The 100 most-cited articles in ACS Applied Materials & Interfaces, 2017

Wearable gas sensors have received lots of attention for diagnostic and monitoring applications, and two-dimensional (2D) materials can provide a promising platform for fabricating gas sensors that can operate at room temperature. In the present study, the room temperature gas-sensing performance of Ti 3 C 2 T x nanosheets was investigated. 2D Ti 3 C 2 T x (MXene) sheets were synthesized by removal of Al atoms from Ti 3 AlC 2 (MAX phases) and were integrated on flexible polyimide platforms with a simple solution casting method. The Ti 3 C 2 T x sensors successfully measured ethanol, methanol, acetone, and ammonia gas at room temperature and showed a p-type sensing behavior. The fabricated sensors showed their highest and lowest response toward ammonia and acetone gas, respectively. The limit of detection of acetone gas was theoretically calculated to be about 9.27 ppm, presenting better performance compared to other 2D material-based sensors. The sensing mechanism was proposed in terms of the interactions between the majority charge carriers of Ti 3 C 2 T x and gas species.

Wearable electronics is expected to be one of the most active research areas in the next decade; therefore, nanomaterials possessing high carrier mobility, optical transparency, mechanical robustness and flexibility, lightweight, and environmental stability will be in immense demand. Graphene is one of the nanomaterials that fulfill all these requirements, along with other inherently unique properties and convenience to fabricate into different morphological nanostructures, from atomically thin single layers to nanoribbons. Graphene-based materials have also been investigated in sensor technologies, from chemical sensing to detection of cancer biomarkers. The progress of graphene-based flexible gas and chemical sensors in terms of material preparation, sensor fabrication, and their performance are reviewed here. The article provides a brief introduction to graphene-based materials and their potential applications in flexible and stretchable wearable electronic devices. The role of graphene in fabricating flexible gas sensors for the detection of various hazardous gases, including…

Ti 3 C 2 MXene is a new two-dimensional material exhibiting a variety of novel properties including good photothermal effect, and the capability of Ti 3 C 2 for multimodal tumor therapy is in urgent need of development. Herein, ultrathin Ti 3 C 2 MXene nanosheets (∼100 nm) have been synthesized by supplying additive Al 3+ to avoid Al loss and employed as a photothermal/photodynamic agent for cancer therapy. The as-obtained nanosheets exhibit outstanding mass extinction coefficient (28.6 Lg –1 cm –1 at 808 nm), superior photothermal conversion efficiency (∼58.3%), and effective singlet oxygen generation ( 1 O 2 ) upon 808 nm laser irradiation. Based on these Ti 3 C 2 nanosheets, a multifunctional nanoplatform (Ti 3 C 2 -DOX) is established via layer-by-layer surface modification with doxorubicin (DOX) and hyaluronic acid (HA). In vitro and in vivo experiments disclose that Ti 3 C 2 -DOX shows enhanced biocompatibility, tumor specific accumulation, and stimuli-responsive drug release behavior and achieve effective cancer cell killing and tumor tissue destruction through…

Solar steam generation is a highly promising technology for harvesting solar energy, desalination and water purification. We introduce a novel bilayered structure composed of wood and graphene oxide (GO) for highly efficient solar steam generation. The GO layer deposited on the microporous wood provides broad optical absorption and high photothermal conversion resulting in rapid increase in the temperature at the liquid surface. On the other hand, wood serves as a thermal insulator to confine the photothermal heat to the evaporative surface and to facilitate the efficient transport of water from the bulk to the photothermally active space. Owing to the tailored bilayer structure and the optimal thermo-optical properties of the individual components, the wood–GO composite structure exhibited a solar thermal efficiency of ∼83% under simulated solar excitation at a power density of 12 kW/m 2 . The novel composite structure demonstrated here is highly scalable and cost-efficient, making it an attractive material for various applications involving large light absorption, photothermal…

