The 100 most-cited articles in ACS Applied Materials & Interfaces, 2020

Aptamers are oligonucleotide sequences with a length of about 25-80 bases which have abilities to bind to specific target molecules that rival those of monoclonal antibodies. They are attracting great attention in diverse clinical translations on account of their various advantages, including prolonged storage life, little batch-to-batch differences, very low immunogenicity, and feasibility of chemical modifications for enhancing stability, prolonging the half-life in serum, and targeted delivery. In this Review, we demonstrate the emerging aptamer discovery technologies in developing advanced techniques for producing aptamers with high performance consistently and efficiently as well as requiring less cost and resources but offering a great chance of success. Further, the diverse modifications of aptamers for therapeutic applications including therapeutic agents, aptamer-drug conjugates, and targeted delivery materials are comprehensively summarized.

Flexible, lightweight, robust, and multifunctional characteristics are greatly desirable for next-generation wearable electromagnetic interference (EMI) shielding materials. In this work, an alternating multilayered structure with robust polymer frame layers and directly contacted conducting layers was designed to prepare high-performance EMI films. Especially, the multilayered films containing alternating cellulose nanofiber (CNF) layers and MXene layers are fabricated via a facile and efficient alternating vacuum filtration approach. Deriving from the mechanical frame effect acted by CNF layers in, which is capable of preventing the nanosized “zigzag” crack in MXene layers from growing to the whole film, the alternating multilayered film (CNF@MXene) revealed the improved mechanical strength (112.5 MPa) and toughness (2.7 MJ m –3 ) compared to both freestanding MXene film and homogeneous CNF/MXene film. Meanwhile, the directly contacted MXene layers resulted in the increased electrical conductivity from 2 (homogeneous CNF/MXene film) to 621–82 S m –1 (CNF@MXene films). In…

The effective dissipation of heat is critical to the performance and longevity of high-power electronics, so it is important to prepare highly thermally conductive polymer-based packaging materials for efficient thermal management. Due to the excellent thermal conductivity of boron nitride nanosheets (BNNSs), the hexagonal boron nitride (hBN) powder was dissolved in a mixed solution of isopropanol and deionized water for ultrasonic exfoliation to obtain hydroxylated BN nanosheets. Then, the prepared BNNS was functionalized with (3-aminopropyl)triethoxysilane (APTES) to enhance its dispersibility and interfacial compatibility in the epoxy resin, which play an important role in the improvement of the thermal conductivity of the composites. Finally, APTES-BNNS was uniformly dispersed in the epoxy resin by solvent mixing, and the oriented APTES-BNNS/epoxy composites were prepared through spin-coating and hot-pressing methods. It was found that APTES-BNNS/epoxy composites prepared herein exhibited significant anisotropic thermal conductivity. The results show that the thermal…

Abstract This paper presents flexible pressure sensors based on free-standing and biodegradable glycine–chitosan piezoelectric films. Fabricated by the self-assembly of biological molecules of glycine within a water-based chitosan solution, the piezoelectric films consist of a stable spherulite structure of β-glycine (size varying from a few millimeters to 1 cm) embedded in an amorphous chitosan polymer. The polymorphic phase of glycine crystals in chitosan, evaluated by X-ray diffraction, confirms formation of a pure ferroelectric phase of glycine (β-phase). Our results show that a simple solvent-casting method can be used to prepare a biodegradable β-glycine/chitosan-based piezoelectric film with sensitivity (∼2.82 ± 0.2 mV kPa–1) comparable to those of nondegradable commercial piezoelectric materials. The measured capacitance of the β-glycine/chitosan film is in the range from 0.26 to 0.12 nF at a frequency range from 100 Hz to 1 MHz, and its dielectric constant and loss factor are 7.7 and 0.18, respectively, in the high impedance range under ambient conditions. The results…

In recent years, highly sensitive pressure sensors that are flexible, biocompatible, and stretchable have attracted significant research attention in the fields of wearable electronics and smart skin. However, there has been a considerable challenge to simultaneously achieve highly sensitive, low-cost sensors coupled with optimum mechanical stability and an ultralow detection limit for subtle physiological signal monitoring devices. Targeting aforementioned issues, herein, we report the facile fabrication of a highly sensitive and reliable capacitive pressure sensor for ultralow-pressure measurement by sandwiching MXene (Ti 3 C 2 T x )/poly(vinylidene fluoride-trifluoroethylene) (PVDF-TrFE) composite nanofibrous scaffolds as a dielectric layer between biocompatible poly-(3,4-ethylenedioxythiophene) polystyrene sulfonate /polydimethylsiloxane electrodes. The fabricated sensor exhibits a high sensitivity of 0.51 kPa –1 and a minimum detection limit of 1.5 Pa. In addition, it also enables linear sensing over a broad pressure range (0–400 kPa) and high reliability over 10,000 cycles…

The effective capture of radioiodine, produced or released from nuclear-related activities, is of paramount importance for the sustainable development of nuclear energy. Here, a series of zirconium-based metal–organic frameworks (Zr-MOFs), with a Zr 6 (μ 3 -O) 4 (μ 3 -OH) 4 cluster and various carboxylate linkers, were investigated for the capture of volatile iodine. Their adsorption kinetics and recyclability were investigated in dry and humid environments. The structural change of Zr-MOFs during iodine trapping was studied using powder X-ray diffraction and pore structure measurements. Experimental spectra (Raman and X-ray photoelectron spectroscopy) and density functional theory (DFT) calculations for the linkers and Zr clusters were performed to understand the trapping mechanism of the framework. When interacting with iodine molecules, MOF-808, NU-1000, and UiO-66, with highly connected and/or rigid linkers, have better structural stability than UiO-67 and MOF-867, which have flexible linkers with less connectivity. Particularly, MOF-808, with a rigid and tritopic…

Paper, as a flexible, low-cost, lightweight, tailorable, environmental-friendly, degradable, and renewable material, is emerging in electronic devices. Especially, many kinds of paper-based (PB) sensors have been reported for wearable applications in recent years. Among them, the PB gas, humidity, and strain sensors are widely studied for monitoring gas, humidity, and strain from the human body and the environment. However, gas, humidity, and strain often coexist and interact, and the paper itself is hydrophilic and flexible, resulting in that it is still challenging to develop high-performance PB sensors specialized for gas, humidity, and strain detections. Therefore, it is necessary to summarize and discuss them systematically. In this review, we focus on summarizing the state-of-art studies of the PB gas, humidity, and strain sensors. Specifically, the fabrications (electrodes and sensing materials) and applications of PB gas, humidity, and strain sensors are summarized and discussed. The current challenges and the potential trends of PB sensors for gas, humidity, and strain…

Graphene-based fibers (GFs) have aroused enormous interest in portable, wearable electronics because of their excellent mechanical flexibility, electrical conductivity, and weavability, which make them advantageous for wearable electronic devices. Herein, we report the development of metal binder-free Ti 3 C 2 T x MXene/graphene hybrid fibers by a scalable wet-spinning process. These hybrid fibers exhibit excellent mechanical and electrical properties for applications in flexible wearable gas sensors. The synergistic effects of electronic properties and gas-adsorption capabilities of MXene/graphene allow the created fibers to show high NH 3 gas sensitivity at room temperature. The hybrid fibers exhibited significantly improved NH 3 sensing response (Δ R / R 0 = 6.77%) compared with individual MXene and graphene. The hybrid fibers also showed excellent mechanical flexibility with a minimal fluctuation of resistance of ±0.2% and low noise resistance even after bending over 2000 cycles, enabling gas sensing during deformation. Furthermore, flexible MXene/graphene hybrid fibers were…

Nanofiltration plays an increasingly large role in many industrial applications, such as water treatment (e.g., desalination, water softening, and fluoride removal) and resource recovery (e.g., alkaline earth metals). Energy consumption and benefits of nanofiltration processes are directly determined by the selectivity of the nanofiltration membranes, which is largely governed by pore-size distribution and Donnan effects. During operation, the separation performance of unmodified nanofiltration membranes will also be impacted (deleteriously) upon unavoidable membrane fouling. Many efforts, therefore, have been directed toward enhancing the selectivity of nanofiltration membranes, which can be classified into membrane fabrication method improvement and process intensification. This review summarizes recent developments in the field and provides guidance for potential future approaches to improve the selectivity of nanofiltration membranes.

Nowadays, great effort has been devoted to establishing wearable electronics with excellent stretchability, high sensitivity, good mechanical strength, and multifunctional characteristics. Herein, a soft conductive hydrogel is rationally designed by proportionally mixing silk fibroin, polyacrylamide, graphene oxide, and poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate). The resultant hydrogel has considerable stretchability and compressibility, which enables it to be assembled into a strain/pressure sensor with a wide sensing range (strain, 2%-600%; pressure, 0.5-119.4 kPa) and reliable stability. Then, the corresponding sensor is capable of monitoring a series of physical signals of the human body (e.g., joint movement, facial gesture, pulse, breathing, etc.). In particular, the hydrogel-based sensor is biocompatible, with no anaphylactic reaction on human skin. More interestingly, this conductive hydrogel exhibits a positive response when it works in a triboelectric nanogenerator; consequently, it lights up 20 commericial green light-emitting diodes. Thus, this silk…

Abstract Solar-steam generation is one of the most promising technologies to mitigate the issue of clean water shortage using sustainable solar energy. Photothermal aerogels, especially the three-dimensional (3D) graphene-based aerogels, have shown unique merits for solar-steam generation, such as lightweight, high flexibility, and superior evaporation rate and energy efficiency. However, 3D aerogels require much more raw materials of graphene, which limits their large-scale applications. In this study, 3D photothermal aerogels composed of reduced graphene oxide (RGO) nanosheets, rice-straw-derived cellulose fibers, and sodium alginate (SA) are prepared for solar-steam generation. The use of rice straw fibers as skeletal support significantly reduces the need for the more expensive RGO by 43.5%, turning the rice straw biomass waste into value-added materials. The integration of rice straw fibers and RGO significantly enhances the flexibility and mechanical stability of the obtained photothermal RGO–SA–cellulose aerogel. The photothermal aerogel shows a strong broad-band light…

Daytime radiative coolers are used to pump excess heat from a target object into a cold exterior space without energy consumption. Radiative coolers have become attractive cooling options. In this study, a daytime radiative cooler was designed to have a selective emissive property of electromagnetic waves in the atmospheric transparency window of 8–13 μm and preserve low solar absorption for enhancing radiative cooling performance. The proposed daytime radiative cooler has a simple multilayer structure of inorganic materials, namely, Al 2 O 3, Si 3 N 4, and SiO 2, and exhibits high emission in the 8–13 μm region. Through a particle swarm optimization method, which is based on an evolutionary algorithm, the stacking sequence and thickness of each layer were optimized to maximize emissions in the 8–13 μm region and minimize the cooling temperature. The average value of emissivity of the fabricated inorganic radiative cooler in the 8–13 μm range was 87%, and its average absorptivity in the solar spectral region (0.3–2.5 μm) was 5.2%. The fabricated inorganic radiative cooler was…

Targeted delivery to the diseased cell or tissue is the key to the successful clinical use of nucleic acid drugs. In particular, delivery of microRNA-140 (miRNA-140, miR-140) into chondrocytes across the dense, nonvascular extracellular matrix of cartilage remains a major challenge. Here, we report the chondrocyte-targeting exosomes as vehicles for the delivery of miR-140 into chondrocytes as a new treatment for osteoarthritis (OA). By fusing a chondrocyte-affinity peptide (CAP) with the lysosome-associated membrane glycoprotein 2b protein on the surface of exosomes, we acquire CAP-exosomes that can efficiently encapsulate miR-140, specifically enter, and deliver the cargo into chondrocytes in vitro. CAP-exosomes, in contrast to nontagged exosome vesicles, are retained in the joints after intra-articular injection with minimal diffusion in vivo. CAP-exosomes also deliver miR-140 to deep cartilage regions through the dense mesochondrium, inhibit cartilage-degrading proteases, and alleviate OA progression in a rat model, pointing toward a potential organelle-based, cell-free therapy…

