-electrode assemblies (MEAs) with highly selective catalysts are a promising route to reduce ohmic losses and achieve high energy efficiency in CO 2 reduction at industrially relevant current densities. In this work, porous silver filtration membranes are demonstrated as simple and efficient gas-diffusion electrodes for CO 2 reduction to CO at high current densities in an MEA-type device. A partial current density for CO of up to ca. 200 mA cm –2 was achieved at a cell voltage of ca. 3.3 V, in tandem with minimal H 2 production. However, the analysis of cathodic and anodic outlet streams revealed that CO 2 cross-over across the anion-exchange membranes, mostly in the form of CO 3 2– but partially as HCOO – generated over the cathode, actually exceeds the amount of CO 2 converted to the target product, resulting in a poor utilization of the reactant and in the early onset of mass transfer limitations. In addition, CO 2 cross-over leads to a nonstoichiometric decrease of the outlet flow rate from the cathodic compartment. This effect can lead to a…

Carbon dots (CDs) with low biotoxicity, high photostability, and well-controlled size are highly desirable imaging agents for optical bioimaging. However, most of the CDs triggered by ultraviolet/blue light present visible/first near-infrared emissions shorter than 820 nm, impairing their imaging applications in vivo by low penetration depth. Hence, developing novel CD-based materials with second near-infrared (NIR-II) emission located in 1000-1700 nm region is an urgent task. Here, a novel NIR-II-emitting CD-based nanoprobe triggered by 808 nm laser is developed. The designed CDs with 900-1200 nm luminescence possess high quantum yield (QY-0.4%) and high biocompatibility, which have proven to be effective probes for in vivo NIR-II bioimaging. Notably, nearly 65% CDs are excreted from mouse urine within 6 h, demonstrating the rapid renal clearance of CDs. Furthermore, the designed CDs also exhibit high photothermal efficiency (30.6%), making them ideal materials for thermal ablation of cancer. Our findings pave the way of designing a multifunctional CD-based theranostic platform for…

Solar-driven interfacial water evaporation is regarded as an effective, renewable, and environment-friendly technology for clean water production. However, biofouling caused by the nonspecific interaction between the steam generator and biofoulants generally hinders the efficient application of wastewater treatment. Herein, this work reports a facile strategy to fabricate flexible anti-biofouling fibrous photothermal membrane consisting of a MXene-coated cellulose membrane for highly efficient solar-driven water steam evaporation toward water purification applications. The as-prepared MXene/cellulose photothermal membrane exhibits light absorption efficiency as high as ∼94% in a wide solar spectrum range and a water evaporation rate up to 1.44 kg m –2 h –1 under one solar illumination. Also, the MXene/cellulose membrane shows very high antibacterial efficiency (above 99.9%) owing to the MXene coating as a highly effective bacteriostatic agent. Such a flexible, anti-biofouling, and high-efficiency photothermal membrane sheds light on practical applications in long-term wastewater…

Two-dimensional Ti 3 C 2 T x MXene-based hybrids-anchored magnetic metal nanoparticles show a huge potential application as effective wave absorbers due to the synergistic electromagnetic (EM) loss effect. In this work, uniform and size-controllable nickel, cobalt, or nickel–cobalt alloy nanoparticles were in situ grown on the surface of MXene via a facile and moderate co-solvothermal method for the first time. As an example, a nickel nanoparticles-anchored MXene (Ni@MXene) hybrid was homodispersed into dielectric polyvinylidene fluoride to develop its EM wave-absorbing capacity to a great extent. As expected, the results showed strong reflection loss (RL min = −52.6 dB at 8.4 GHz), broad effective absorption bandwidth (EAB = 3.7 GHz including 71% of X-band), low loading (10 wt % Ni@MXene), and thin thickness (3.0 mm). By adjusting the sample thickness, EAB can cover completely the whole X-band with a maximum of 6.1 GHz, showing a huge potential of Ni@MXene hybrid applying as aircraft stealth coating. The mechanism analyses revealed that the excellent impedance matching,…

The development of biodegradable and antibacterial hemostatic materials with high blood absorption to halt the internal hemorrhage of deep noncompressible wounds remains a challenge. In this study, a novel hemostatic nanocomposite (OBC/COL/CS) was fabricated by coupling oxidized bacterial cellulose (OBC) and chitosan (CS) with collagen (COL), that is, during the electrostatic self-assembly of OBC with CS (OBC/CS), COL was ingeniously attached as a functional component by the electrostatic attraction of cationic CS and anionic OBC. The introduction of collagen was anticipated to provide functional properties such as enhanced hemostasis and promotion of wound healing so as to achieve a new functional composite. This study is the first to evaluate the performance of OBC, OBC/CS, and the OBC/COL/CS composite for rapid internal hemostasis using a rat liver injury model. To our knowledge, this is also the first study to report that OBC has a faster biodegradability in vivo than commercial hemostatic oxidized regenerated plant cellulose (ORC). The OBC/COL/CS nanocomposite exhibited…

Rapid and early diagnosis of respiratory viruses is key to preventing infections from spreading and guiding treatments. Here, we developed a sensitive and quantitative surface-enhanced Raman scattering-based lateral flow immunoassay (SERS-based LFIA) strip for simultaneous detection of influenza A H1N1 virus and human adenovirus (HAdV) by using Fe 3 O 4 @Ag nanoparticles as magnetic SERS nanotags. The new type of Fe 3 O 4 @Ag magnetic tags, which were conjugated with dual-layer Raman dye molecules and target virus-capture antibodies, performs the following functions: specific recognition and magnetic enrichment of target viruses in the solution and SERS detection of the viruses on the strip. Based on this strategy, the magnetic SERS strip can directly be used for real biological samples without any sample pretreatment steps. The limits of detection for H1N1 and HAdV were 50 and 10 pfu/mL, respectively, which were 2000 times more sensitive than those from the standard colloidal gold strip method. Moreover, the proposed strip is easy to operate, rapid, stable, and can achieve high…

Ti 3 C 2 T x (MXene) exhibits attractive properties in different applications. However, traditional synthesis leads to unsatisfactory yield of two-dimensional (2D) Ti 3 C 2 T x, e.g., lower than 20%, which stems from the strong interactions of potential Ti–Ti bonds and residual Ti–Al bonds between the adjacent Ti 3 C 2 layers, hindering the effective intercalation and delamination. Herein, we propose a facile hydrothermal-assisted intercalation (HAI) strategy to boost the yield of 2D sheets, achieving a record high value of 74%. This HAI assists the diffusion and intercalation of reagent effectively, promoting the subsequent delamination; meanwhile, an antioxidant is applied to protect these Ti 3 C 2 T x from oxidation during the HAI process. Therefore, massive Ti 3 C 2 T x 2D sheets can be easily synthesized. Thanks to the synergistic effect of high conductivity and substantial terminated functionalities, these Ti 3 C 2 T x 2D sheets show promising application in supercapacitor, providing a high capacitance of 482 F g –1 . Besides, the ultrafast carrier dynamics results of Ti 3 C 2…