Abstract Organic–inorganic halide perovskite materials (e.g., MAPbI3, FAPbI3, etc.; where MA = CH3NH3+, FA = CH(NH2)2+) have been studied intensively for photovoltaic applications. Major concerns for the commercialization of perovskite photovoltaic technology to take off include lead toxicity, long-term stability, hysteresis, and optimal bandgap. Therefore, there is still need for further exploration of alternative candidates. Elemental composition engineering of MAPbI3 and FAPbI3 has been proposed to address the above concerns. Among the best six certified power conversion efficiencies reported by National Renewable Energy Laboratory on perovskite-based solar cells, five are based on mixed perovskites (e.g., MAPbI1–xBrx, FA0.85MA0.15PbI2.55Br0.45, Cs0.1FA0.75MA0.15PbI2.49Br0.51). In this paper, we review the recent progress on the synthesis and fundamental aspects of mixed cation and halide perovskites correlating with device performance, long-term stability, and hysteresis. In the outlook, we outline the future research directions based on the reported results as well as related…

This Review provides a comprehensive analysis of recent development in the field of aggregation-induced emission (AIE)-active tetraphenylethylene (TPE) luminophores and their applications in biomolecular science. It begins with a discussion of the diverse range of structural motifs that have found particular applications in sensing, and demonstrates that TPE structures and their derivatives have been used for a diverse range of analytes such as such as H +, anions, cations, heavy metals, organic volatiles, and toxic gases. Advances are discussed in depth where TPE is utilized as a mechanoluminescent material in bioinspired receptor units with specificity for analytes for such as glucose or RNA. The rapid advances in sensor research make this summary of recent developments in AIE-active TPE luminophores timely, in order to disseminate the advantages of these materials for sensing of analytes in solution, as well as the importance of solid and aggregated states in controlling sensing behavior.

Solar-enabled steam generation has attracted increasing interest in recent years because of its potential applications in power generation, desalination, and wastewater treatment, among others. Recent studies have reported many strategies for promoting the efficiency of steam generation by employing absorbers based on carbon materials or plasmonic metal nanoparticles with well-defined pores. In this work, we report that natural wood can be utilized as an ideal solar absorber after a simple flame treatment. With ultrahigh solar absorbance (∼99%), low thermal conductivity (0.33 W m –1 K –1 ), and good hydrophilicity, the flame-treated wood can localize the solar heating at the evaporation surface and enable a solar-thermal efficiency of ∼72% under a solar intensity of 1 kW m –2, and it thus represents a renewable, scalable, low-cost, and robust material for solar steam applications.

Low-cost and highly efficient bifunctional electrocatalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) are intensively investigated for overall water splitting. Herein, we combined experimental research with first-principles calculations based on density functional theory (DFT) to engineer the NiCo 2 S 4 @NiFe LDH heterostructure interface for enhancing overall water-splitting activity. The DFT calculations exhibit strong interaction and charge transfer between NiCo 2 S 4 and NiFe LDH, which change the interfacial electronic structure and surface reactivity. The calculated chemisorption free energy of hydroxide (Δ E OH ) is reduced from 1.56 eV for pure NiFe LDH to 1.03 eV for the heterostructures, indicating a dramatic improvement in OER performance, while the chemisorption free energy of hydrogen (Δ E H ) maintains almost invariable. By the use of the facile hydrothermal method, NiCo 2 S 4 nanotubes, NiFe LDH nanosheets, and NiCo 2 S 4 @NiFe LDH heterostructures are prepared on nickel foam, of which the corresponding experimental OER…

2D/2D interface heterostructures of g-C 3 N 4 and NiAl-LDH are synthesized utilizing strong electrostatic interactions between positively charged 2D NiAl-LDH sheets and negatively charged 2D g-C 3 N 4 nanosheets. This new 2D/2D interface heterojunction showed remarkable performance for photocatalytic CO 2 reduction to produce renewable fuels such as CO and H 2 under visible-light irradiation, far superior to that of either single phase g-C 3 N 4 or NiAl-LDH nanosheets. The enhancement of photocatalytic activity could be attributed mainly to the excellent interfacial contact at the heterojunction of g-C 3 N 4 /NiAl-LDH, which subsequently results in suppressed recombination, and improved transfer and separation of photogenerated charge carriers. In addition, the optimal g-C 3 N 4 /NiAl-LDH nanocomposite possessed high photostability after successive experimental runs with no obvious change in the production of CO from CO 2 reduction. Our findings regarding the design, fabrication and photophysical properties of 2D/2D heterostructure systems may find use in other photocatalytic…