Conductive hydrogels have become one of the most promising materials for skin-like sensors because of their excellent biocompatibility and mechanical flexibility. However, the limited stretchability, low toughness, and fatigue resistance lead to a narrow sensing region and insufficient durability of the hydrogel-based sensors. In this work, an extremely stretchable, highly tough, and anti-fatigue conductive nanocomposite hydrogel is prepared by integrating hydrophobic carbon nanotubes (CNTs) into hydrophobically associated polyacrylamide (HAPAAm) hydrogel. In this conductive hydrogel, amphiphilic sodium dodecyl sulfate was used to ensure uniform dispersion of CNTs in the hydrogel network, and hydrophobic interactions between the hydrogel matrix and the CNT surface formed, greatly improving the mechanical properties of the hydrogel. The obtained CNTs/HAPAAm hydrogel showed excellent stretchability (ca. 3000%), toughness (3.42 MJ m –3 ), and great anti-fatigue property. Moreover, it exhibits both high tensile strain sensitivity in the wide strain ranges (gauge factor = 4.32, up to…

Detection of volatile organic compounds (VOCs) at room temperature (RT) currently remains a challenge for metal oxide semiconductor (MOS) gas sensors. Herein, for the first time, we report on the utilization of porous SnO 2 thin films for RT detection of VOCs by defect engineering of oxygen vacancies. The oxygen vacancies in the three-dimensional-ordered SnO 2 thin films, prepared by a colloidal template method, can be readily manipulated by thermal annealing at different temperatures. It is found that oxygen vacancies play an important role in the RT sensing performances, which successfully enables the sensor to respond to triethylamine (TEA) with an ultrahigh response, for example, 150.5–10 ppm TEA in a highly selective manner. In addition, the sensor based on oxygen vacancy-rich SnO 2 thin films delivers a fast response and recovery speed (53 and 120 s), which can be further shortened to 10 and 36 s by elevating the working temperature to 120 °C. Notably, a low detection limit of 110 ppb has been obtained at RT. The overall performances surpass most previous reports on TEA…

Cryogels with tissue adhesion have great potential as wound dressings for rapid hemostasis for uncontrollable nonpressing surface hemorrhage and wound healing, but their use has not been reported previously. Herein, we designed a series of antibacterial and antioxidant tissue-adhesive cryogels based on quaternized chitosan (QCS) and polydopamine (PDA). These cryogels had good blood cell and platelet adhesion, enrichment, and activation properties for rapid nonpressing surface hemostasis and wound healing. The cryogels exhibited outstanding mechanical strength and easy removability, antioxidant activity, and NIR photothermal-enhanced antibacterial performance. The cryogels showed much better hemostasis than gauze and gelatin sponge in a standardized strip rat liver injury model, a standardized circular rabbit liver section model, and a pig skin laceration model. Furthermore, the excellent hemostatic performance of the QCS/PDA2.0 cryogel (containing 20 mg/mL QCS and 2.0 mg/mL PDA) for coagulopathic hemorrhages was confirmed in a standardized coagulation disorder rabbit circular liver…

Organic and polymer materials have been extensively investigated as electrode materials for rechargeable batteries because of the low cost, abundance, environmental benignity, and high sustainability. To date, organic electrode materials have been applied in a large variety of energy storage devices, including nonaqueous Li-ion, Na-ion, K-ion, dual-ion, multivalent-metal, aqueous, all-solid-state, and redox flow batteries, because of the universal properties of organic electrode materials. Moreover, some organic materials enable the batteries to be operated in the extreme conditions, such as a wide temperature range (−70 to 150 °C), a wide pH range, and in the presence of O 2 . As a guidance for the research in organic batteries, this Review focuses on the reaction mechanisms and applications of organic electrode materials. Six categories of reaction mechanisms and the applications of organic and polymer materials in various rechargeable batteries are discussed to provide an overview of the state-of-the-art organic batteries.

Although flexible and multifunctional textile-based electronics are promising for wearable devices, it is still a challenge to seamlessly integrate excellent conductivity into textiles without sacrificing their intrinsic flexibility and breathability. Herein, the vertically interconnected conductive networks are constructed based on a meshy template of weave cotton fabrics with interwoven warp and weft yarns. The two-dimensional early transition metal carbides/nitrides (MXenes), with unique metallic conductivity and hydrophilic surfaces, are uniformly and intimately attached to the preformed fabric via a spray-drying coating approach. Through adjusting the spray-drying cycles, the degree of conductive interconnectivity for the fabrics is precisely tuned, thereby affording highly conductive and breathable fabrics with integrated Joule heating, electromagnetic interference (EMI) shielding and strain sensing performances. Interestingly, triggered by the interwoven conductive architecture, the MXene-decorated fabrics with a low loading of 6 wt % (0.78 mg cm –2 ) offer an outstanding…

Abstract Commercial or clinical tissue adhesives are currently limited due to their weak bonding strength on wet biological tissue surface, low biological compatibility, and slow adhesion formation. Although catechol-modified hyaluronic acid (HA) adhesives are developed, they suffer from limitations: insufficient adhesiveness and overfast degradation, attributed to low substitution of catechol groups. In this study, we demonstrate a simple and efficient strategy to prepare mussel-inspired HA hydrogel adhesives with improved degree of substitution of catechol groups. Because of the significantly increased grafting ratio of catechol groups, dopamine-conjugated dialdehyde–HA (DAHA) hydrogels exhibit excellent tissue adhesion performance (i.e., adhesive strength of 90.0 ± 6.7 kPa), which are significantly higher than those found in dopamine-conjugated HA hydrogels (∼10 kPa), photo-cross-linkable HA hydrogels (∼13 kPa), or commercially available fibrin glues (2–40 kPa). At the same time, their maximum adhesion energy is 384.6 ± 26.0 J m–2, which also is 40–400-fold, 2–40-fold, and…

Flexible electromagnetic interference (EMI) shielding materials with excellent thermal conductivities and Joule heating performances are of urgent demand in the communication industry, artificial intelligence, and wearable electronics. In this work, highly conductive silver nanowires (AgNWs) were prepared using the polyol method. Cellulose sheets were then prepared by dissolving natural cotton in a green and efficient NaOH/urea aqueous solution. Finally, multifunctional flexible EMI shielding AgNWs/cellulose films were fabricated based on vacuum-assisted filtration and hot-pressing. AgNWs are evenly embedded in the inner cellulose matrix and overlap with each other to form a 3D network. AgNWs/cellulose films, with a thickness of 44.5 μm, obtain the superior EMI shielding effectiveness of 101 dB, which is the highest value ever reported for shielding materials with the same thickness. In addition, AgNWs/cellulose films present excellent tensile strength (60.7 MPa) and tensile modulus (3.35 GPa), ultrahigh electrical conductivity (σ, 5571 S/cm), and excellent in-plane thermal…

Excellent electromagnetic interference (EMI) shielding ability, light weight, and good heat resistance are highly required for practical applications of EMI shielding materials, such as in areas of aerospace, aircraft, and automobiles. Herein, a lightweight and robust carbon nanotube (CNT)/polyimide (PI) foam was developed for efficient and heat-resistant EMI shielding. Thanks to poly(vinyl pyrrolidone) (PVP) as a surfactant that not only promotes the uniform dispersion of CNTs to form perfect CNT conductive networks but also can be removed in situ during the polymerization process, the density of resultant CNT/PI foam is only 32.1 mg·cm –3, and the EMI shielding effectiveness (EMI SE) is up to 41.1 dB, which represents one of the highest EMI SE values compared to previously reported polymer-based foams. The CNT/PI foam also achieves the absorption coefficient ( A ) of up to 82.3%, which is very impressive in CNT/polymer foams at comparable EMI SE levels. The PI matrix endows the foam with excellent heat resistance. The as-prepared CNT/PI foam presents a higher EMI SE than 35 dB…

Passive anti-icing or icephobic superhydrophobic surfaces have attracted great interest due to their potential multifaceted implications for the prevention and/or easy removal of undesired ice in many applications. However, a superhydrophobic surface with both excellent anti-icing and icephobic performances has rarely been reported due to difficulties in sustaining a good Cassie state stability. This is the case especially under high humidity and freezing environment conditions. In the present study, a new triple-scale micro/nanostructured superhydrophobic surface with both excellent anti-icing and icephobic properties has been designed via a hybrid method, combining ultrafast laser ablation and chemical oxidation. The novel surface structure is composed of periodical microcone arrays covered with densely grown nanograsses and dispersedly distributed microflowers. This surface exhibits an excellent Cassie state stability with its critical Laplace pressure reaching up to 1450 Pa, which is essential for good anti-icing and icephobic performances. The anti-icing feature of the prepared…

Transparent conductive film (TCF) is promising for optoelectronic instrument applications. However, designing a robust, stable, and flexible TCF that can shield electromagnetic waves and work in harsh conditions remains a challenge. Herein, a multifunctional and flexible TCF with effective electromagnetic interference shielding (EMI) performance and outstanding electro-photo-thermal effect is proposed by orderly coating Ti 3 C 2 T x MXene and a silver nanowire (AgNW) hybrid conductive network using a simple and scalable solution-processed method. Typically, the air-plasma-treated polycarbonate (PC) film was sequentially spray-coated with MXene and AgNW to construct a highly conductive network, which was transferred and partly embedded into an ultrathin poly(vinyl alcohol) (PVA) film using spin coating coupled with hot pressing to enhance the interfacial adhesion. The peeled MXene/AgNW-PVA TCF exhibits an optimal optical and electrical performance of sheet resistance 18.3 Ω/sq and transmittance 52.3%. As a consequence, the TCF reveals an effective EMI shielding efficiency of 32 dB in…

The electrochemical nitrogen reduction reaction (NRR) is a very efficient method for sustainable NH 3 production, but it requires effective catalysts to expedite the NRR kinetics and inhibit the concomitant hydrogen evolution reaction (HER). Two-dimensional (2D)/2D interface engineering is an effective method to design powerful catalysts due to intimate face-to-face contact of two 2D materials that facilitates the strong interfacial electronic interactions. Herein, we explored a 2D/2D MoS 2 /C 3 N 4 heterostructure as an active and stable NRR catalyst. MoS 2 /C 3 N 4 exhibited a conspicuously improved NRR performance with an NH 3 yield of 18.5 μg h –1 mg –1 and a high Faradaic efficiency (FE) of 17.8% at −0.3 V, far better than those of the individual MoS 2 or C 3 N 4 component. Density functional theory calculations revealed that the interfacial charge transport from C 3 N 4 to MoS 2 could enhance the NRR activity of MoS 2 /C 3 N 4 by promoting the stabilization of the key intermediate *N 2 H on Mo edge sites of MoS 2 and concurrently decreasing the reaction energy barrier.…

Anisotropic polyimide (PI)/graphene composite aerogels were fabricated by unidirectional freezing. A poly(amic acid) (PAA) ammonium salt/graphene dispersion was first synthesized by mixing together PAA, H 2 O, triethylamine (TEA), and graphene and then was successively subjected to one-way freezing, freeze-drying, and thermal imidization. The one-way growth of ice crystals endowed the composite aerogels with highly arranged tubular pores. The PI/graphene composite aerogels possessed anisotropic conductivity, electromagnetic interference (EMI) shielding, heat transfer, and compression performance. Moreover, the composite aerogels with low density (0.076 g·cm –3 ) exhibited high EMI shielding effectiveness (SE) of 26.1–28.8 dB, and its specific EMI SE value achieved 1373–1518 dB·cm 2 ·g –1 when the graphene content was 13 wt %. The main electromagnetic interference shielding mechanism of these composite aerogels was microwave absorption. The composite aerogels had excellent thermal stability, and their 5% weight loss temperature was higher than 546 °C in nitrogen. This research…