All-solid-state batteries (ASSBs) based on inorganic solid electrolytes promise improved safety, higher energy density, longer cycle life, and lower cost than conventional Li-ion batteries. However, their practical application is hampered by the high resistance arising at the solid-solid electrode-electrolyte interface. Although the exact mechanism of this interface resistance has not been fully understood, various chemical, electrochemical, and chemo-mechanical processes govern the charge transfer phenomenon at the interface. This paper reports the interfacial behavior of the lithium and the cathode in oxide and sulfide inorganic solid-electrolytes and how that affects the overall battery performance. An overview of the recent reports dealing with high resistance at the anodic and cathodic interfaces is presented and the scientific and engineering aspects of the approaches adopted to solve the issue are summarized.

The development of catalysts that effectively activate target pollutants and promote their complete conversion is an admirable objective in the environmental photocatalysis field. In this work, graphitic carbon nitride (g-C 3 N 4 ) microtubes with tunable N-vacancy concentrations were controllably fabricated using an in situ soft-chemical method. The morphological evolution of g-C 3 N 4, from the bulk to the porous tubular architecture, is discussed in detail with the aid of time-resolved hydrothermal experiments. We found that the NO removal ratio and apparent reaction rate constant of the g-C 3 N 4 microtubes were 1.8 and 2.6 times higher than those of pristine g-C 3 N 4, respectively. By combining detailed experimental characterization and density functional theory calculations, the effects of N-vacancies in the g-C 3 N 4 microtubes on O 2 and NO adsorption activation, electron capture, and electronic structure were systematically investigated. These results demonstrate that surface N-vacancies act as specific sites for the adsorption activation of reactants and photoinduced…

Thermal-stable dielectric capacitors with high energy density and power density have attracted increasing attention in recent years. In this work, (1 – x )Bi 0.5 Na 0.5 TiO 3 – x NaTaO 3 [(1 – x )BNT– x NT, x = 0–0.30] lead-free relaxor ferroelectric ceramics are developed for capacitor applications. The x = 0.20 ceramic exhibits superior thermal stability of discharged energy density ( W D ) with a variation of less than 10% in an ultrawide temperature range of −50 to 300 °C, showing a significant advantage compared with the previously reported ceramic systems. The W D reaches 4.21 J/cm 3 under 38 kV/mm at room temperature. Besides, a record high of power density ( P D ≈ 89.5 MW/cm 3 ) in BNT-based ceramics is also achieved in x = 0.20 ceramic with an excellent temperature insensitivity within 25–160 °C. The x = 0.20 ceramic is indicated to be an ergodic relaxor ferroelectric with coexisted R 3 c nanodomains and P 4 bm polar nanoregions at room temperature, greatly inducing large maximum polarization, maintaining low remnant polarization, and thus achieving high W D and P D .…

Battery safety, at the foundation of fast charging, is critical to the application of lithium-ion batteries, especially for high energy density cells applied in electric vehicles. In this paper, an earlier thermal runaway of cells after fast charging application is illustrated. Under this condition, the reaction between the plated lithium and electrolyte is revealed to be the mechanism of thermal runaway triggering. The mechanism is proved by the accelerated rate calorimetry tests for partial cells, which determine the triggering reactions of thermal runaway in the anode-electrolyte thermodynamic system. The reactants in this system are analyzed by nuclear magnetic resonance and differential scanning calorimetry, proving that the vigorous exothermic reaction is induced by the interaction between the plated lithium and electrolyte. As a result, the finding of thermal runaway triggered by the plated lithium on anode surface of cells after fast charging promotes the understanding of thermal runaway mechanisms, which warns of the danger of plated lithium in the utilization of…

Recently, a paper-based (PB) strain sensor has turned out to be an ideal substitute for the polymer-based one because of the merits of renewability, biodegradability, and low cost. However, the hygroexpansion and degradation of the paper after absorbing water are the great challenges for the practical applications of the PB strain sensor. Herein, the superhydrophobic electrically conductive paper was fabricated by simply dip-coating the printing paper into the carbon black (CB)/carbon nanotube (CNT)/methyl cellulose suspension and hydrophobic fumed silica (Hf-SiO 2 ) suspension successively to settle the problem. Because of the existence of ultrasensitive microcrack structures in the electrically conductive CB/CNT layer, the sensor was capable of detecting an ultralow strain as low as 0.1%. During the tension strain range of 0–0.7%, the sensor exhibited a gauge factor of 7.5, almost 3 times higher than that of the conventional metallic-based sensors. In addition, the sensor displayed frequency-independent and excellent durability and reproductivity over 1000 tension cycles.…

Recent introduction of data-driven approaches based on deep-learning technology has revolutionized the field of nanophotonics by allowing efficient inverse design methods. In this paper, a simultaneous inverse design of materials and structure parameters of core-shell nanoparticles is achieved for the first time using deep learning of a neural network. A neural network to learn the correlation between the extinction spectra of electric and magnetic dipoles and core-shell nanoparticle designs, which include material information and shell thicknesses, is developed and trained. We demonstrate deep-learning-assisted inverse design of core-shell nanoparticles for (1) spectral tuning electric dipole resonances, (2) finding spectrally isolated pure magnetic dipole resonances, and (3) finding spectrally overlapped electric dipole and magnetic dipole resonances. Our finding paves the way for the rapid development of nanophotonics by allowing a practical utilization of deep-learning technology for nanophotonic inverse design.