Ultralight, high-performance electromagnetic interference (EMI) shielding graphene foam (GF)/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) composites are developed by drop coating of PEDOT:PSS on cellular-structured, freestanding GFs. To enhance the wettability and the interfacial bonds with PEDOT:PSS, GFs are functionalized with 4-dodecylbenzenesulfonic acid. The GF/PEDOT:PSS composites possess an ultralow density of 18.2 × 10 –3 g/cm 3 and a high porosity of 98.8%, as well as an enhanced electrical conductivity by almost 4 folds from 11.8 to 43.2 S/cm after the incorporation of the conductive PEDOT:PSS. Benefiting from the excellent electrical conductivity, ultralight porous structure, and effective charge delocalization, the composites deliver remarkable EMI shielding performance with a shielding effectiveness (SE) of 91.9 dB and a specific SE (SSE) of 3124 dB·cm 3 /g, both of which are the highest among those reported in the literature for carbon-based polymer composites. The excellent electrical conductivities of composites arising from both the GFs with…

Abstract The combination of magnetic nanoparticles and metal–organic frameworks (MOFs) has demonstrated their prospective for pollutant sequestration. In this work, a magnetic metal–organic framework nanocomposite (Fe3O4@AMCA-MIL53­(Al) was prepared and used for the removal of U­(VI) and Th­(IV) metal ions from aqueous environment. Fe3O4@AMCA-MIL53­(Al) nanocomposite was characterized by TGA, FTIR, SEM-EDX, XRD, HRTEM, BET, VSM (vibrating sample magnetometry), and XPS analyses. A batch technique was applied for the removal of the aforesaid metal ions using Fe3O4@AMCA-MIL53­(Al) at different operating parameters. The isotherm and kinetic data were accurately described by the Langmuir and pseudo-second-order models. The adsorption capacity was calculated to be 227.3 and 285.7 mg/g for U­(VI) and Th­(IV), respectively, by fitting the equilibrium data to the Langmuir model. The kinetic studies demonstrated that the equilibrium time was 90 min for each metal ion. Various thermodynamic parameters were evaluated which indicated the endothermic and spontaneous nature of adsorption. The…

Novel zinc anodes are synthesized via electroplating with organic additives in the plating solution. The selected organic additives are cetyltrimethylammonium bromide (CTAB), sodium dodecyl sulfate (SDS), polyethylene-glycol (PEG-8000), and thiourea (TU). The synthesized zinc anode materials, namely, Zn-CTAB, Zn-SDS, Zn-PEG, and Zn-TU, are characterized by powder X-ray diffraction and scanning electron microscopy. The results show that each additive produces distinctively different crystallographic orientation and surface texture. The surface electrochemical activity is characterized by linear polarization when the zinc is in contact with the battery's electrolyte. Tafel fitting on the linear polarization data reveals that the synthetic zinc materials using organic additives all exhibit 6-30 times lower corrosion currents. When using Zn-SDS as the anode in the rechargeable hybrid aqueous battery, the float current decreases as much as 2.5 times. The batteries with Zn-SDS, Zn-PEG, and Zn-TU anodes display the capacity retention of 79%, 76%, and 80% after 1000 cycles of…