Layered two-dimensional (2D) graphene oxide (GO) films are integrated with silicon-on-insulator (SOI) nanowire waveguides to experimentally demonstrate an enhanced Kerr nonlinearity, observed through self-phase modulation (SPM). The GO films are integrated with SOI nanowires using a large-area, transfer-free, layer-by-layer coating method that yields precise control of the film thickness. The film placement and coating length are controlled by opening windows in the silica cladding of the SOI nanowires. Owing to the strong mode overlap between the SOI nanowires and the highly nonlinear GO films, the Kerr nonlinearity of the hybrid waveguides is significantly enhanced. Detailed SPM measurements using picosecond optical pulses show significant spectral broadening enhancement for SOI nanowires coated with 2.2 mm long films of 1-3 layers of GO and 0.4 mm long films with 5-20 layers of GO. By fitting the experimental results with theory, the dependence of GO's Kerr nonlinearity on layer number and pulse energy is obtained, showing interesting physical insights and trends of the layered…

Magnesium (Mg) and its alloys are regarded as the most promising engineering materials because of their unique property. However, the Mg alloys were easily corroded in humid environments, which restricted their wider applications. Herein, the superhydrophobic ZIF-8/PVDF/LDH (SZPL) double-layered coating was fabricated on Mg alloys via electrodeposition and dip-coating methods, which consisted of the underlying layered double hydroxide (LDH) transition structure and top superhydrophobic zeolitic imidazolate framework-8 (ZIF-8) layer. Besides, the LDH transition structure not only worked as a protection shield but also strengthened the binding force between the substrate and the top superhydrophobic ZIF-8 layer. The top superhydrophobic ZIF-8 layer could serve as an armor on the LDH layer to further prevent the corrosive ions from infiltrating the microporous defects. In addition, the as-prepared SZPL double-layered coating showed robust superhydrophobic and self-cleaning properties, which could block the electrolyte invasion. Furthermore, the electrochemical tests demonstrated that…

Clean water resources are essential to our human society. Oil leakage has caused water contamination, which leads to serious shortage of clean water, environmental deterioration, and even increasing number of deaths. It is of great urgency to solve the oil-polluted water problems worldwide. Efficient oil/water separation, especially emulsified oil/water mixture separation, is widely used to mitigate water pollution issues. Recently, advanced materials with special wettability have been employed for oily wastewater remediation. Moreover, by endowing them with various intelligent functions, smart materials can effectively separate complex oil/water mixtures including extremely stable emulsions. In this review, oil/water separation mechanisms and various fabrication methods of special wettability separation materials are summarized. We highlight the special wettable materials with intelligent functions, including photocatalytic, self-healing, and switchable oil/water separation materials, which can achieve self-cleaning, self-healing, and efficient oily wastewater treatment. In each…

Stable photocatalysts with excellent optical adsorption and low reaction barrier are the key for the water splitting. Here, we find that a two-dimensional Janus WSSe monolayer possesses the compelling photocatalytic properties from density functional theory simulations, which can be well modulated with strain deformation. Comprehensive investigations indicate that the Janus material not only exhibits strong optical absorbance in the visible spectrum, suitable band edge potentials, high carrier separation, and transfer efficiency but also has adequate driving forces of photoexcited carrier for water redox reaction and good resistance against photoinduced corrosion. Janus WSSe is therefore predicted to be a promising photocatalyst for water splitting. Moreover, we also find that tensile strains could further improve the photocatalytic performance for water splitting by effectively increasing the energy conversion efficiency and reducing the exciton binding energy. Our results not only predict a photocatalyst, which can utilize the visible light for overall water splitting, but also…

As one of the most promising drug delivery carriers, hydrogels have received considerable attention in recent years. Many previous efforts have focused on diffusion-controlled release, which allows hydrogels to load and release drugs in vitro and/or in vivo. However, it hardly applies to lipophilic drug delivery due to their poor compatibility with hydrogels. Herein, we propose a novel method for lipophilic drug release based on a dual pH-responsive hydrogel actuator. Specifically, the drug is encapsulated and can be released by a dual pH-controlled capsule switch. Inspired by the deformation mechanism of Drosera leaves, we fabricate the capsule switch with a double-layer structure that is made of two kinds of pH-responsive hydrogels. Two layers are covalently bonded together through silane coupling agents. They can bend collaboratively in a basic or acidic environment to achieve the "turn on" motion of the capsule switch. By incorporating an array of parallel elastomer stripes on one side of the hydrogel bilayer, various motions (e.g., bending, twisting, and rolling) of the…

Taking serious microwave pollution issues and the complex application environment into consideration, it is quite urgent to integrate several functions into one material. Electromagnetic (EM) absorbing materials with multiple functions are highly attractive to next-generation wireless techniques and portable electronic devices. Herein, melamine foam provides a decent platform for the uniform growth of Co-based metal-organic frameworks (MOFs), which bring the as-obtained hybrid foam with three-dimensional porous network structure and combination of dielectric along with magnetic attenuation abilities as advanced materials in multifunctional fields. Remarkably, the relevant microwave absorption (MA) performance of the hybrid foam can reach an extremely high reflection loss value of -59.82 dB. Furthermore, the hybrid foam exhibits excellent infrared stealth and optimiztic heat insulation function, demonstrating the potential in plenty of practical applications. These results may arouse interests and inspirations of the elaborately design and facilely synthesis of high-performance…

Conductive hydrogels have attracted intensive attention for versatile functions in flexible electronics because of their unique combination of mechanical flexibility and conductivity. However, hydrogels containing plenty of water inevitably freeze at subzero temperature, leading to invalid electronics with failed mechanical advantages and negligible conductivity. Moreover, the inferior elasticity and fatigue resistance of hydrogels result in unstable sensing performance and poor reusability of hydrogel-based electronics. Herein, a freezing-tolerant, high-sensitive, durable strain and pressure sensor was constructed from an ionic conductive chitosan–poly(acrylamide- co -acrylic acid) double-network [CS–P(AM- co -AA) DN] hydrogel with dual-dynamic cross-links (chitosan physical network and ionic coordination [CO 2 LFe III ]), which was feasibly fabricated by soaking the CS–P(AM- co -AA) composite hydrogel in FeCl 3 solution. The ions immobilized in dynamic cross-links exerted crucial effects on improving mechanics [prominent tensile performance, supercompressibility, extraordinary…

Creatively constructing Z-scheme composites is a promising and common strategy for designing effective photocatalyst systems. Herein, we synthesized Z-scheme Fe 2 O 3 @Ag–ZnO@C heterostructures from the Fe-MOFs and applied it to photodegradation of tetracycline and methylene blue pollutants in wastewater. The optimized sample exhibits a remarkable performance as well as stability under visible light irradiation. The calculating and experimental results demonstrate that the Fe 2 O 3 @ZnO nanointerface and carbon sheath together boost the transfer efficiency of photogenerated carriers and absorption ability, thereby improving the photocatalytic activity. Furthermore, detailed mechanism investigation reveals the pivotal role of reactive oxygen species ( • OH and • O 2 – ) generated, resulting in remarkable performance. In addition, cell biology experiments reveal that the wastewater after photocatalytic treatment has good biological compatibility, which is important for applications. This work provides valuable information for constructing high-performance Z-scheme photocatalysts from…

As a promising microwave absorber filler, molybdenum disulfide (MoS 2 ), because of the unique structure, high electrical conductivity, and polarization effect, is receiving more and more interest. Developing MoS 2 -based composites with specific structure and morphology is a hot top in the field of microwave absorbers, because of its strong multiple scattering and reflecting for microwaves as well as its unique interfacial characteristics. Now, with a facile solvothermal method, a novel core–shell CoFe 2 O 4 @1T/2H-MoS 2 composite is synthesized, where the CoFe 2 O 4 nanospheres are entirely embedded in a special three-dimensional (3D) nest-like 1T/2H phase MoS 2 . Notably, in comparison with superparamagnetic CoFe 2 O 4 nanospheres, the coercivities of as-synthesized CoFe 2 O 4 @1T/2H-MoS 2 composites greatly increase. Here, 1T/2H-MoS 2 exhibits ferromagnetism superimposed onto large diamagnetism. It is noted that, by adjusting the content of 1T/2H-phase MoS 2, the microwave absorption performance of as-synthesized composites can be effectively tuned. The combination of 1T/2H-MoS…

Although extensive studies have been done on lead-free dielectric ceramics to achieve excellent dielectric behaviors and good energy storage performance, the major problem of low energy density has not been solved so far. Here, we report on designing the crossover relaxor ferroelectrics (CRFE), a crossover region between the normal ferroelectrics and relaxor ferroelectrics, as a solution to overcome the low energy density. CRFE exhibits smaller free energy and lower defect density in the modified Landau theory, which helps to obtain ultrahigh energy density and efficiency. The (1– x )Ba 0.65 Sr 0.35 TiO 3 – x Bi(Mg 2/3 Nb 1/3 )O 3 ((1– x )BST– x BMN) ( x = 0, 0.08, 0.1, 0.18, 0.2) ceramic was synthesized by a solid-state reaction method. The solid solutions exhibit dielectric frequency dispersion, which suggests typical relaxor characteristics with the increasing BMN content. The crossover ferroelectrics of 0.9BST–0.1BMN ceramic possesses a high energy storage efficiency (η) of 85.71%, a high energy storage density ( W ) of 3.90 J/cm 3, and an ultrahigh recoverable energy storage…

Abstract Piezoelectric polymers are promising energy materials for wearable and implantable applications for replacing bulky batteries in small and flexible electronics. Therefore, many research studies are focused on understanding the behavior of polymers at a molecular level and designing new polymer-based generators using polyvinylidene fluoride (PVDF). In this work, we investigated the influence of voltage polarity and ambient relative humidity in electrospinning of PVDF for energy-harvesting applications. A multitechnique approach combining microscopy and spectroscopy was used to study the content of the β-phase and piezoelectric properties of PVDF fibers. We shed new light on β-phase crystallization in electrospun PVDF and showed the enhanced piezoelectric response of the PVDF fiber-based generator produced with the negative voltage polarity at a relative humidity of 60%. Above all, we proved that not only crystallinity but also surface chemistry is crucial for improving piezoelectric performance in PVDF fibers. Controlling relative humidity and voltage polarity increased the…

When external pressure drives an electrolyte solution in a capillary tube with a charged inner surface, we obtain a streaming potential/current. This effect is also manifested when water flows through the microchannels of a tree, which is driven by capillary pressure and natural evaporation. Thus, by making use of natural evaporation, we took advantage of the anisotropic three-dimensional wood structures to fabricate nanogenerators drawing electricity from the streaming potential/current. As a result, direct current can be harvested continuously, simply through a piece of wood. A 300 mV open-circuit voltage and a 10 μA short-circuit current ( I SC ) were recorded from a single device, which surpassed the I SC values of most previous works by an order. By connecting five wood nanogenerators in series, a calculator can be completely functional, as a demonstration for practical application.