Graphene foams with three-dimensional (3D) network structure, high porosity, and ultralow density have been regarded as lightweight microwave absorption materials. Herein, nitrogen-doped reduced graphene oxide/multi-walled carbon nanotube composite foams were prepared through a two-step strategy of hydrothermal self-assembly and subsequent high-temperature calcination. Morphology analysis indicated that the 3D networks were composed of overlapped flaky reduced graphene oxide. In addition, the influences of nitrogen doping, calcination temperature, and filler ratios on microwave absorption of composite foams were explored. Results manifested that the microwave absorption of composite foams was remarkably improved with the calcination temperature increased. Dramatically, it was noteworthy that the composite foam obtained under 600 °C calcination (bulk density of ∼10.8 mg/cm 3 ) with an 8 wt % mass filler ratio presented the strongest microwave absorption of −69.6 dB at 12.5 GHz and broadest absorption bandwidth achieved 4.3 GHz (13.2–17.5 GHz) at an extremely low matching thickness…

Solar steam generation is regarded as a perspective technology, due to its potentials in solar light absorption and photothermal conversion for seawater desalination and water purification. Although lots of steam generation systems have been reported to possess high conversion efficiencies recently, researches of simple, cost-effective, and sustainable materials still need to be done. Here, inspired by natural young sunflower heads’ property increasing the temperature of dish-shaped flowers by tracking the sun, we used 3D-structured carbonized sunflower heads as an effective solar steam generator. The evaporation rate and efficiency of these materials under 1 sun (1 kW m –2 ) are 1.51 kg m –2 h –1 and 100.4%, respectively, beyond the theoretical limit of 2D materials. This high solar efficiency surpasses all other biomass-based materials ever reported. It is demonstrated that such a high capability is mainly attributed to the 3D-structured top surface, which could reabsorb the lost energy of diffuse reflection and thermal radiation, as well as provide enlarged water/air interface…

High-efficient electrocatalysts are crucial for fuel cell applications; however, the whole cell performance is generally restricted by the anodic part because of the sluggish kinetics involved in the oxygen evolution reaction (OER) process. Herein, a hierarchical hollow (Co,Ni)Se 2 @NiFe layered double hydroxide (LDH) nanocage was synthesized by deriving from the metal–organic framework (MOF) of ZIF-67. Concretely, it involves first fabrication of hollow rhombic (Co,Ni)Se 2 nanocages and then deposition of NiFe LDH nanosheets on the surface of nanocages. Notably, the incorporation of Ni into Co-based ZIF-67 (via ion-exchange) could tail the atomic arrangement of the MOF, exposing more additional active sites in the following selenization treatment. The as-synthesized (Co,Ni)Se 2 @NiFe LDH demonstrates splendid OER performance with a small overpotential of 277 mV (to launch a current density of 10 mA cm –2 ), a small Tafel slope of 75 mV dec –1, and robust durability (a slight stability decay of 5.1% after 17 h of continuous test), not only surpassing the commercial RuO 2 but also…

Lead-free double perovskite nanocrystals (NCs) have emerged as a new category of materials that hold the potential for overcoming the instability and toxicity issues of lead-based counterparts. Doping chemistry represents a unique avenue toward tuning and optimizing the intrinsic optical and electronic properties of semiconductor materials. In this study, we report the first example of doping Yb 3+ ions into lead-free double perovskite Cs 2 AgBiX 6 (X = Cl –, Br – ) NCs via a hot injection method. The doping of Yb 3+ endows the double perovskite NCs with a newly emerged near-infrared emission band (sensitized from the NC hosts) in addition to their intrinsic trap-related visible photoluminescence. By controlling the Yb-doping concentration, the dual emission profiles and photon relaxation dynamics of the double perovskite NCs can be systematically tuned. Furthermore, we have successfully inserted divalent Mn 2+ ions in Cs 2 AgBiCl 6 NCs and observed emergence of dopant emission. Our work illustrates an effective and facile route toward modifying and optimizing optical properties of…

Respiration monitoring is important for evaluating human health. Humidity sensing is a promising way to establish a relationship between human respiration and electrical signal. This work describes polymer humidity sensors with ultrafast response for respiration monitoring. The humidity-sensitive polyelectrolyte is in situ cross-linked on the substrate printed with interdigitated electrodes by a thiol-ene click reaction. The polyelectrolyte humidity sensor shows rapid water adsorption/desorption ability, excellent stability, and repeatability. The sensor with ultrafast response and recovery (0.29/0.47 s) when changing humidity between 33 and 95% shows good application prospects in breath monitoring and touchless sensing. Different respiration patterns can be distinguished, and the breath rate/depth of detection subjects can also be determined by the sensor. In addition, the obtained sensor can sense the skin evaporation in a noncontact way.

Co nanoparticles embedded in nitrogen-doped carbon nanocubes (Co/NCs) for applications as anode materials in rechargeable lithium-ion batteries were synthesized by calcining Co-based metal-organic framework. Sizes of Co nanoparticles were ∼15 nm according to X-ray diffraction (XRD) and transmission electron microscopy. Electrochemical performances of the as-prepared anode nanocube composite at 700 °C showed a high initial capacity of 1375.1 mAh g –1 in the voltage range of 0.01–3.0 V at the current rate of 0.1 A g –1 . After 100 cycles, capacity remained at 688.6 mAh g –1 . Thereinto, the role of Co nanoparticles in electrochemical reaction was also elucidated by in situ XRD experiment. Capacity increase of Co/NCs at the high currents was observed, which are potentially caused by the activation of electrode and pseudocapacitance during cycling. High surface area and abundant mesopores contributed to the improved electrochemical performances of the anode, providing numerous pathways and sites for Li + transfer and storage and accordingly contributing to pseudocapacitance capacity.

Carbon nanocoils (CNCs) are employed to fabricate fast, high-resolution, and reversible humidity sensor based on a flexible liquid crystal polymer (LCP) substrate. The humidity sensor displays fast-response (1.9 s) and recovery time (1.5 s), a broad relative humidity (RH) detection range (4-95%), linearity, repeatability, and stability. The rapid response and recovery are considered to benefit from the hydrophobic effect of the LCP substrate and high purity of the CNCs, which give rise to weak physical adsorption. Meanwhile, the high sensitivity results from both the unique helical structure of CNCs and the microporous structure of the LCP substrate. The distinctive structure-related properties enable the sensor to reliably perceive an extremely small RH variation of 0.8%, which is too small to be detected by most humidity sensors reported previously. These features allow the sensor to monitor a variety of important human activities, such as respiration, speaking, blowing, and noncontact fingertip sensation, accurately. Furthermore, different human physical conditions can be…

Abstract Cellulose nanofibrils (CNFs) in the form of hydrogels stand out as a platform biomaterial in bioink formulation for 3D printing because of their low cytotoxicity and structural similarity to extracellular matrices. In the present study, 3D scaffolds were successfully printed with low-concentration inks formulated by 1 w/v % 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized CNF with less than 1 w/v % gelatin methacrylate (GelMA). Quartz crystal microbalance with dissipation monitoring (QCM-D) measurements showed strong interaction between the two biopolymers. The UV cross-linking ability of GelMA (≤1 w/v %) was enhanced in the presence of TEMPO-oxidized CNFs. Multiple factors including strong physical interaction between CNF and GelMA, in situ cross-linking of CNF by Ca2+, and UV cross-linking of GelMA enabled successful 3D printing of low-concentration inks of CNF/GelMA into scaffolds possessing good structural stability. The mechanical strength of the scaffolds was tuned in the range of 2.5 to 5 kPa. The cell culture with 3T3 fibroblasts revealed noncytotoxic…