Robust, stretchable, and strain-sensitive hydrogels have recently attracted immense research interest because of their potential application in wearable strain sensors. The integration of the synergistic characteristics of decent mechanical properties, reliable self-healing capability, and high sensing sensitivity for fabricating conductive, elastic, self-healing, and strain-sensitive hydrogels is still a great challenge. Inspired by the mechanically excellent and self-healing biological soft tissues with hierarchical network structures, herein, functional network hydrogels are fabricated by the interconnection between a “soft” homogeneous polymer network and a “hard” dynamic ferric (Fe 3+ ) cross-linked cellulose nanocrystals (CNCs–Fe 3+ ) network. Under stress, the dynamic CNCs–Fe 3+ coordination bonds act as sacrificial bonds to efficiently dissipate energy, while the homogeneous polymer network leads to a smooth stress-transfer, which enables the hydrogels to achieve unusual mechanical properties, such as excellent mechanical strength, robust toughness, and stretchability, as…

All-solid-state lithium-ion batteries have the potential to become an important class of next-generation electrochemical energy storage devices. However, for achieving competitive performance, a better understanding of the interfacial processes at the electrodes is necessary for optimized electrode compositions to be developed. In this work, the interfacial processes between the solid electrolyte (Li 10 GeP 2 S 12 ) and the electrode materials (In/InLi and Li x CoO 2 ) are monitored using impedance spectroscopy and galvanostatic cycling, showing a large resistance contribution and kinetic hindrance at the metal anode. The effect of different fractions of the solid electrolyte in the composite cathodes on the rate performance is tested. The results demonstrate the necessity of a carefully designed composite microstructure depending on the desired applications of an all-solid-state battery. While a relatively low mass fraction of solid electrolyte is sufficient for high energy density, a higher fraction of solid electrolyte is required for high power density.

Herein, we studied the adsorption behaviors of organic micropollutants, such as anticonvulsant carbamazepine (CBZ) and antibiotic tetracycline hydrochloride (TC), on zirconium metal–organic framework UiO-66 in water. The maximum adsorption capacities of CBZ and TC on the UiO-66 were 37.2 and 23.1 mg·g –1 at 25 °C, respectively. The adsorption isotherms and kinetics of CBZ and TC were well described by using the Langmuir model and pseudo-second-order model, respectively, and the adsorptions on UiO-66 are endothermic reactions. The adsorption capacities of CBZ and TC on UiO-66 were decreased with the increase of solution pH. The presence of humic acid could improve the adsorption of CBZ and TC on UiO-66, but K + ion inhibited their adsorption obviously. In addition, Ca 2+ and Al 3+ ions also suppressed the adsorption of TC on UiO-66. The competitive adsorption suggested that the adsorption sites for CBZ on UiO-66 were different from those for TC. The surface interactions between UiO-66 and the two micropollutants were demonstrated by powder X-ray diffraction, Fourier transform…

Colorimetric and fluorescent dual mode detection methods have gained much attention in recent years; however, it is still desirable to develop new colorimetric and fluorescent dual mode nanosensors with more simple preparation procedures, low cost, and excellent biocompatibility. Herein, a colorimetric and fluorescent nanosensor based on B, N, S- co -doped carbon dots (BNS-CDs) was synthesized by one-step hydrothermal treatment of 2,5-diaminobenzenesulfonic acid and 4-aminophenylboronic acid hydrochloride. Using this nanosensor, a highly sensitive assay of Fe 3+ in the range of 0.3–546 μM with a detection limit of 90 nM was provided by quenching the red emission fluorescence. It is more attractive that Fe 3+ can also be visualized by this nanosensor via evident color changes of the solution (from red to blue) under sunlight without the aid of an ultraviolet (UV) lamp. Furthermore, the designed nanosensor can be applied for efficient detection of intracellular Fe 3+ with excellent biocompatibility and cellular imaging capability, and it holds great promise in biomedical applications.

Aqueous zinc-ion batteries attract increasing attention due to their low cost, high safety, and potential application in stationary energy storage. However, the simultaneous realization of high cycling stability and high energy density remains a major challenge. To tackle the above-mentioned challenge, we develop a novel Zn/V 2 O 5 rechargeable aqueous hybrid-ion battery system by using porous V 2 O 5 as the cathode and metallic zinc as the anode. The V 2 O 5 cathode delivers a high discharge capacity of 238 mAh g –1 at 50 mA g –1 . 80% of the initial discharge capacity can be retained after 2000 cycles at a high current density of 2000 mA g –1 . Meanwhile, the application of a “water-in-salt” electrolyte results in the increase of discharge platform from 0.6 to 1.0 V. This work provides an effective strategy to simultaneously enhance the energy density and cycling stability of aqueous zinc ion-based batteries.