Organophoshorus nerve agents are among the most toxic chemicals known to humans, and because of their unfortunate recent use despite international bans, there is an urgent need to develop materials that can effectively degrade these nerve agents. Within the past decade, zirconium-based metal-organic frameworks (Zr-MOFs) have emerged as a bioinspired class of materials capable of rapidly hydrolyzing these compounds and significantly diminishing their toxicity. Both experimental and computational insights have guided the design of Zr-MOFs, leading to the development of catalysts capable of detoxifying nerve agents and simulants, chemicals with similar functionality but lower toxicity, via hydrolysis within seconds in basic aqueous solutions. While these systems are acceptable for the elimination of stockpile weapons, translating this catalytic performance to filters incorporating Zr-MOFs that can be used in masks or protective clothing is not trivial. As such, a large area of focus recently has been targeted toward integrating these hydrolysis catalysts into protective clothing and…

Here, we reported that sulfur vacancy-rich O-doped 1T-MoS 2 nanosheets (denoted as SV-1T-MoS 2 ) can surpass the activity of Pt as cocatalysts to assist in the photocatalytic nitrogen fixation of CdS nanorods. SV-1T-MoS 2 cocatalysts exhibit sulfur vacancies, O-doping, more metallic 1T phase, and high electronic conductivity, thus leading to the exposure of more active edge sites, high Brunauer–Emmett–Teller surface area, enhanced visible light absorption, and improved electron separation and transfer, which are beneficial for photocatalytic nitrogen fixation. Consequently, the optimized 30 wt % SV-1T-MoS 2 -/CdS composites exhibit an outstanding nitrogen fixation rate of 8220.83 μmol L –1 h –1 g –1 and long-term stability under simulated solar light irradiation, significantly higher than pure CdS nanorods, CdS–Pt (0.1 wt %), and 30 wt % 1T-MoS 2 /CdS composites. The catalytic mechanism of photocatalytic nitrogen fixation on SV-1T-MoS 2 is discussed by density functional theory calculations.

Flexible strain sensors have been widely used in wearable electronic devices for body physical parameter capturing. However, regardless of the stretchability of the sensing material, the resolution of small strain changes or the hysteresis between loading/unloading states has always limited the various applications of these sensors. In this paper, a microfluidic flexible strain sensor was achieved by introducing liquid metal eutectic gallium indium (EGaIn) embedded into a wave-shaped microchannel elastomeric matrix (300 μm width × 70 μm height). The microfluidic sensor can withstand a strain of up to 320%, and the hysteresis performance was also improved from 6.79 to 1.02% by the wave-patterned structure which can restrain the viscoelasticity of the elastomer effectively. Moreover, an enhanced wave-shaped strain sensor was fabricated by increasing the length of the microfluidic channel; it has high sensitivity (GF = 4.91) and resolution, and even as low as 0.09% strain change could be detected, which is capable of resolving microdeformation; besides, the enhanced wave-shaped strain…

The development of natural polymer-based hydrogels, combining outstanding injectability, self-healing, and tissue adhesion, with mechanical performance, able to facilitate full-thickness skin wound healing, remains challenging. We have developed an injectable micellar hydrogel (AF127/HA-ADH/OHA-Dop) with outstanding adhesive and self-healing properties able to accelerate full-thickness skin wound healing. Dopamine-functionalized oxidized hyaluronic acid (OHA-Dop), adipic acid dihydrazide-modified HA (HA-ADH), and aldehyde-terminated Pluronic F127 (AF127) were employed as polymer backbones. They were cross-linked in situ using Schiff base dynamic covalent bonds (AF127 micelle/HA-ADH network and HA-ADH/OHA-Dop network), hydrogen bonding, and π–π stacking interactions. The resulting multicross-linked double-network design forms a micellar hydrogel. The unique multicross-linked double-network structure endows the hydrogel with both improved injection abilities and mechanical performance while self-healing faster than single-network hydrogels. Inspired by mussel foot adhesive protein,…

Instrument-free, portable, and direct read-out mini-devices have wider application prospects in various fields, especially for real-time/on-site sensing. Herein, combined with a paper strip, a smartphone sensing platform integrated with a UV lamp and dark cavity by 3D-printing technology has been developed for the rapid, sensitive, instrument-free, and visual quantitative analysis in real-time/on-site conditions. The platform proved the feasibility for visual quantitative detection of pesticide via a fluorescence “on–off–on” response with a single dual-emissive ratiometric paper strip. Red-emitting CdTe quantum dots (rQDs) were embedded into the silica nanoparticles (SiO 2 NPs) as an internal reference, while blue-emitting carbon dots (bCDs) as a signal report unit were covalently linked to the outer surface of SiO 2 NPs. The blue fluorescence could be quenched by gold nanoparticles (Au NPs) and then recovered with pesticide. The red (R), green (G), and blue (B) channel values of the generated images were determined by a color recognizer application (APP) installed in the…

Photocatalytic CO 2 reduction is an appealing approach to convert solar energy into high value-added chemicals. All-inorganic CsPbBr 3 quantum dots (QDs) have emerged as a promising photocatalyst for reducing CO 2 . However, pristine CsPbBr 3 has a low catalytic performance, mainly due to severe charge recombination. Herein, a 0D/2D heterojunction of CsPbBr 3 QDs/Bi 2 WO 6 nanosheet (CPB/BWO) photocatalysts is fabricated for photocatalytic CO 2 reduction. The CPB/BWO photocatalyst achieves excellent photocatalytic performance: the total yield of CH 4 /CO is 503 μmol g –1, nearly 9.5 times higher than the pristine CsPbBr 3 . The CPB/BWO heterojunction also exhibits much-improved stability during photocatalytic reactions. On the basis of various characterization techniques, our investigations verified a direct Z-scheme charge migration mechanism between CsPbBr 3 QDs and Bi 2 WO 6 nanosheets. The improved photocatalytic performance is originated from the high spatial separation of photoexcited charge carriers in CPB/BWO, which can also preserve strong individual redox abilities of two…

Abstract In the present work, Janus monolayers WSSe and WSTe are investigated by combining first-principles calculations and semiclassical Boltzmann transport theory. Janus WSSe and WSTe monolayers show a direct band gap of 1.72 and 1.84 eV at K-points, respectively. These layered materials have an extraordinary Seebeck coefficient and electrical conductivity. This combination of high Seebeck coefficient and high electrical conductivity leads to a significantly large power factor. In addition, the lattice thermal conductivity in the Janus monolayer is found to be relatively very low as compared to the WS2 monolayer. This leads to a high figure of merit (ZT) value of 2.56 at higher temperatures for the Janus WSTe monolayer. We propose that the Janus WSTe monolayer could be used as a potential thermoelectric material due to its high thermoelectric performance. The result suggests that the Janus monolayer is a better candidate for excellent thermoelectric conversion.

The construction of an efficient oxygen reduction reaction and oxygen evolution reaction (ORR/OER) bifunctional electrocatalyst is of great significance but still remains a giant challenge for high-performance metal–air batteries. In this study, uniform FeS/Fe 3 C nanoparticles embedded in a porous N,S-dual doped carbon honeycomb-like composite ( abbr. FeS/Fe 3 [email protected] ) have been conveniently fabricated by pyrolysis of a single-crystal Fe-MOF, which has a low potential gap Δ E of ca. 0.72 V, a competitive power density of 90.9 mW/cm 2, a specific capacity as high as 750 mAh/g Zn, and excellent cycling stabilities over 865 h (1730 cycles) at 2 mA/cm 2 when applied as a cathode material for rechargeable zinc–air batteries. In addition, the two series-linked Zn–air batteries successfully powered a 2.4 V LED light as a real power source. The efficient ORR/OER bifunctional electrocatalytic activity and long-term durability of the obtained composite might be attributed to the characteristic honeycomb-like porous structure with sufficient accessible active sites, the synergistic…

In the pursuit for future mobility, solid-state batteries open a wide field of promising battery concepts with a variety of advantages, ranging from energy density to power capability. However, trade-offs need to be addressed, especially for large-scale, cost-effective processing, which implies the use of a polymeric binder in the composite electrodes. Here, we investigate three-dimensional microstructure models of the active material, solid electrolyte, and binder to link cathode design and binder content with electrode performance. Focusing on lithium-ion transport, we evaluate the effective ionic conductivity and tortuosity in a flux-based simulation. Therein, we address the influence of electrode composition and active material particle size as well as the process-controlled design parameters of the void space and binder content. Even though added in small amounts, the latter has a strong negative influence on the ion transport paths and the active surface area. The simulation of ion transport within four-phase composites is supplemented by an estimation of the limiting current…

In 2011, with the successful isolation of Ti 3 C 2, a door of 2D layered MXene has been opened and received growing attention from researchers. MXene refers to a family of two-dimensional (2D) materials made up of atomic layers of the transition metal, carbide, nitrides, or carbonitrides. Given the large surface area, adjustable surface terminal groups, and excellent conductivity of MXene, it has shown exciting potential in photocatalysis, energy conversion, and many other fields. Among many 2D MXene, Ti 3 C 2 was the most studied for its availability, low cost, facile modification procedure, and outstanding electronic properties. In previous investigations, Ti 3 C 2 has shown huge potential in the photocatalysis area. Ti 3 C 2 in a photocatalysis system can enhance the separation of photoinduced electrons and holes, reduce charge recombination, and thus improve the photocatalysis performance in many systems. To adjust the performance of Ti 3 C 2 in different applications, the properties of Ti 3 C 2 including morphology, structures, and stability are tunable by different…

Poly(vinylidene fluoride) (PVDF)-based piezoelectric materials are promising candidates for sensors, transducers, and actuators, due to several distinctive characteristics such as good flexibility, easy processability, and high mechanical resistance. In the present work, PVDF-based nanocomposites loaded with BaTiO 3 nanoparticles (NPs) of various weight fractions were prepared by the electrospinning technique and used for the fabrication of a flexible piezoelectric pressure tactile sensor (PPTS). The addition (5, 10, and 20 wt %) of piezoelectric BaTiO 3 NPs improves the piezoelectric performance, especially the β phase crystals of PVDF/BaTiO 3 (10 wt %) nanocomposites that can reach 91.0%. In addition, the mechanical strength of PVDF/BaTiO 3 nanocomposites is up to 26.7 MPa, which is an increase of 66% compared to neat PVDF. It should be emphasized that the elongation at break continuously increases from 71% to 153% with increasing BaTiO 3 NPs. More importantly, the PPTS (piezoelectric pressure tactile sensor) with the combination of electrospun PVDF/BaTiO 3 nanocomposite membranes…

Wastewater pollution has always been one of the most severe worldwide environmental problems. In addition, in light of the frequent oil spills that have occurred in recent years, the treatment of oily wastewater is particularly important. In this work, a novel zeolitic imidazolate framework-8@thiolated graphene (ZIF-8@GSH) composites-based polyimide (PI) nanofibrous membrane was developed via a facile electrospinning and in situ hydrothermal synthesis approaches for effective purification of oily wastewater. The membrane showed superhydrophobicity/superoleophilicity and high separation efficiency (>99.9%) for a wide range of oil/water mixtures and water-in-oil emulsions. Besides, the membrane demonstrated excellent photocatalytic dye degradation, antibacterial, self-cleaning, and mechanochemical durable abilities, showing high potential in oily wastewater treatment and water remediation.