Bacterial infection is still a ticklish clinical challenge even though some advanced antibacterial materials and techniques have been put forward. This work reports that rapid and effective antibacterial performance is achieved by the synergistic local photothermal and photodynamic therapy (PTDT). Within 10 min of light irradiation, both Escherichia coli and Staphylococcus aureus are almost completely eliminated by the action of photothermy (52.1 °C) and limited reactive oxygen species (ROS), the corresponding bacterial killing efficiencies are 99.91 and 99.97%, respectively, which are far higher than single modal therapy, i.e., photothermal therapy or photodynamic therapy with antibacterial efficacy of 50 or 70%, respectively. The mechanism is that bacterial membrane permeation is increased by PTDT because photothermy shows more severe impact only on E. coli by destroying the outmost bacterial panniculus, whereas the inner panniculus of the two kinds of bacteria is more sensitive to ROS. Hence, ROS penetrates the bacterial membrane more easily, and meanwhile, the proteins in the…

Three-dimensional (3D) porous conductive composites explored in highly sensitive tactile sensors have attracted extensive close attention in recent years owing to their peculiar porous structure and unique physical properties in terms of excellent mechanical flexibility, high relative dielectric permittivity, and good elastic property. Herein, we report an practical, efficient, and macroscopic dip-coating process to manufacture rapid-response, low detection limit, high-sensitivity, and highly sensitive capacitive flexible tactile sensors. The fabrication process, tactile perception mechanism, and sensing performance of the developed devices are comparatively investigated. The homogeneous 3D hybrid network constructed by graphene nanoplatelets/carboxyl-functionalized multiwalled carbon nanotubes/silicone rubber composites anchored on polyurethane sponge skeletons exhibits a significantly improved dielectric property, resulting in a high-performance capacitive flexible tactile sensor with a fast response time (∼45 ms), an extremely low-pressure detection limit of ∼3 Pa, excellent…

Nanostructured photothermal membranes hold great potential for solar-driven seawater desalination; however, their pragmatic applications are often limited by substantial salt accumulation. To solve this issue, we have designed and prepared flexible and washable carbon-nanotube-embedded polyacrylonitrile nonwoven fabrics by a simple electrospinning route. The wet fabric exhibits a strong photoabsorption in a wide spectral range (350–2500 nm), and it has a photoabsorption efficiency of 90.8%. When coated onto a polystyrene foam, the fabric shows a high seawater evaporation rate of 1.44 kg m –2 h –1 under simulated sunlight irradiation (1.0 kW m –2 ). With a high concentration of simulated seawater as the model, the accumulation of solid salts can be clearly observed on the surface of the fabric, resulting in a severe decay of the evaporation rate. These salts can be effortlessly washed away from the fabric through a plain handwashing process. The washing process has a negligible influence on the morphology, photoabsorption, and evaporation performance of the fabric, demonstrating good…

Heterojunction photocatalysts have attracted widespread interest in photocatalysis because of their high-efficiency interfacial charge-transfer characteristics of nanoarchitectures. In this study, Ag-bridged 2D/2D Bi 5 FeTi 3 O 15 /ultrathin g-C 3 N 4 Z-scheme heterojunction photocatalysts with powerful interfacial charge transfer has been synthesized via a facile ultrasound method coupled with a photoreduction strategy for efficient photocatalytic degradation of antibiotics. The morphology analysis displays that the bridged Ag nanoparticles were anchored on the interface of layered Bi 5 FeTi 3 O 15 and ultrathin g-C 3 N 4 nanosheets. Owing to its unique 2D/2D ternary heterostructure, the Bi 5 FeTi 3 O 15 /2%Ag/10% ultrathin g-C 3 N 4 composite exhibited the best tetracycline degradation performance under visible-light and simulated solar irradiation. Meanwhile, the intermediates and degradation pathways were proposed by a liquid-phase mass spectrometry system. Characterizations and density functional theory studies together verify that the matched band structure of Bi 5 FeTi 3 O 15…

Piezoelectric nanomaterials have been utilized to realize effective charge separation for degrading organic pollutants in water under the action of mechanical vibrations. However, in particulate form, the nanostructured piezoelectric catalysts can flow into the aqueous pollutant and limit its recyclability and reuse. Here, we report a new method of using a barium titanate (BaTiO 3, BTO)–polydimethylsiloxane composite porous foam catalyst to address the challenge of secondary pollution and reusable limits. Piezo-catalytic dye degradation activity of the porous foam can degrade a Rhodamine B (RhB) dye solution by ∼94%, and the composite material exhibits excellent stability after repeated decomposition of 12 cycles. It is suggested that under ultrasonic vibrations, the piezoelectric BTO materials create separated electron–hole pairs that react with hydroxyl ions and oxygen molecules to generate superoxide ( • O 2 – ) and hydroxyl ( • OH) radicals for organic dye degradation. The degradation efficiency of RhB is associated with the piezoelectric constant, the specific surface area, and…

Herein, we developed a nanocomposite membrane with synergistic photodynamic therapy and photothermal therapy antibacterial effects, triggered by a single near-infrared (NIR) light illumination. First, upconversion nanoparticles (UCNPs) with a hierarchical structure (UCNPs@TiO 2 ) were synthesized, which use NaYF 4:Yb,Tm nanorods as the core and TiO 2 nanoparticles as the outer shell. Then, nanosized graphene oxide (GO), as a photothermal agent, was doped into UCNPs@TiO 2 core–shell nanoparticles to obtain UCNPs@TiO 2 @GO. Afterward, the mixture of UCNPs@TiO 2 @GO in poly(vinylidene) fluoride (PVDF) was applied for electrospinning to generate the nanocomposite membrane (UTG-PVDF). Generation of reactive oxygen species (ROS) and changes of temperature triggered by NIR action were both investigated to evaluate the photodynamic and photothermal properties. Upon a single NIR light (980 nm) irradiation for 5 min, the nanocomposite membrane could simultaneously generate ROS and moderate temperature rise, triggering synergistic antibacterial effects against both Gram-positive and -negative…

P2-type Na 2/3 Ni 1/3 Mn 2/3 O 2 is a promising cathode material for practical applications in Na-ion batteries, due to its high energy density, high volumetric capacity, excellent Na ion conductivity, ease of synthesis, and good stability in air. Yet, it is subject to structural rearrangements on charging to high voltage/low Na content and Na + /vacancy ordering transitions, which lead to poor reversibility and dramatic capacity decay upon cycling. In this Review, we present the latest advances related to Na 2/3 Ni 1/3 Mn 2/3 O 2, with a main focus on strategies to stabilize the structural framework and improve the electrochemical properties. Practical issues and challenges are also proposed on the basis of current research status and progress.