Three-dimensional structures capable of reversible changes in shape, i.e., four-dimensional-printed structures, may enable new generations of soft robotics, implantable medical devices, and consumer products. Here, thermally responsive liquid crystal elastomers (LCEs) are direct-write printed into 3D structures with a controlled molecular order. Molecular order is locally programmed by controlling the print path used to build the 3D object, and this order controls the stimulus response. Each aligned LCE filament undergoes 40% reversible contraction along the print direction on heating. By printing objects with controlled geometry and stimulus response, magnified shape transformations, for example, volumetric contractions or rapid, repetitive snap-through transitions, are realized.

In this work, we report a fabrication of epoxy resin/ordered three-dimensional boron nitride (3D-BN) network composites through combination of ice-templating self-assembly and infiltration methods. The polymer composites possess much higher thermal conductivity up to 4.42 W m –1 K –1 at relatively low loading 34 vol % than that of random distribution composites (1.81 W m –1 K –1 for epoxy/random 3D-BN composites, 1.16 W m –1 K –1 for epoxy/random BN composites) and exhibit a high glass transition temperature (178.9–229.2 °C) and dimensional stability (22.7 ppm/K). We attribute the increased thermal conductivity to the unique oriented 3D-BN thermally conducive network, in which the much higher thermal conductivity along the in-plane direction of BN microplatelets is most useful. This study paves the way for thermally conductive polymer composites used as thermal interface materials for next-generation electronic packaging and 3D integration circuits.

In this work, mesoporous carbon hollow microspheres (PCHMs) with designable mesoporous shell and interior void are constructed by a facile in situ stöber templating approach and a pyrolysis-etching process. The PCHMs are characterized by scanning electron microscopy, transmission electron microscopy, X-ray photoelectron spectra, Raman spectroscopy, and nitrogen adsorption and desorption system. A uniform mesoporous shell (pore size 4.7 nm) with a thickness of 55 nm and a cavity size of 345 nm is realized. The composite of paraffin mixed with 20 wt % PCHMs exhibits a minimum reflection coefficient (RC min ) of −84 dB at 8.2 GHz with a sample thickness of 3.9 mm and an effective absorption bandwidth (EAB) of 4.8 GHz below −10 dB (>90% electromagnetic wave is attenuated). Moreover, the composite of phenolic resin mixed with 20 wt % PCHMs exhibits an ultrawide EAB of 8 GHz below −10 dB with a thinner thickness of 2.15 mm. Such excellent electromagnetic wave absorption properties are ascribed to the large carbon–air interface in the mesoporous shell and interior void, which is favorable…

It is highly desirable and a great challenge for red light emission of carbon dots under long wavelength excitation. Here, we developed a facile route to synthesize carbon dots with red emission due to the doping effect of S and N elements, borrowing from the concept of the semiconductor. The maximum emission locates at 594 nm under 560 nm excitation. The absolute photoluminescence (PL) quantum yield (QY) is as high as 29% and 22% in ethanol and water, respectively. XPS and FTIR spectra illustrated that there exist -SCN and -COOH groups on the surface of the carbon dots. They endow the carbon dots with high sensitivity for ion detection of Fe 3+ . The quenched PL emission of Fe 3+ -S,N-CDs can be recovered by adding ascorbic acid to release the -COOH and -SCN group due to Fe 2+ formation in the presence of ascorbic acid. High PL QY of red emission is beneficial to application in bioimaging. Doxorubicin was loaded onto carbon dots through π–π stacking to form a theranostic agent. When the CD-Dox was injected into the tumor site, a strong PL emission was observed. The PL intensity…