The application of conductive hydrogels in intelligent biomimetic electronics is a hot topic in recent years, but it is still a great challenge to develop the conductive hydrogels through a rapid fabrication process at ambient temperature. In this work, a versatile poly(acrylamide) @cellulose nanocrystal/tannic acid–silver nanocomposite (NC) hydrogel integrated with excellent stretchability, repeatable self-adhesion, high strain sensitivity, and antibacterial property, was synthesized via radical polymerization within 30 s at ambient temperature. Notably, this rapid polymerization was realized through a tannic acid–silver (TA-Ag) mediated dynamic catalysis system that was capable of activating ammonium persulfate and then initiated the free-radical polymerization of the acrylamide monomer. Benefiting from the incorporation of TA-Ag metal ion nanocomplexes and cellulose nanocrystals, which acted as dynamic connecting bridges by hydrogen bonds to efficiently dissipate energy, the obtained NC hydrogels exhibited prominent tensile strain (up to 4000%), flexibility, self-recovery, and…

Designing bone adhesives with adhesiveness, antideformation, biocompatibility, and biofunctional effects has great practical significance for bone defect reconstructive treatment, especially for bone graft repair surgery. Here, we designed zeolitic imidazolate framework-8 nanoparticle (ZIF-8 NP)-modified catechol-chitosan (CA-CS) multifunctional hydrogels (CA-CS/Z) to stabilize the bone graft environment, ensure blood supply, promote osteogenic differentiation, and accelerate bone reconstruction. Characterizations confirmed the successful synthesis of CA-CS/Z hydrogels. Hydrogels exhibited advanced rheological properties, reliable mechanical strength, and excellent adhesion for clinical applications. Based on excellent biocompatibility, it could enhance paracrine of the vascular endothelial growth factor (VEGF) in rat bone marrow mesenchymal stem cells (rBMSCs) to ensure blood supply reconstruction in bone defect areas. Furthermore, the ZIF-8 NPs released from the hydrogels could also up-regulate the production and secretion of alkaline phosphatase, collagen 1, and osteocalcin,…

Abstract With the undergoing unprecedented development of lithium-ion batteries (LIBs), the recycling of end-of-life batteries has become an urgent task considering the demand for critical materials, environmental pollution, and ecological impacts. Selective recovery of targeted element(s) is becoming a topical field that enables metal recycling in a short path with highly improved material efficiencies. This research demonstrates a process of selective recovery of spent Ni–Co–Mn (NCM)-based lithium-ion battery by systematically understanding the conversion mechanisms and controlling the sulfur behavior during a modified-sulfation roasting. As a result, Li from complex cathode components can be selectively extracted with high efficiency by only using water. Notably, the sulfur driven recovery processes can be divided into two stages: (i) part of the structure of NCM523 was destroyed, and Ni, Co, and Mn were reduced to divalent in different degrees to form sulfate (NiSO4, CoSO4, MnSO4) when reacting with H2SO4 at ambient temperature; (ii) with increasing temperature, Li ions in the…

Abstract The main challenges of a solar steam generation device based on biomass materials are complicated processing techniques and relatively low efficiency. To solve these problems, we reported a simple immersion treatment method by depositing polydopamine (PDA) and silver nanoparticles (AgNPs) on natural wood to prepare a novel solar interface evaporation device. Ag-PDA@wood exhibits a unique bilayer structure. The absorbance of the top light absorption layer is higher than 96% in a wide wavelength range (300–2500 nm). Owing to the synergistic photothermal effect between PDA and AgNPs, Ag-PDA@wood has ultrafast solar–thermal response (a temperature increase of 42.5 °C within 5 min under 1 sun), and more heat is located at the steam generation interface (the surface temperature is 45.1 °C). The natural wood layer at the bottom with low thermal conductivity provides sufficient water supply and reduces the bulk heat loss. A high evaporation rate of 1.58 kg m–2 h–1 is achieved using Ag-PDA@wood under 1 sun (1 kW m–2). Its evaporation efficiency reaches 88.6%. The results upon sewage…

A stretchable electronic skin (e-skin) requires a durable elastomeric matrix to serve in various conditions. Therefore, excellent and balanced properties such as elasticity, water proof capability, toughness, and self-healing are demanded. However, it is very difficult and often contradictory to optimize them at one time. Here, a polyurethane (BS-PU-3) containing a polydisperse hard segment, hydrophobic soft segment, and a dynamic disulfide bond was prepared by one-pot synthesis. Unlike the normal two-pot reaction, BS-PU-3 obtained through the one-pot method owned a higher density of self-healing points along the main chain and a faster self-healing speed, which reached 1.11 μm/min in a cut-through sample and recovered more than 93% of virgin mechanical properties in 6 h at room temperature. Moreover, a remarkable toughness of 27.5 MJ/m 3 assures its durability as an e-skin matrix. Even with a 1 mm notch (half of the total width) on a standard dumbbell specimen, it could still bear the tensile strain up to 324% without any crack propagation. With polybutadiene as the soft segment,…

With an ever increasing scientific, technological, and industrial interest in high surface area, porous nanofiber mats, electrospinning has emerged as a popular method to produce fibrous assemblies for use across biomedical, energy, and environmental applications. However, not all precursor solutions nor complex geometries can be easily fabricated using the traditional single-nozzle apparatus. Therefore, coaxial electrospinning, a modified version of electrospinning that features a concentrically aligned dual nozzle, has been developed. This review will first describe the mechanism of electrospinning two precursor solutions simultaneously and the operational parameters that need to be optimized to fabricate continuous fibers. Modifications that can be made to the coaxial electrospinning process, which enable the fabrication of uniform fibers with improved properties, as well as the fabrication of fibers that are hollow, functionalized, and from "nonspinnable precursors" will be discussed as a means of promoting the advantages of using a coaxial setup. Examples of how coaxially…

Artificial visual system with information sensing, processing, and memory function is promoting the development of artificial intelligence techniques. Photonic synapse as an essential component can enhance the visual information processing efficiency owing to the high propagation speed, low latency, and large bandwidth. Herein, photonic synaptic transistors based on organic semiconductor poly[2,5-(2-octyldodecyl)-3,6-diketopyrrolopyrrole-alt-5,5-(2,5-di(thien-2-yl)thieno [3,2-b]thiophene)] (DPPDTT) and perovskite CsPbBr 3 quantum dots are fabricated by a simple solution process. The device can simulate fundamental synaptic behaviors, including excitatory postsynaptic current, pair-pulse facilitation, the transition of short-term memory to long-term memory, and “learning experience” behavior. Combining the advantages of the high photosensitivity of perovskites and relatively high conductivity of DPPDTT, the device can exhibit excellent synaptic performances at a low voltage of −0.2 V. Even under an ultralow operation voltage of −0.0005 V, the device can still show obvious synaptic…

The wide bandgap, high-breakdown electric field, and high carrier mobility makes GaN an ideal material for high-power and high-frequency electronics applications, such as wireless communication and radar systems. However, the performance and reliability of GaN-based high-electron-mobility transistors (HEMTs) are limited by the high channel temperature induced by Joule heating in the device channel. Integration of GaN with high thermal conductivity substrates can improve the heat extraction from GaN-based HEMTs and lower the operating temperature of the device. However, heterogeneous integration of GaN with diamond substrates presents technical challenges to maximize the heat dissipation potential brought by the ultrahigh thermal conductivity of diamond substrates. In this work, two modified room-temperature surface-activated bonding (SAB) techniques are used to bond GaN and single-crystal diamond. Time-domain thermoreflectance (TDTR) is used to measure the thermal properties from room temperature to 480 K. A relatively large thermal boundary conductance (TBC) of the GaN/diamond…

Abstract Polarization-sensitive photodetectors are highly desirable for high-performance optical signal capture and stray light shielding in order to enhance the capability for detection and identification of targets in dark, haze, and other complex environments. Usually, filters and polarizers are utilized for conventional devices to achieve polarization-sensitive detection. Herein, to simplify the optical system, a two-dimensional self-powered polarization-sensitive photodetector is fabricated based on a stacked GeSe/MoS2 van der Waals (vdW) heterojunction which facilitates efficient separation and transportation of the photogenerated carriers because of type-II band alignment. Accordingly, a high-performance self-powered photodetector is achieved with merits of a very large on–off ratio photocurrent at zero bias of currently 104 and a high responsivity (Rλ) of 105 mA/W with an external quantum efficiency of 24.2%. Furthermore, a broad spectral photoresponse is extended from 380 to 1064 nm owing to the high absorption coefficient in a wide spectral region. One of the key benefits…

Functional polymeric micro-/nanofibers have emerged as promising materials for the construction of structures potentially useful in biomedical fields. Among all kinds of technologies to produce polymer fibers, spinning methods have gained considerable attention. Herein, we provide a recent review on advances in the design of micro- and nanofibrous platforms via spinning techniques for biomedical applications. Specifically, we emphasize electrospinning, solution blow spinning, centrifugal spinning, and microfluidic spinning approaches. We first introduce the fundamentals of these spinning methods and then highlight the potential biomedical applications of such micro- and nanostructured fibers for drug delivery, tissue engineering, regenerative medicine, disease modeling, and sensing/biosensing. Finally, we outline the current challenges and future perspectives of spinning techniques for the practical applications of polymer fibers in the biomedical field.

Laser-induced graphene (LIG) is a multifunctional graphene foam that is commonly direct-written with an infrared laser into a carbon-based precursor material. Here, a visible 405 nm laser is used to directly convert polyimide into LIG. This enabled the formation of LIG with a spatial resolution of ∼12 μm and a thickness of <5 μm. The spatial resolution enabled by the relatively smaller focused spot size of the 405 nm laser represents a >60% reduction in LIG feature sizes reported in prior publications. This process occurs in situ in an SEM chamber, thus allowing direct observation of LIG formation. The reduced size of the LIG features enables the direct-write formation of flexible electronics that are not visible to the unaided eye. A humidity sensor is demonstrated which could detect human breath with a response time of 250 ms. With the growing interest in LIG for flexible electronics and sensors, finer features can greatly expand its utility.

Microwave dielectric ceramics are vital for filters, dielectric resonators, and dielectric antennas in the 5G era. It was found that the (Cu 1/3 Nb 2/3 ) 4+ substitution can effectively adjust the TCF (temperature coefficient of resonant frequency) of Li 2 TiO 3 and simultaneously increase its Q × f ( Q and f denote the quality factor and the resonant frequency, respectively) value. Notably, excellent microwave dielectric properties (ε r (permittivity) ≈ 18.3, Q × f ≈ 77,840 GHz, and TCF ≈ +9.8 ppm/°C) were achieved in the Li 2 Ti 0.8 (Cu 1/3 Nb 2/3 ) 0.2 O 3 (LTCN 0.2 ) ceramic sintered at 1140 °C. Additionally, the sintering temperature of LTCN 0.2 was reduced to 860 °C by the addition of 3 wt % H 3 BO 3, exhibiting superior microwave dielectric properties ( ε r ≈ 21.0, Q × f ≈ 51,940 GHz, and TCF ≈ 1.4 ppm/°C) and being chemically compatible with silver. Moreover, LTCN 0.2 + 3 wt % H 3 BO 3 ceramics were designed as a patch antenna and a dielectric resonator antenna, both of which showed high simulated radiation efficiencies (88.4 and 93%) and gains (4.1 and 4.03 dBi) at the…

Wound bleeding and infection are two of the major threats to patients’ lives, but developing safe materials with high hemostasis efficiency and antibacterial activity remains a major challenge. Silver nanoparticles (AgNPs) are suitable as antibacterial agents in the hemostatic process, but the application is hampered because of easy accumulation of toxicity. Herein, thiol-modified chitosan (TMC) was prepared by modifying with mercaptosuccinic acid and then was used to immobilize AgNPs to obtain composite sponges (TMC/AgNPs) for stemming the bleeding and preventing infection. TMC/AgNPs sponges had complex interlaced tubular porous structure with high porosity (99.42%), indicating high absorption. TMC had high immobilization efficiency for AgNPs—the release rate of AgNPs was 14.35% after 14 days—but the TMC/AgNPs sponge still had excellent antibacterial activity against Staphylococcus aureus, Escherichia coli, and Pseudomonas aeruginosa . In vitro and in vivo experiments confirm that the TMC/AgNPs sponge had fast and efficient hemostatic performance in comparison with the PVF sponge,…

Hydrogels are important for stretchable and wearable multifunctional sensors, but their application is limited by their low mechanical strength and poor long-term stability. Herein, a conductive organohydrogel with a 3D honeycomb structure was prepared by integrating carbon nanotubes (CNTs) and carbon black (CB) into a poly(vinyl alcohol)/glycerol (PVA/Gly) organohydrogel. Such a nanocomposite organohydrogel is built on a physical cross-linking network formed by the hydrogen bonds among PVA, glycerol, and water. CNTs and CB had an add-in synergistic impact on the mechanical and electrical performances of the PVA/Gly organohydrogel because of the distinct aspect ratios and geometric shapes. The prepared organohydrogel integrated with a tensile strength of 4.8 MPa, a toughness of 15.93 MJ m –3, and flexibility with an elongation at break up to 640%. The organohydrogels also showed good antifreezing feature, long-term moisture retention, self-healing, and thermoplasticity. Sensors designed from these organohydrogels displayed high stretching sensitivity to tensile strain and…