Fluorescent carbon dots (CDs) have been synthesized via the calcination method using natural gynostemma as the precursor, without any toxic ingredients or surface passivation chemicals. CDs have a narrow size distribution, and the mean particle size is about 2.5 nm. CDs exhibit good water dispersibility and can emit intense blue fluorescence under 365 nm UV light in an aqueous solution, which can be stable in different conditions. The biotoxicity of CDs on the embryonic development of zebrafish is evaluated, the hatch rate and survival rate of embryos are around 90%, and the malformation rate is less than 10%. Because of the excellent fluorescence stability and biocompatibility, CDs can be used in zebrafish for bioimaging. In addition, the antioxidative stress property of CDs is investigated both in vitro and in vivo, and the presence of CDs can promote the mRNA expression of related genes to encode more antioxidant proteins in zebrafish. Therefore, fluorescent CDs would be a potential candidate for bioimaging and treating diseases caused by excessive oxidation damage, such as…

Photocatalytic reduction of CO 2 to renewable solar fuels is considered to be a promising strategy to simultaneously solve both global warming and energy crises. However, development of a superior photocatalytic system with high product selectivity for CO 2 reduction under solar light is the prime requisite. Herein, a series of nature-inspired Z-scheme g C 3 N 4 /FeWO 4 composites are prepared for higher performance and selective CO 2 reduction to CO as solar fuel under solar light. The novel direct Z-scheme coupling of the visible light-active FeWO 4 nanoparticles with C 3 N 4 nanosheets is seen to exhibit excellent performance for CO production with a rate of 6 μmol/g/h at an ambient temperature, almost 6 times higher compared to pristine C 3 N 4 and 15 times higher than pristine FeWO 4 . More importantly, selectivity for CO is 100% over other carbon products from CO 2 reduction and more than 90% over H 2 products from water splitting. Our results clearly demonstrate that the staggered band structure between FeWO 4 and C 3 N 4 reflecting the nature-inspired Z-scheme system not…

Metal-organic framework (MOF)-derived magnetic metal/carbon nanocomposites have shown tremendous potential for lightweight electromagnetic wave (EMW) absorption. However, it is a challenge but highly significant to design and construct mixed-dimensional hierarchical architectures with synergistically integrated characteristics from individual MOFs for advancing the EMW absorption performance. Inspired by the structure of cactus, a novel hierarchical one-dimensional (1D)-two-dimensional (2D) mixed-dimensional Co/N-decorated carbon architecture comprising carbon nanotubes grafted on carbon flakes (abbreviated as CoNC/CNTs) has been fabricated by the pyrolysis of bimetallic CoZn-ZIF-L. The CoNC/CNTs integrate the advantages of 1D nanotubes for the extra polarization of EMW and 2D nanoflakes with an interconnected porous structure for multiple reflection losses of EMW and optimization of impedance matching. The resultant CoNC/CNTs demonstrate excellent EMW absorbing performance. For the optimal EMW absorbing material of CoNC/CNT-3/1, minimum reflection loss reaches -44.6 dB at 5.20 GHz…

Wearable epidermal sensors are attracting growing interests in human activity monitoring and flexible touch display, but they are still limited by the poor self-healing property and the difficult dissolvable feature. Herein, we report polyvinyl alcohol (PVA)-stabilized liquid metal particles (LMPs) (PVA-LMPs) hydrogels with excellent self-healing performance and the dissolvable feature for wearable epidermal sensors, constructed by dispersing LMPs of eutectic gallium and indium into the borate-modified PVA polymer networks. Interestingly, the PVA-LMPs hydrogels exhibited excellent electrically and mechanically self-healing ability. Moreover, the PVA-LMPs hydrogel can be fabricated as epidermal sensors, which can accurately monitor the human activities. Additionally, the epidermal sensors are dissolvable, showing an attractive feature for on demand transient electronics. It is demonstrated that the hydroxyl groups of PVA can stabilize LMPs via hydrogen-bonding interactions. Furthermore, the dynamic cross-linking bonds between hydrogels and LMPs can rupture and coalesce reversibly in…

Multilayered microwave absorbers which can provide massive interfaces are highly needed for electromagnetic-wave absorption property enhancement. Meanwhile, how to effectively avoid agglomeration and further widen the absorption band is still a challenge. Herein, accordion-like magnetized MXene/Ni composites were fabricated by the electrostatic self-assembly interaction between multilayer MXene and Ni(OH) 2 nanoplates and subsequent in situ reduction in the H 2 /Ar atmosphere. Ni nanoparticles were uniformly distributed without magnetic agglomeration between the multilayered gaps of the adjacent 2D (2 dimension) MXene (Ti 3 C 2 T x ) of MXene/Ni nanocomposites (magnetized MXene), which hold the distinct absorption performance that the reflection loss maximum measures up to −50.5 dB at 5.5 GHz. Moreover, dynamic magnetic response of the magnetized MXene absorber was first researched by the electron holography analysis. The related key mechanism includes the enhanced magnetic loss, less dual-agglomeration (multilayer MXene itself and magnetic agglomeration), and more interfaces and…

In order to improve the catalytic performance of oxygen reduction reaction (ORR), it is pivotal to increase the density and accessibility of the active sites. Herein, we have developed a template-free melamine-assisted cocalcined strategy to afford Fe-embedded and N-doped carbons (Fe–N–C) with not only high density of atomically dispersed Fe–N x active sites but also abundant three-dimensional interconnected mesopores by directly pyrolyzing Fe-ZIF-8 covered with a controllable melamine layer. It is demonstrated that the introduction of melamine in the precursor plays a key role in constructing various carbonized products with controllable morphology, porosity, and components. With an optimal mass ratio 1:1 of melamine to Fe-ZIF-8, the resultant Fe@MNC-1 exhibits excellent ORR activity and stability, which exceeds 20 wt % commercial Pt/C catalyst (with a half-wave potential of 0.88 V vs 0.85 V) in an alkaline electrolyte and is even comparable to the commercial Pt/C catalyst (with a half-wave potential of 0.78 V vs 0.80 V) in an acidic electrolyte. To the best of our knowledge,…