In this work, two novel flowerlike NiO hierarchical structures, rose-flower (S1) and silk-flower (S2), were synthesized by using a facial hydrothermal method, coupled with subsequent postannealing process. Structures, morphologies, and magnetic and electromagnetic properties of two NiO structures have been systematically investigated. SEM and TEM results suggested that S1 had a hierarchical rose-flower architecture with diameters in the range of 4–7 μm, whereas S2 exhibited a porous silk-flower architecture with diameters of 0.7–1.0 μm. Electromagnetic performances indicated that the NiO hierarchical structures played a crucial role in determining their dielectric behavior and impedance matching characteristic, which further influenced the microwave attenuation property of absorbers based on them. Due to its hierarchical and porous architectures, S2 had higher microwave absorption performances than S1. The maximum R L value for sample S2 can reach −65.1 dB at 13.9 GHz, while an efficient bandwidth of 3 GHz was obtained. In addition, the mechanism of the improved microwave absorption…

Dynamic noncovalent interactions with reversible nature are critical for the integral synthesis of self-healing biological materials. In this work, we developed a simple one-pot strategy to prepare a fully physically cross-linked nanocomposite hydrogel through the formation of the hydrogen bonds and dual metal-carboxylate coordination bonds within supramolecular networks, in which iron ions (Fe 3+ ) and TEMPO oxidized cellulose nanofibrils (CNFs) acted as cross-linkers and led to the improved mechanical strength, toughness, time-dependent self-recovery capability and self-healing property. The spectroscopic analysis and rheological measurements corroborated the existence of hydrogen bonds and dual coordination bonds. The mechanical tests and microscopic morphology were explored to elucidate the recovery properties and toughening mechanisms. The hydrogen bonds tend to preferentially break prior to the coordination bonds associated complexes that act as skeleton to maintain primary structure integrity, and the survived coordination bonds with dynamic feature also serve as sacrificial…

In this study, we introduced a targeting polymer poly(ethylene glycol)–folic acid (PEG–FA) on the surface of polydopamine (PDA)-modified mesoporous silica nanoparticles (MSNs) to develop the novel nanoparticles (NPs) MSNs@PDA–PEG–FA, which were employed as a drug delivery system loaded with doxorubicin (DOX) as a model drug for cervical cancer therapy. The chemical structure and properties of these NPs were characterized by transmission electron microscopy, X-ray photoelectron spectroscopy, N 2 adsorption/desorption, dynamic light scattering-autosizer, thermogravimetric analysis, and Fourier transform infrared spectroscopy. The pH-sensitive PDA coating served as a gatekeeper. The in vitro drug release experiments showed pH-dependent and sustained drug release profiles that could enhance the therapeutic anticancer effect and minimize potential damage to normal cells due to the acidic microenvironment of the tumor. These MSNs@PDA–PEG–FA achieved significantly high targeting efficiency, which was demonstrated by the in vitro cellular uptake and cellular targeting assay. Compared with…

A new method based on one-step solvothermal reaction is demonstrated to synthesize ultrathin Ni–Co layered double hydroxide (LDH) nanosheets, which grow directly on a flexible carbon fiber cloth (NiCo-LDH/CFC). Through using 2-methylimidazole as complex and methanol as solvent, the as-prepared NiCo-LDH/CFC shows a (003) facet preferential growth and an expanded interlayer spacing structure, resulting in a unique 3D porous nanostructure with a thickness of nanosheets of around 5–7 nm that shows high energy storage performance. By controlling the ratio of Ni/Co = 4:1 in the precursor solution, the electrode shows a specific capacitance of 2762.7 F g –1 (1243.2 C g –1 ) at a current density of 1 A g –1 . Nevertheless, the optimal composition is obtained with Ni/Co = 1:1, which produces a specific capacitance of 2242.9 F g –1 (1009.3 C g –1 ) at 1 A g –1 and shows an excellent rate capability with 61% of the original capacitance being retained at a current density of 60 A g –1 . The hybrid supercapacitor (HSC) based on the NiCo-LDH/CFC exhibits a maximum energy density of 59.2 Wh kg –1…