Abstract Lanthanide-based luminescent nanothermometers play a crucial role in optical temperature determination. However, because of the strong thermal quenching of the luminescence, as well as the deterioration of their sensitivity and resolution with temperature elevation, they can operate in a relatively low-temperature range, usually from cryogenic to ≈800 K. In this work, we show how to overcome these limitations and monitor very high-temperature values, with high sensitivity (≈2.1% K–1) and good thermal resolution (≈1.4 K) at around 1000 K. As an optical probe of temperature, we chose upconverting Yb3+–Tm3+ codoped YVO4 nanoparticles. For ratiometric sensing in the low-temperature range, we used the relative intensities of the Tm3+ emissions associated with the 3F2,3 and 3H4 thermally coupled levels, that is, 3F2,3 → 3H6/3H4 → 3H6 (700/800 nm) band intensity ratio. In order to improve sensitivity and resolution in the high-temperature range, we used the 940/800 nm band intensity ratio of the nonthermally coupled levels of Yb3+ (2F5/2 → 2F7/2) and Tm3+ (3H4 → 3H6). These NIR…

Abstract The utilization of nonprecious metal electrocatalysts for water-splitting may be the ultimate solution for sustainable and clean hydrogen energy. MXene, an emerging two-dimensional material, exhibits many unique properties such as possible metal-like conductivity, hydrophilic surface, and rich chemistry, rendering a group of promising catalysts and catalyst support materials. In this study, exfoliated Ti3C2 MXenes serve as a substrate to perpendicularly grow uniform mesoporous NiCoP nanosheets through an in situ interface-growth strategy and subsequent phosphorization. The obtained Ti3C2@mNiCoP materials with a stable hierarchical sandwich structure possess excellent conductivity, large surface area, and uniform mesopores with high pore volume. With these beneficial properties, the Ti3C2@mNiCoP material exhibits superior overall water-splitting performance compared with that of its building-block counterparts, matching the state-of-the-art water-splitting electrocatalysts.

Regenerative medicine leverages the innate potential of the human body to efficiently repair and regenerate damaged tissues using engineered biomaterials. By designing responsive biomaterials with the appropriate biophysical and biochemical characteristics, cellular response can be modulated to direct tissue healing. Recently, inorganic biomaterials have been shown to regulate cellular responses including cell-cell and cell-matrix interactions. Moreover, ions released from these mineral-based biomaterials play a vital role in defining cell identity, as well as driving tissue-specific functions. The intrinsic properties of inorganic biomaterials, such as the release of bioactive ions (e.g., Ca, Mg, Sr, Si, B, Fe, Cu, Zn, Cr, Co, Mo, Mn, Au, Ag, V, Eu, and La), can be leveraged to induce phenotypic changes in cells or modulate the immune microenvironment to direct tissue healing and regeneration. Biophysical characteristics of biomaterials, such as topography, charge, size, electrostatic interactions, and stiffness can be modulated by addition of inorganic micro- and nanoparticles to…

The therapeutic effect of traditional chemodynamic therapy (CDT) agents is severely restricted by their weakly acidic pH and glutathione (GSH) overexpression in the tumor microenvironment. Here, fusiform-like copper(II)-based tetrakis(4-carboxy phenyl)porphyrin (TCPP) nanoscale metal–organic frameworks (nMOFs) were designed and constructed for the first time (named PCN-224(Cu)-GOD@MnO 2 ). The coated MnO 2 layer can not only avoid conjugation of glucose oxidase (GOD) to damage normal cells but also catalyzes the generation of O 2 from H 2 O 2 to enhance the oxidation of glucose (Glu) by GOD, which also provides abundant H 2 O 2 for the subsequent Cu + -based Fenton-like reaction. Meanwhile, the Cu 2+ chelated to the TCPP ligand is converted to Cu + by the excess GSH in the tumor, which reduces the tumor antioxidant activity to improve the CDT effect. Next, the Cu + reacts with the plentiful H 2 O 2 by enzyme catalysis to produce a toxic hydroxyl radical ( • OH), and singlet oxygen ( 1 O 2 ) is synchronously generated from combination with Cu +, O 2, and H 2 O via the Russell…

Recent studies show that biomaterials are capable of regulating immune responses to induce a favorable osteogenic microenvironment and promote osteogenesis and angiogenesis. In this study, we investigated the effects of zinc silicate/nanohydroxyapatite/collagen (ZS/HA/Col) scaffolds on bone regeneration and angiogenesis and explored the related mechanism. We demonstrate that 10ZS/HA/Col scaffolds significantly enhanced bone regeneration and angiogenesis in vivo compared with HA/Col scaffolds. ZS/HA/Col scaffolds increased tartrate-resistant acid phosphatase (TRAP)-positive cells, nestin-positive bone marrow stromal cells (BMSCs) and CD31-positive neovessels, and expression of osteogenesis ( Bmp- 2 and Osterix ) and angiogenesis-related ( Vegf-α and Cd31 ) genes increased in nascent bone. ZS/HA/Col scaffolds with 10 wt % ZS activated the p38 signaling pathway in monocytes. The monocytes subsequently differentiated into TRAP + cells and expressed higher levels of the cytokines SDF-1, TGF-β1, VEGF-α, and PDGF-BB, which recruited BMSCs and endothelial cells (ECs) to the defect areas.…

Stimulus-responsive hydrogels, such as conductive hydrogels and thermoresponsive hydrogels, have been explored extensively and are considered promising candidates for smart materials such as wearable devices and artificial muscles. However, most of the existing studies on stimulus-responsive hydrogels have mainly focused on their single stimulus-responsive property and have not explored multistimulus-responsive or multifunction properties. Although some works involved multifunctionality, the prepared hydrogels were incompatible. In this work, a multistimulus-responsive and multifunctional hydrogel system (carboxymethyl cellulose/poly acrylic-acrylamide) with good elasticity, superior flexibility, and stable conductivity was prepared. The prepared hydrogel not only showed excellent human motion detection and physiological signal response but also possessed the ability to respond to environmental temperature changes. By integrating a conductive hydrogel with a thermoresponsive poly( N -isopropylacrylamide) (PNIPAM) hydrogel to form a bilayer hydrogel, the prepared bilayer also…

The burgeoning development of wearable electronic devices has resulted in urgent demands for electromagnetic interference (EMI) shielding films that feature excellent fireproof and heat dissipation capability. Herein, multifunctional fireproof EMI shielding films with excellent anisotropic thermal conductivity are constructed based on MXene and montmorillonite (MMT) via a simple vacuum-assisted filtration technique. The presence of MMT can protect the MXene from oxidation and endow the composite films with exceptional fire-resistant ability. The impressive thermal conductivity performance, high in-plane thermal conductivity (28.8 W m –1 K –1 ) and low cross-plane thermal conductivity (0.27 W m –1 K –1 ), ingeniously enables highly efficient in-plane heat dissipation and cross-plane heat insulation in the MXene-based films simultaneously. The high electrical conductivity (4420 S m –1 ) of the composite film enables an excellent EMI shielding effectiveness of over 65 dB in the entire X-band and a high specific shielding effectiveness of over 10 000 dB cm 2 g –1 at a thickness of only…

Recently, several types of lead halide perovskites have been demonstrated as active layers in resistive switching memory or artificial synaptic devices for neuromorphic computing applications. However, the thermal instability and toxicity of lead halide perovskites severely restricted their further practical applications. Herein, the environmentally friendly and uniform Cs 3 Cu 2 I 5 perovskite films are introduced to act as the active layer in the Ag/Cs 3 Cu 2 I 5 /ITO memristor. Generally, the Ag ions could react with iodide ions and form AgI x compounds easily, so the Ag/PMMA/Cs 3 Cu 2 I 5 /ITO memristor was designed by employing the ultrathin polymethylmethacrylate (PMMA) layer to avoid the direct contact between the top Ag electrode and Cs 3 Cu 2 I 5 perovskite films. After optimization, the obtained memristor demonstrated bipolar resistive switching with low operating voltage (< ±1 V), large on/off ratio (10 2 ), stable endurance (100 cycles), and long retention (>10 4 s). Additionally, biological synaptic behaviors including long-term potentiation and long-term depression…

The core challenge of MnO 2 as the cathode material of zinc-ion batteries remains to be their poor electrochemical kinetics and stability. Herein, MnO 2 superfine nanowires (∼10 nm) with rich crystal defects (oxygen vacancies and cavities) are demonstrated to possess high efficient zinc-ion storage capability. Experimental and theoretical studies demonstrate that the defects facilitate the adsorption and diffusion of hydrogen/zinc for fast ion transportation and the build of a local electric field for improved electron migration. In addition, the superfine nanostructure could provide sufficient active sites and short diffusion pathways for further promotion of capacity and reaction kinetics of MnO 2 . Remarkably, the defect-enriched MnO 2 nanowires manifest an energy density as high as 406 W h kg –1 and an excellent durability over 1000 cycles without noticeable capacity degradation. Mechanistic analysis substantiates a reversible coinsertion/extraction process of H + and Zn 2+ with a simultaneous deposition/dissolution of zinc sulfate hydroxide hydrate nanoflakes. This work could…

Physicians have long been calling for an inherent antimicrobial wound dressing, which will be a great progress for treating complicated infections. Here, we report a novel bioadhesive hydrogel with inherent antibacterial properties prepared by mixing modified hyaluronic acid (HA) and ε-polylysine (EPL). This hydrogel can effectively kill Gram (+) and (-) bacteria for its high positive charge density on the surface. The sol-gel transition occurs within seconds via horseradish peroxidase enzymatic cross-linking and Schiff base reaction, which also allows the hydrogel to recover completely from destruction quickly within 5 min. In an infected rat wound model, histological studies indicated that the hydrogels effectively killed bacteria on the surface of wounds and accelerated wound healing. Histological analysis indicated that the thickness of the newborn skin, the density of the newborn microvascular, granulation tissue, and the collagen of rats treated with hydrogel dressings were twice as high as those treated by commercial fibrin glue. These results indicate that the HA/EPL…

Molybdenum disulfide (MoS 2 ) with excellent properties has been widely reported in recent years. However, it is a great challenge to achieve p-type conductivity in MoS 2 because of its native stubborn n-type conductivity. Substitutional transition metal doping has been proved to be an effective approach to tune their intrinsic properties and enhance device performance. Herein, we report the growth of Nb-doping large-area monolayer MoS 2 by a one-step salt-assisted chemical vapor deposition method. Electrical measurements indicate that Nb doping suppresses n-type conductivity in MoS 2 and shows an ambipolar transport behavior after annealing under the sulfur atmosphere, which highlights the p-type doping effect via Nb, corresponding to the density functional theory calculations with Fermi-level shifting to valence band maximum. This work provides a promising approach of two-dimensional materials in electronic and optoelectronic applications.