Hydrogels that electronically respond to mechanical changes can be used as strain sensors. However, these systems usually require external power to convert changes in strain into electrical signals. Here, a self-powered strain sensor is developed based on a gelatin-based hydrogel and a galvanic cell. In the hydrogel matrix, hydrophobic interactions and hydrogen bonding between tannic acid and gelatin give the prepared hydrogel great potential for elongation (1600%). The hydrogel also has a rapid self-healing ability (within 0.65 s) and high self-healing efficiency (95%). The hydrogel operates as an efficient electrolyte material and forms a hydrogel battery when assembled with a thin layer of zinc and an air electrode. This device had excellent tolerance to large compressional strain without sacrificing open-circuit voltage. On the basis of this hydrogel battery, we fabricated a self-powered strain sensor by connecting the hydrogel battery to a fixed resistor to form a closed loop. By converting its chemical energy into electrical energy, the self-powered sensor efficiently…

As a new class of two-dimensional materials, the MXene family has triggered attention because of its unique electrical and mechanical properties. MXene’s excellent electrical conductivity and hydrophilicity make it an ideal option for polymer nanocomposite fabrication. For the first time, polymer nanocomposites of polyvinyl alcohol (PVA)/Ti 3 C 2 T x (MXene) were used for charge storage applications in the X-band frequency range (8.2–12.4 GHz). By implementing solution casting and vacuum-assisted filtration (VAF), flexible thin films with exceptional dielectric properties (solution casting @ 10.0 wt % MXene: ε′ = 370.5 and tan δ = 0.11 and VAF @ 10.0 wt % MXene: ε′ = 3166 and tan δ = 0.09) were fabricated. The reported dielectric constants in this study are among the highest values obtained in X-band frequency with low dielectric losses. This outstanding performance originates from the high electrical conductivity of synthesized Ti 3 C 2 T x MXene (σ ≈ 1.4 ± 0.077 × 10 6 S/m; the highest reported value for Ti 3 C 2 T x MXene to date in the literature), great dispersion state, and…

Abstract For many photonic applications, it is important to confine light of a specific wavelength at a certain volume of interest at low losses. So far, it is only possible to use the polarized light perpendicular to the solid grid lines to excite waveguide–plasmon polaritons in a waveguide-supported hybrid structure. In our work, we use a plasmonic grating fabricated by colloidal self-assembly and an ultrathin injection layer to guide the resonant modes selectively. We use gold nanoparticles self-assembled in a linear template on a titanium dioxide (TiO2) layer to study the dispersion relation with conventional ultraviolet–visible–near-infrared spectroscopic methods. Supported with finite-difference in time-domain simulations, we identify the optical band gaps as hybridized modes: plasmonic and photonic resonances. Compared to metallic grids, the observation range of hybridized guided modes can now be extended to modes along the nanoparticle chain lines. With future applications in energy conversion and optical filters employing these cost-efficient and upscalable directed…

Metal–organic frameworks (MOFs), as newly emerging materials, show compelling intrinsic structural features, e.g., the highly crystalline nature and designable and tunable porosity, as well as tailorable functionality, rendering them suitable for proton-conducting materials. The proton conduction of MOF is significantly improved using the postsynthesis or encapsulation strategy. In this work, the MOF-based proton-conducting material Im@MOF-808 has been prepared by incorporating the imidazole molecules into the pores of proton-conducting MOF-808. Compared with MOF-808, Im@MOF-808 not only possesses higher proton conductivity of 3.45 × 10 –2 S cm –1 at 338 K and 99% RH, superior to that of any imidazole-encapsulated proton-conducting materials reported to date, but also good durable and stable proton conduction. Moreover, the thermal stability of H-bond networks is much improved owing to the water molecules partially replaced by higher boiling point imidazole molecules. Additionally, it is further discussed for the possible mechanism of imidazole encapsulation into the pores of…

It was expected that the properties of intrinsic point defects would be simple in the binary semiconductor Sb 2 Se 3 . However, we show using first-principles calculations that the intrinsic defects in this quasi-one-dimensional (Q1D) semiconductor are unexpectedly complicated and different from those in conventional photovoltaic semiconductors such as CdTe or GaAs. First, the same type of defects located on non-equivalent atomic sites can have very different properties due to the low symmetry of the Q1D structure, which makes the properties of point defects complicated, even though there are only a few point defects. Second, uncommon defects such as the cation-replace-anion antisite Sb Se, anion-replace-cation antisite Se Sb, and even two-anion-replace-one-cation antisite 2Se Sb, which are difficult to form in CdTe and GaAs, can have high concentrations and even be dominant in Sb 2 Se 3 due to the weak van der Waals interactions and the large void space between different [Sb 4 Se 6 ] n atomic chains of the Q1D structure. These defects produce a series of acceptor and donor levels…

Metal–organic framework (MOF) based proton conductors have received immense importance recently. The present study endeavors to design two post synthetically modified UiO-66-based MOFs and examines the effects of their structural differences on their proton conductivity. UiO-66-NH 2 is modified by reaction with sultones to prepare two homologous compounds, that is, PSM 1 and PSM 2, with SO 3 H functionalization in comparable extent (Zr:S = 2:1) in both. However, the pendant alkyl chain holding the −SO 3 H group is of different length. PSM 2 has longer alkyl chain attachment than PSM 1 . This difference in the length of side arms results in a huge difference in proton conductivity of the two compounds. PSM 1 is observed to have the highest MOF-based proton conductivity (1.64 × 10 –1 S cm –1 ) at 80 °C, which is comparable to commercially available Nafion, while PSM 2 shows significantly lower conductivity (4.6 × 10 –3 S cm –1 ). Again, the activation energy for proton conduction is one of the lowest among all MOF-based proton conductors in the case of PSM 1, while PSM 2 requires…

Electrochemical reduction of carbon dioxide to hydrocarbons, driven by renewable power sources, is a fascinating and clean way to remedy greenhouse gas emission as a result of overdependence on fossil fuels and produce value-added fine chemicals. The Cu-based catalysts feature unique superiorities; nevertheless, achieving high hydrocarbon selectivity is still inhibited and remains a great challenge. In this study, we report on a tailor-made multifunction-coupled Cu-metal–organic framework (Cu-MOF) electrocatalyst by time-resolved controllable restructuration from Cu 2 O to Cu 2 O@Cu-MOF. The restructured electrocatalyst features a time-responsive behavior and is equipped with high specific surface area for strong adsorption capacity of CO 2 and abundant active sites for high electrocatalysis activity based on the as-produced MOF on the surface of Cu 2 O, as well as the accelerated charge transfer derived from the Cu 2 O core in comparison with the Cu-MOF. These intriguing characteristics finally lead to a prominent performance towards hydrocarbons, with a high hydrocarbon Faradaic…