Two-dimensional titanium carbide (Ti 3 C 2 T x ), or MXene, is a new nanomaterial that has attracted increasing interest due to its metallic conductivity, good solution processability, and excellent energy storage performance. However, Ti 3 C 2 T x MXene flakes suffer from degradation through oxidation due to prolonged exposure to oxygenated water. Preventing the occurrence of oxidation, i.e., the formation of TiO 2 particles, was found to be crucial in maintaining MXene quality. In the present work, we found that freezing aqueous MXene dispersions at a low temperature can effectively prevent the formation of TiO 2 nanoparticles at the flake edge, which is known as the early stage of oxidation. The Ti 3 C 2 T x flakes in frozen dispersion remain consistent in morphology and elemental composition for over 650 days, compared with freshly synthesized MXene, which in contrast exhibits flake edge degradation within two days when stored at room temperature. This result suggests that freezing a MXene dispersion dramatically postpones the oxidation of MXene flakes and that the stored MXene…

Piezocatalysts have attracted much attention due to their excellent degradation ability for organics. In this work, three types of BaTiO 3 (BTO) nanostructures, including hydrothermally synthesized nanocubes (NCs), sol–gel calcined nanoparticles (NPs), and electrospun nanofibers (NFs), are prepared for catalyzing the dye degradation. Compared with the NCs and NPs, the NFs exhibit a higher piezocatalytic degradation performance due to the large specific surface area, fine crystal size, and easy deformation structure. Moreover, the kinetic factors, including initial dye concentration, ionic strength, ultrasonic power, and applied action, influencing the degradation performance of the BTO NFs are analyzed deeply. A high degradation rate constant of 0.0736 min –1 is achieved for rhodamine B, which is superior compared with the previous reports. The excellent stability of BTO NFs is demonstrated by the cycling tests, where a high degradation efficiency of 97.6% within 110 min is still obtained after the third cycle. Furthermore, the mechanism of piezocatalysis revealed that the hydroxyl…

Flexible and transparent surface-enhanced Raman scattering (SERS) substrates have long been sought-after for nondestructive detection of analytes on nonplanar surfaces, but there is still a lack of one convenient and robust way to fabricate such SERS substrates rapidly. Herein, we demonstrate the fabrication of a high-performance SERS substrate consisting of plasmonic Ag nanocube (Ag NC) arrays anchored onto a flexible transparent poly(dimethylsiloxane) (PDMS) membrane. Through a simple organic/water interfacial self-assembly method, arrays of presynthesized Ag NCs are obtained and directly retrieved onto the PDMS membrane without the aid of rigid substrates (e.g., Si wafers or glass slides). The plasmonic Ag NC arrays can produce strong electromagnetic enhancement, achieving high SERS enhancement factor (∼3.43 × 10 6 ) and ideal detection capability for methylene blue (MB) and Rhodamine 6G (R6G) at respective trace amounts of 10 –10 and 10 –9 M. Moreover, without the need to transfer from substrate to substrate, the regular Ag NC arrays are kept intact, thereby yielding a good…

MXene has exhibited great potential for use in wearable devices, especially as pressure sensors, due to its lamellar structure, which changes its resistance as a function of interlayer distance. Despite the good performance of the reported pure MXene pressure sensors, their practical applications are limited by moderate flexibility, excessively high MXene conductivity, and environmental effects. To address the above challenges, we incorporated multilayer MXene particles into hydrophobic poly(vinylidene fluoride) trifluoroethylene (P(VDF-TrFE)) and prepared freestanding, flexible, and stable films via spin-coating. These films were assembled into highly sensitive piezoresistive pressure sensors, which show a fast response time of 16 ms in addition to excellent long-term stability with no obvious responsivity attenuation when the sensor is exposed to air, even after 20 weeks. Moreover, the fabricated sensors could monitor human physiological signals such as knee bending and cheek bulging and could be used for speech recognition. The mapping spatial pressure distribution function was…

Piezoresistive composite-based flexible pressure sensors often suffer from a trade-off between the sensitivity and measurement range. Moreover, the sensitivity or measurement range is theoretically limited owing to the negative piezoresistive coefficient, resulting in resistance variation below 100%. Here, flexible pressure sensors were fabricated using the three-dimensional (3D) printing technique to improve both the sensitivity and sensing range through the positive piezoresistive effect. With the addition of carbon nanotubes (CNTs) and fumed silica nanoparticles (SiNPs) as a conductive filler and rheology modifier, respectively, the viscoelastic silicone rubber solution converted to a printable gel ink. Soft and porous composites (SPCs) were then directly printed in air at room temperature. The sensitivity and sensing range of the SPC-based pressure sensor can be simultaneously tuned by adjusting the conducting CNT and insulating SiNP contents. By optimizing the density of the CNT conductive network in the matrix, positive piezoresistive sensitivity (+0.096 kPa –1 ) and a large…

In the management of accelerating wound healing, moist environments play an important role. Compared with other scaffolds of various forms, hydrogels can maintain a moist environment in the wound area. They are cross-linked hydrophilic polymeric networks that resemble natural soft tissues and extracellular matrices. Among them, injectable hydrogels have attracted great attention in wound repair, as they can be injected into irregular-shaped skin defects and formed in situ to shape the contour of different dimensions. The excellent compliance makes hydrogels easy to adapt to the wound under different conditions of skin movement. Here, we oxidized hydroxyethyl starch (O-HES) and modified carboxymethyl chitosan (M-CMCS) to fabricate an in situ forming hydrogel with excellent self-recoverable extensibility-compressibility, biocompatibility, biodegradability, and transparency for accelerating wound healing. The oxidation degree of O-HES was 74%. The amino modification degree of M-CMCS was 63%. M-CMCS/O-HES hydrogels were formed through the Schiff base reaction. The physicochemical…

Monometallic and bimetallic MOF-74-M (M = Mn, Co, Ni, Zn, MnCo, MnNi, and MnZn) catalysts were prepared by the solvothermal method for NH 3 -SCR. XRD, BET, SEM, and EDS-mapping tests indicate the successful synthesis of the MOF-74-M catalyst with uniform distribution of metal elements and large specific surface area, and the morphology is almost hexagonal. Adding Mn element to a single-metal catalyst can enhance activity, which is mainly because of the existence of various valence states of Mn so that it has excellent redox properties; the catalytic activity of water and sulfur resistance tests showed that the catalytic activity of MOF-74-M increases after adding a proper amount of SO 2, mainly because of the increase in acidic sites. In situ DRIFTS results indicate that the low-temperature range of MOF-74-MnCo and MOF-74-Mn is dominated by the E–R mechanism and the high-temperature range is dominated by the L–H mechanism. The entire temperature range of MOF-74-Zn is dominated by the L–H mechanism.

It is essential to impart the thermal stability, high sensitivity, self-healing, and transparent attributes to the emerging wearable and stretchable electronics. Here, a facile solvent replacement strategy is exploited to introduce ethylene glycol/glycerol (Gly) in hydrogels for enhancing their thermal sensitivity and stability synchronously. For the first time, we find that the solvent plays a key role in the thermal sensitivity of hydrogels. By adjusting the water content in hydrogels using a simple dehydration treatment, the thermal sensitivity is raised to 13.1%/°C. Thanks to the ionic transport property and water-Gly binary solvent, the organohydrogel achieves an unprecedented thermal sensitivity of 19.6%/°C, which is much higher than those of previously reported stretchable thermistors. The mechanism for the thermal response is revealed by considering the thermally activated ion mobility and dissociation. The stretchable thermistors are conformally attached on curved surfaces for the practical monitoring of minute temperature change. Notably, the uncovered Gly-organohydrogel…

Owing to the characteristics of mimicking human skin’s function and transmitting sensory signals, electronic skin (e-skin), as an emerging and exciting research field, has inspired tremendous efforts in the biomedical field. However, it is frustrating that most e-skins are prone to bacterial infections, resulting a serious threat to human health. Therefore, the construction of e-skin with an integrated perceptual signal and antibacterial properties is highly desirable. Herein, the dynamic supramolecular hydrogel was prepared through a freezing/thawing method by cross-linking the conductive graphene (G), biocompatible polyvinyl alcohol (PVA), self-adhesive polydopamine (PDA), and in situ formation antibacterial silver nanoparticles (AgNPs). Having fabricated the hierarchical network structure, the PVA–G–PDA–AgNPs composite hydrogel with a tensile strength of 1.174 MPa and an elongation of 331% paves way for flexible e-skins. Notably, the PVA–G–PDA–AgNPs hydrogel exhibits outstanding antibacterial activity to typical pathogenic microbes (e.g., Gram-negative Escherichia coli and…

A high-performance formaldehyde sensor based on nickel (Ni)-doped indium trioxide (In 2 O 3 )/tungsten disulfide (WS 2 ) nanocomposite was demonstrated. An epoxy substrate served as matrix of the Ni–In 2 O 3 /WS 2 nanocomposite sensor. The material properties of self-assembled Ni–In 2 O 3 /WS 2 nanoheterostructure were fully characterized and confirmed. The formaldehyde-sensing properties of the Ni–In 2 O 3 /WS 2 composite were tested at 25 °C. Compared to the In 2 O 3, WS 2, and their composite, the Ni–In 2 O 3 /WS 2 sensor demonstrated significant improvement on the formaldehyde-sensing performance, including a low detection limit of 15 ppb, good selectivity, repeatability, fast detection rate, and a fair logarithmic function toward formaldehyde concentration. The dramatically enhanced sensing performance of Ni–In 2 O 3 /WS 2 film sensor can be attributed to the Ni ion doping and synergistic interfacial incorporation of In 2 O 3 /WS 2 heterojunction. The sensitive mechanism of the Ni–In 2 O 3 /WS 2 film sensor toward formaldehyde is explored through density functional theory (DFT)…

The rapid expansion of the development of the electrochemical capacitor appliance and its industry areas has created the need for long cycling stability of over 30 000 cycles along with an ultrafast performance (referred to as ultrafast longevity). In recent years, zinc-ion hybrid supercapacitors (ZICs) are considered to be emerging energy storage applications thanks to their high specific capacity and remarkable cycling stability. However, ZICs still face serious challenges in overcoming the ultrafast performance and lifetime limitations related to the cathode materials, activated carbon (AC), due to inadequate electrical properties and poor wettability between the electrolyte and the electrode, which cause reductions in specific capacity and lifetime rapidly at high current densities during cycling. To address these drawbacks, a novel phosphorus (P) and boron (B) codoped AC (designated P&B-AC) is presented herein with enhanced electrical properties due to B-doping along with improved wettability due to P-doping to provide an ultrafast longevity ZICs. The prepared ZICs display a…

High Resolution Image Download MS PowerPoint Slide SARS-CoV-2, the virus that causes the disease COVID-19, remains viable on solids for periods of up to 1 week, so one potential route for human infection is via exposure to an infectious dose from a solid. We have fabricated and tested a coating that is designed to reduce the longevity of SARS-CoV-2 on solids. The coating consists of cuprous oxide (Cu 2 O) particles bound with polyurethane. After 1 h on coated glass or stainless steel, the viral titer was reduced by about 99.9% on average compared to the uncoated sample. An advantage of a polyurethane-based coating is that polyurethane is already used to coat a large number of everyday objects. Our coating adheres well to glass and stainless steel as well as everyday items that people may fear to touch during a pandemic, such as a doorknob, a pen, and a credit card keypad button. The coating performs well in the cross-hatch durability test and remains intact and active after 13 days of being immersed in water or after exposure to multiple cycles of exposure to the virus and…

Abstract Ceramic dielectrics are reported with superior energy storage performance for applications, such as power electronics in electrical vehicles. A recoverable energy density (Wrec) of ∼4.55 J cm–3 with η ∼ 90% is achieved in lead-free relaxor BaTiO3-0.06Bi2/3(Mg1/3Nb2/3)O3 ceramics at ∼520 kV cm–1. These ceramics may be co-fired with Ag/Pd, which constitutes a major step forward toward their potential use in the fabrication of commercial multilayer ceramic capacitors. Compared to stoichiometric Bi(Mg2/3Nb1/3)O3-doped BaTiO3 (BT), A-site deficient Bi2/3(Mg1/3Nb2/3)O3 reduces the electrical heterogeneity of BT. Bulk conductivity differs from the grain boundary only by 1 order of magnitude which, coupled with a smaller volume fraction of conducting cores due to enhanced diffusion of the dopant via A-site vacancies in the A-site sublattice, results in higher breakdown strength under an electric field. This strategy can be employed to develop new dielectrics with improved energy storage performance.