Metal–organic frameworks (MOFs) have been considered as a class of promising electrode materials for supercapacitors owing to their large surface area, rich porosity, and variable redox sites; however, direct application of pristine MOFs in energy storage has been largely hindered by their poor electrical conductivity and stability issues. In this work, we demonstrate a facile two-step approach to address the controlled growth of Ni-MOF arrays on the surface of NiCo 2 O 4 nanowires by modulating the formation reaction of MOFs. By taking advantage of the intriguing merits from the NiCo 2 O 4 core and Ni-MOF shell as well as their synergistic effects, the optimized NiCo 2 O 4 @Ni-MOF hybrid electrode exhibits boosted electrochemical performance, in terms of high specific capacity (208.8 mA h/g at 2 mA/cm 2 ) and good rate capability. In addition, the assembled flexible solid-state HSC device based on the optimized NiCo 2 O 4 @Ni-MOF and activated carbon as the cathode and anode achieves a maximum energy density of 32.6 W h/kg at a power density of 348.9 W/kg without sacrificing its…

Cartilage tissue is deprived of intrinsic self-regeneration capability; hence, its damage often progresses to a chronic condition which reduces the quality of life. Toward the fabrication of functional tissue substitutes, three-dimensional (3D) bioprinting has progressed vastly over the last few decades. However, this progress is challenged by the difficulty in developing suitable bioink materials as most of them require toxic chemical cross-linking. In this study, our goal was to develop a cross-linker-free bioink with optimal rheology for polymer extrusion, aqueous, and nontoxic processing and offers structural support for cartilage regeneration. Toward this, we use the self-gelling ability of silk fibroin blends ( Bombyx mori and Philosamia ricini ) along with gelatin as a bulking agent. Silk and gelatin interact with each other through entanglement and physical cross-linking. The ink was rheologically and structurally optimized for printing efficiency in printing grid-like structures. The printed 3D constructs show optimal swelling capability, degradability, and compressive…

Two-dimensional lattice structures with specific geometric features have been reported to have a negative Poisson's ratio, termed as auxetic metamaterials, that is, stretching-induced expansion in the transversal direction. In this paper, we designed a novel auxetic metamaterial; by utilizing the shape memory effect of the constituent materials, the in-plane moduli and Poisson's ratios can be continuously tailored. During deformation, the curved meshes ensure the rotation of the mesh joints to achieve auxetics. The rotations of these mesh joints are governed by the mesh curvature, which continuously changes during deformation. Because of the shape memory effect, the mesh curvature after printing can be programmed, which can be used to tune the rotation of the mesh joints and the mechanical properties of auxetic metamaterial structures, including Poisson's ratios, moduli, and fracture strains. Using the finite element method, the deformation of these auxetic meshes was analyzed. Finally, we designed and fabricated gradient/digital patterns and cylindrical shells and used the auxetics…

Wound repair and tissue regeneration are complex processes that involve many physiological signals. Thus, employing novel wound dressings with potent biological activity and physiological signal response ability to accelerate wound healing is a possible solution. Herein, inspired by mussel chemistry, we developed a polydopamine (PDA)-reduced graphene oxide (pGO)-incorporated chitosan (CS) and silk fibroin (SF) (pGO-CS/SF) scaffold with good mechanical, electroactive, and antioxidative properties as an efficient wound dressing. First, pGO with good dispersibility and cell affinity was obtained upon reduction by PDA under alkali conditions. Second, pGO was dispersed into a CS/SF mixture, and then CS and SF chains were dual-cross-linked by poly(ethylene glycol) diglycidyl ether and glutaraldehyde to obtain a pGO-incorporated gel. Finally, the gel underwent a freeze-dry process to obtain the pGO-CS/SF scaffold. Owing to PDA reduction and functionalization, pGO in the scaffold plays important roles for the performances of the scaffolds. First, the pGO acts as nanoreinforcement to enhance…

In recent times, high-performance flexible pressure sensors that can be fabricated in an environmentally friendly and low-cost manner have received considerable attention owing to their potential applications in wearable health monitors and intelligent soft robotics. This paper proposes a highly sensitive flexible piezoresistive pressure sensor based on hybrid porous microstructures that can be designed and fabricated using a bio-inspired and low-cost approach employing the Epipremnum aureum leaf and sugar as the template. The sensitivity and detection limit of the obtained pressure sensor can be as high and low as 83.9 kPa –1 (<140 Pa) and 0.5 Pa, respectively. According to the mechanism and simulation analyses, the hybrid porous microstructures lower the effective elastic modulus of the sensor and introduce an additional pore resistance, which increases the contact area and conductive path with loads, thereby contributing to the high sensitivity that exceeds that of traditional microstructured pressure sensors. Real-time monitoring of human physiological signals such as finger…

Recent developments in various technologies, such as hybrid electric vehicles and pulsed power systems, have challenged researchers to discover affordable, compact, and super-functioning electric energy storage devices. Among the existing energy storage devices, polymer nanocomposite film capacitors are a preferred choice due to their high power density, fast charge and discharge speed, high operation voltage, and long service lifetime. In the past several years, they have been extensively researched worldwide, with 0D, 1D, and 2D nanofillers being incorporated into various polymer matrixes. However, 1D nanofillers appeared to be the most effective in producing large dipole moments, which leads to a considerably enhanced dielectric permittivity and energy density of the nanocomposite. As such, this Review focuses on recent advances in polymer matrix nanocomposites using various types of 1D nanofillers, i.e., linear, ferroelectric, paraelectric, and relaxor-ferroelectric for energy storage applications. Correspondingly, the latest developments in the nanocomposite dielectrics with…

Stretchable electronic materials have drawn strong interest due to their important applications in areas such as bioelectronics, wearable devices, and soft robotics. The stretchable electrode is an integral unit of stretchable systems. Intrinsically conductive polymers such as poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) can have high mechanical flexibility and good biocompatibility. However, their electrical conductivity and mechanical stretchability should be greatly improved for its applications as the stretchable electrode. Here, we report highly conductive and highly stretchable PEDOT:PSS by incorporating biocompatible d-sorbitol. d-Sorbitol can serve as both the secondary dopant and plasticizer for PEDOT:PSS. It can not only significantly improve the conductivity but also the stretchability. d-Sorbitol-PEDOT:PSS (s-PEDOT:PSS) can have a conductivity of >1000 S/cm, and the conductivity could be maintained at a strain up to 60%. The resistance of s-PEDOT:PSS remains almost constant during repeated stretching-releasing cycles. The mechanism for the…

A highly-sensitive ammonia (NH 3 ) gas sensor based on molybdenum trioxide nanoribbons was developed in this study. α-MoO 3 nanoribbons (MoO 3 NRs) were successfully synthesized via a hydrothermal method and systematically characterized using various advanced technologies. Following a simple drop-cast process, a high-performance chemiresistive NH 3 sensor was fabricated through the deposition of a MoO 3 NR sensing film onto Au interdigitated electrodes. At an optimal operation temperature of 450 °C, the MoO 3 nanoribbon-based sensor exhibited an excellent sensitivity (0.72) at NH 3 concentration as low as 50 ppb, a fast response time of 21 s, good stability and reproducibility, and impressive selectivity against the interfering gases such as H 2, NO 2, and O 2 . More importantly, the sensor represents a remarkable limit of detection of 280 ppt (calculated based on a signal-to-noise ratio of 3), which makes the as-prepared MoO 3 NR sensor the most sensitive NH 3 sensor in the literature. Moreover, density functional theory (DFT) simulations were employed to understand the adsorption…

Upconverting core@shell type β-NaYF 4:Yb 3+ –Er 3+ @SiO 2 nanorods have been obtained by a two-step synthesis process, which encompasses hydrothermal and microemulsion routes. The synthesized nanomaterial forms stable aqueous colloids and exhibits a bright dual-center emission (λ ex = 975 nm), i.e., upconversion luminescence of Er 3+ and down-shifting emission of Yb 3+, located in the first (I-BW) and the second (II-BW) biological windows of the spectral range, respectively. The intensity ratios of the emission bands of Er 3+ and Yb 3+ observed in the vis–near-infrared (NIR) range monotonously change with temperature, i.e., the thermalized Er 3+ levels ( 2 H 11/2 → 4 I 15/2 / 4 S 3/2 → 4 I 15/2 ) and the nonthermally coupled Yb 3+ /Er 3+ levels ( 2 F 5/2 → 2 F 7/2 / 4 I 9/2 → 4 I 15/2 or 4 F 9/2 → 4 I 15/2 ). Hence, their thermal evolutions have been correlated with temperature using the Boltzmann type distribution and second-order polynomial fits for temperature-sensing purposes, i.e., Er 3+ 525/545 nm (max S r = 1.31% K –1 ) and Yb 3+ /Er 3+ 1010/810 nm (1.64% K –1 ) or 1010/660…

The mussel-inspired properties of dopamine have attracted immense scientific interest for surface modification of nanoparticles due to the high potential of dopamine functional groups to increase the adhesion of nanoparticles to flat surfaces. Here, we report for the first time a novel type of inhibitor-loaded nanocontainer using polydopamine (PDA) as a pH-sensitive gatekeeper for mesoporous silica nanoparticles (MSNs). The encapsulated inhibitor (benzotriazole) was loaded into MSNs at neutral pH, demonstrating fast release in an acidic environment. The self-healing effect of water-borne alkyd coatings doped with nanocontainers was achieved by both on-demand release of benzotriazole during the corrosion process and formation of the complexes between the dopamine functional groups and iron oxides, thus providing dual self-healing protection for the mild steel substrate. The coatings were characterized by electrochemical impedance spectroscopy, visual observations, and confocal Raman microscopy. In all cases, the coatings with embedded benzotriazole-loaded MSNs with PDA-decorated…

Photomediated cancer therapy, mainly including photothermal (PT) therapy (PTT) and photodynamic therapy (PDT), has attracted tremendous attention in recent years thanks to its noninvasive and stimuli-responsive features. The single mode of PTT or PDT, however, has obvious drawbacks, either requiring high-power laser irradiation to generate enough heat or only providing limited efficacy due to the hypoxia nature inside tumors. In addition, the reported synergistic PTT/PDT generally utilized two excitation sources to separately activate PTT and PDT, and the problem of high-power laser irradiation for PTT was still not well solved. Herein, a new concept, loading a small amount of photosensitizers onto a PTT agent (both of them can be triggered by a single-near-infrared (NIR) laser), was proposed to evade the shortcomings of PTT and PDT. To validate this idea, minute quantities of photosensitizer chlorin e6 (Ce6) (0.56% of mass) were anchored onto amino-rich red emissive carbon dots (RCDs) that possess superior photothermal (PT) character under 671 nm NIR laser (PT conversion efficiency…

Humidity sensors have broad applications in health monitoring, environmental protection and human-machine interface, and robotics. Here, we developed a humidity sensor using alkali oxidation method to grow in situ TiO 2 nanowires on two-dimensional Ti 3 C 2 MXene. With an order of magnitude larger surface area compared to pure Ti 3 C 2 or TiO 2 materials, the urchin-like Ti 3 C 2 /TiO 2 composite demonstrates a record high sensitivity in a low relative humidity (RH) environment (∼280 pF/% RH from 7% RH to 33% RH). Complex impedance spectroscopy and Schottky junction theory were employed to understand the underlying sensing mechanisms of the Ti 3 C 2 /TiO 2 composite under various humidity conditions. We demonstrate the application of humidity sensors made with the Ti 3 C 2 /TiO 2 composite for noncontact detection of the presence of various liquids as well as human fingers.

Solar-blind photodetectors have captured intense attention due to their high significance in ultraviolet astronomy and biological detection. However, most of the solar-blind photodetectors have not shown extraordinary advantages in weak light signal detection because the forewarning of low-dose deep-ultraviolet radiation is so important for the human immune system. In this study, a high-performance solar-blind photodetector is constructed based on the n -Ga 2 O 3 / p -CuSCN core–shell microwire heterojunction by a simple immersion method. In comparison with the single device of the Ga 2 O 3 and CuSCN, the heterojunction photodetector demonstrates an enhanced photoelectric performance with an ultralow dark current of 1.03 pA, high photo-to-dark current ratio of 4.14 × 10 4, and high rejection ratio ( R 254 / R 365 ) of 1.15 × 10 4 under a bias of 5 V. Excitingly, the heterostructure photodetector shows high sensitivity to the weak signal (1.5 μW/cm 2 ) of deep ultraviolet and high-resolution detection to the subtle change of signal intensity (1.0 μW/cm 2 ). Under the illumination…