A new approach is employed to boost the electrochemical kinetics and stability of vanadium oxygen hydrate (VOH, V 2 O 5 · n H 2 O) employed for aqueous zinc-ion battery (ZIB) cathodes. The methodology is based on electrically conductive polyaniline (PANI) intercalated–exfoliated VOH, achieved by preintercalation of an aniline monomer and its in situ polymerization within the oxide interlayers. The resulting graphene-like PANI–VOH nanosheets possess a greatly boosted reaction-controlled contribution to the total charge storage capacity, resulting in more material undergoing the reversible V 5+ to V 3+ redox reaction. The PANI–VOH electrode obtains an impressive capacity of 323 mAh g –1 at 1 A g –1, and state-of-the-art cycling stability at 80% capacity retention after 800 cycles. Because of the facile redox kinetics, the PANI–VOH ZIB obtains uniquely promising specific energy–specific power combinations: an energy of 216 Wh kg –1 is achieved at 252 W kg –1, while 150 Wh kg –1 is achieved at 3900 W kg –1 . Electrochemical impedance spectroscopy (EIS) and galvanostatic intermittent…

Diabetic skin ulcer is one of the severe complications of diabetes mellitus, which has a high incidence and may cause death or disability. Platelet-rich plasma (PRP) is widely used in the treatment of diabetic wounds due to the effect of growth factors (GFs) derived from it. However, the relatively short half-life of GFs limits their applications in clinics. In addition, the presence of a large amount of proteases in the diabetic wound microenvironment results in the degradation of GFs, which further impedes angiogenesis and diabetic wound healing. In our study, we fabricated a self-healing and injectable hydrogel with a composite of chitosan, silk fibroin, and PRP (CBPGCTS–SF@PRP) for promoting diabetic wound healing. CBPGCTS–SF@PRP could protect PRP from enzymatic hydrolysis, release PRP sustainably, and enhance the chemotaxis of mesenchymal stem cells. The results showed that it could promote the proliferation of repair cells in vitro . Moreover, it could enhance wound healing by expediting collagen deposition, angiogenesis, and nerve repair in a type 2 diabetic rat model and a…

A loose nanofiltration (NF) membrane with excellent dye rejection and high permeation of inorganic salt is required to fractionate dye/salt mixture in dye wastewater treatment. In this study, we fabricated the loose NF membrane by using the electrospray interfacial polymerization (EIP) method. It is a novel and facile interfacial polymerization method, which controls the thickness of the poly(piperazine-amide) (PPA) layer in nanometers (1 nm/min) and changes cross-linking degree of PPA layer and pore size by varying the electrospray time; consequently, water permeance and dye/salt rejection ratio can be handled. The fabricated EIP membrane with an optimized fabrication condition (M30, electrospray time was 30 min) possessed excellent pure water permeance (20.2 LMH/bar), high dye rejection (e.g., 99.6% for congo red (CR)), and low salt rejection (e.g., 6.3% for NaCl). Moreover, the EIP membrane exhibited enhanced antifouling property than commercial NF membrane (NF90) with a high flux recovery rate (FRR) of 87.1% and low irreversible fouling ( R ir ) of 12.9% after fouled by bovine…

This paper presents a ZnO-CuO p-n heterojunction chemiresistive sensor that comprises CuO hollow nanocubes attached to ZnO spherical cores as active materials. These ZnO-CuO core-hollow cube nanostructures exhibit a remarkable response of 11.14 at 1 ppm acetone and 200 °C, which is a superior result to those reported by other metal-oxide-based sensors. The response can be measured up to 40 ppb, and the limit of detection is estimated as 9 ppb. ZnO-CuO core-hollow cube nanostructures also present high selectivity toward acetone against other volatile organic compounds and demonstrate excellent stability for up to 40 days. The outstanding gas-sensing performance of the developed nanocubes is attributed to their uniform and unique morphology. Their core-shell-like structures allow the main charge transfer pathways to pass the interparticle p-p junctions, and the p-n junctions in each particle increase the sensitivity of the reactions to gas molecules. The small grain size and high surface area of each domain also enhance the surface gas adsorption.

With the growing development of the Internet of Things, organic photovoltaic (OPV) cells are highly desirable for indoor applications because of the unique features of light weight, flexibility, and coloration. Emission spectra of the commonly used indoor light sources are much narrower with lower light intensity as compared to the standard solar spectrum. High tunability in optical absorption, insensitivity to series resistance and the active layer thickness, and mild operating conditions make indoor OPV cells promising as a practically relevant technology. Currently, the OPV module has obtained a power conversion efficiency of over 20%, with excellent stability under indoor conditions. However, at the present stage, the device physics investigations and material design strategies developed in an OPV cell for indoor applications lag behind those for outdoor applications. In particular, the emerging characterizations in photovoltaic measurements have severely affected the reliability of reports. This Spotlight on Applications highlights these opportunities and challenges of OPV…

Abstract Despite that two-dimensional transition metal carbides and carbonitrides (MXenes) are burgeoning candidates for remediation of environmental pollutants, the construction of robust functionalized MXene nanosheets with a high affinity for target heavy metal ions and radionuclides remains a challenge. Here we report the successful placement of amidoxime chelating groups on Ti3C2Tx MXene surface by diazonium salt grafting. The introduction of amidoxime functional groups significantly enhances the selectivity of Ti3C2Tx nanosheets for uranyl ions and also greatly improves their stability in aqueous solution, enabling efficient, rapid, and recyclable uranium extraction from aqueous solutions containing competitive metal ions. Benefiting from the excellent conductivity of MXenes, the amidoxime functionalized Ti3C2Tx nanosheets show outstanding electrochemical performance such that when loaded on carbon cloth the application of an electric field increases the uranium adsorption capacity from 294 to 626 mg/g, outperforming all organic electrochemical sorption materials reported…

Preventing ice formation and ice swift removal from the solid surface are essential in numerous application fields. Superhydrophobic coating is an effective way to delay the icing phenomenon. However, the superhydrophobic coating was wetted easily after icing-deicing cycles that led to the failure of anti-icing. In this study, a robust, amphiphobic coating consisted of fluorinated multiwalled carbon nanotubes (FMWCNTs) and commercial polyurethane was constructed by a simply spray process. Because of the addition of FMWCNTs, the coating demonstrated a good amphiphobic feature and highly efficient photothermal conversion, which endowed the coating surface with excellent deicing and defrosting characteristics under sunlight irradiation. In addition, self-cleaning and self-healing properties of the coating under sunlight ensured its efficient photothermal conversion and long service life. To further improve the photothermal deicing effect, a coating system containing a photothermal layer (P), thermal-conductive layer (C), and thermal-protective layer (P) was constructed. The heat…

Carbon-coated SiO x microparticles (SiO x /C) demonstrate attractive potential for anode use in high-energy-density lithium-ion batteries due to high capacity and proper cycling stability. However, the excessive irreversible consumption of Li ions during the initial cycling remains a serious challenge arising from the limited lithium in full cells. Here, we endow SiO x /C anode with high initial Coulombic efficiency using the chemical pre-lithiation strategy. The lithium silicate is uniformly pregenerated in SiO x /C microparticles, which could effectively counteract the irreversible consumption of Li ions and avoid the complicated pre-lithiation process. Moreover, this strategy guarantees the structural integrity and processability of anode materials because of the homogeneous Li–organic complex solution pre-lithiation and high-temperature calcination process. The obtained SiO x /C microparticles can be applied as anode materials by directly mixing with commercial graphite, which demonstrates proper specific capacity, high initial Coulombic efficiency, and excellent cycling…

Magnetic soft materials (MSMs) have shown potential in soft robotics, actuators, metamaterials, and biomedical devices because they are capable of untethered, fast, and reversible shape reconfigurations as well as controllable dynamic motions under applied magnetic fields. Recently, magnetic shape memory polymers (M-SMPs) that incorporate hard magnetic particles in shape memory polymers demonstrated superior shape manipulation performance by realizing reprogrammable, untethered, fast, and reversible shape transformation and shape locking in one material system. In this work, we develop a multimaterial printing technology for the complex structural integration of MSMs and M-SMPs to explore their enhanced multimodal shape transformation and tunable properties. By cooperative thermal and magnetic actuation, we demonstrate multiple deformation modes with distinct shape configurations, which further enable active metamaterials with tunable physical properties such as sign-change Poisson's ratio. Because of the multiphysics response of the M-MSP/MSM metamaterials, one distinct feature is…

Cell membrane camouflaged nanoparticles (NPs) have been increasingly explored to leverage natural cellular functions and adapt to various biomedical applications. Herein, we report an OMV-CC hybrid membrane, which consists of a bacterial outer membrane vesicle (OMV) and B16-F10 cancer cell (CC) membrane, and successfully coat it onto hollow polydopamine (HPDA) NPs. We harness the advantage of OMV immunotherapy together with HPDA-mediated photothermal therapy (PTT) to improve the antitumor efficacy toward melanoma. When injected intravenously via the tail vein, HPDA@[OMV-CC] NPs homogeneously target melanoma and activate the immune response by rapidly stimulating dendritic cell (DC) maturation in lymph nodes in the vaccinated mice. Our results show that the antitumor immune response and PTT reciprocally potentiate the therapeutic ability and fully eradicate melanoma without notable adverse effects. The homogeneous-target and immune activation hybrid biomimetic membrane provides the adaptability to various synergistic therapeutic and imaging applications by incorporating payload with…

Nanocellulose-based porous materials have been recently considered as ideal candidates in various applications. However, challenges on performances remain owing to the disorderly structure and the limited transport specificity. Herein, wood-inspired composite sponges consisting of cellulose nanofibrils (CNFs) and high-aspect-ratio silver nanowires (AgNWs) were generated with anisotropic properties by the directional freeze-drying. The obtained composite sponges exhibited attractive features, such as an excellent compressive stress of 24.5 kPa, low percolation threshold of 0.1 vol % AgNWs, and high electrical conductivity of 1.52 S/cm. Furthermore, the self-assembled ordered structure in the longitudinal direction and synergistic effect between CNFs and AgNWs benefited the sponge interesting anisotropic electrical conductivity, thermal diffusivity, ultrafast electrically induced heating (<5 s), sensitive pressure sensing (errors <0.26%), and electromagnetic interference (EMI) shielding for special practical demands. This multifunctional material inspired by natural woods is expected…

Hard carbon (HC) is an attractive anode material for low-cost and high-energy density sodium-ion batteries (SIBs); however, its low initial Coulombic efficiency (ICE) limits its practical battery application. To overcome this problem, we reported a facile strategy to compensate the irreversible capacity loss of HC anodes simply by a chemical presodiation reaction of the HC electrode with a sodiation reagent (sodium biphenyl, Na-Bp). Benefiting from the strong sodiation ability of Na-Bp, HC anodes can be presodiated rapidly in a very short time and the presodiated HC (Na x HC) is found to have a desirable ICE of 100%. When coupled with the Na 3 V 2 (PO 4 ) 3 cathode to build a SIB full cell, the Na x HC||Na 3 V 2 (PO 4 ) 3 cell exhibits a high ICE of ∼95.0% and an elevated energy density of 218 W h kg –1, which are far superior to those of the control cell using a pristine HC anode (50% ICE and 120 W h kg –1, respectively), suggesting great advantages brought about by the chemical presodiation process. More importantly, this presodiation reaction is very mild and highly efficient and…

Sulfur-doped two-dimensional (2D) graphitic carbon nitride nanosheets (2D-SCN) with efficient photocatalytic activity were synthesized via (1) polycondensation of thiourea to form bulk sulfur-doped graphitic carbon nitride (SCN) and (2) followed by thermal oxidative treatment of the prepared SCN via an etching strategy to form 2D-SCN. Sulfur was doped in situ into SCN by using thiourea as the precursor, and the 2D nanosheet structure was obtained during the thermal oxidative etching process. The structural, morphological, and optical properties of the 2D-SCN sample were investigated in detail. Herein, it is shown that the thermal oxidative etching treatment and sulfur doping induced a 2D nanosheet structure (2D-SCN-3h) with a thickness of about 4.0 nm and exposure of more sulfur elements on the surface. The surface area increased from 16.6 m 2 /g for SCN to 226.9 m 2 /g. Compared to bulk SCN, a blue shift of the absorption peaks was observed for the obtained 2D-SCN-3h photocatalyst, and the absorption intensity was higher than that of the sulfur-free counterpart (2D-CN). The…