Metal–organic frameworks (MOFs) with high porosity and a regular porous structure have emerged as a promising electrode material for supercapacitors, but their poor electrical conductivity limits their utilization efficiency and capacitive performance. To increase the overall electrical conductivity as well as the efficiency of MOF particles, three-dimensional networked MOFs are developed via using preprepared conductive polypyrrole (PPy) tubes as the support for in situ growth of MOF particles. As a result, the highly conductive PPy tubes that run through the MOF particles not only increase the electron transfer between MOF particles and maintain the high effective porosity of the MOFs but also endow the MOFs with flexibility. Promoted by such elaborately designed MOF–PPy networks, the specific capacitance of MOF particles has been increased from 99.2 F g –1 for pristine zeolitic imidazolate framework (ZIF)-67 to 597.6 F g –1 for ZIF–PPy networks, indicating the importance of the design of the ZIF–PPy continuous microstructure. Furthermore, a flexible supercapacitor device based on…

On the basis of the thermoreversible sol-gel transition behavior of κ-carrageenan in water, a double-network (DN) hydrogel has been fabricated by combining an ionically cross-linked κ-carrageenan network with a covalently cross-linked polyacrylamide (PAAm) network. The κ-carrageenan/PAAm DN hydrogel demonstrated an excellent recoverability and significant self-healing capability (even when notched). More importantly, the warm pregel solution of κ-carrageenan/AAm can be used as an ink of a three-dimensional (3D) printer to print complex 3D structures with remarkable mechanical strength after UV exposure. Furthermore, the κ-carrageenan/PAAm DN hydrogel exhibited a great strain sensitivity with a gauge factor of 0.63 at the strain of 1000%, and thus, the hydrogel can be used as sensitive strain sensors for applications in robotics and human motion detection.

Stretchable and flexible sensors attached onto the surface of the human body can perceive external stimuli, thus attracting extensive attention due to their lightweight, low modulus, low cost, high flexibility, and stretchability. Recently, a myriad of efforts have been devoted to improving the performance and functionality of wearable sensors. Herein, this review focuses on recent remarkable advancements in the development of flexible and stretchable sensors. Multifunction of these wearable sensors is realized by incorporating some desired features (e.g., self-healing, self-powering, linearity, and printing). Next, focusing on the characteristics of carbon nanomaterials, nanostructured metal, conductive polymer, or their hybrid composites, two major strategies (e.g., materials that stretch and structures that stretch) and diverse design approaches have been developed to achieve highly flexible and stretchable electrodes. Strain sensing performances of recently reported sensors indicate that the appropriate choice of geometric engineering as well as intrinsically stretchable…

perovskite nanocrystals (CPB-NCs) often quickly changes to yellow, followed by large photoluminescence (PL) loss. To figure out what is happening on CPB-NCs during the color change process, the morphology, structure, and PL evolutions are systematically investigated by varying the influence factors of illumination, moisture, oxygen, and temperature. We find that the yellow color is mainly originated from the large CPB crystals formed in the illumination process. With maximized isolation of oxygen for the sandwiched film or the uncovered film stored in nitrogen, the color change can be dramatically slowed down whether there is water vapor or not. Under dark condition, the PL emissions are not significantly influenced by the varied relative humidity (RH) levels and temperatures up to 60 °C. Under the precondition of oxygen or air, color change and PL loss become more obvious when increasing the illumination power or RH level, and the large-sized cubic CPB crystals are further evolved into the oval-shaped crystals. We confirm that oxygen is the crucial factor to drive the color change,…

Composite polymer solid electrolytes (CPEs) containing ceramic fillers embedded inside a polymer-salt matrix show great improvements in Li + ionic conductivity compared to the polymer electrolyte alone. Lithium lanthanum zirconate (Li 7 La 3 Zr 2 O 12, LLZO) with a garnet-type crystal structure is a promising solid Li + conductor. We show that by incorporating only 5 wt % of the ceramic filler comprising undoped, cubic-phase LLZO nanowires prepared by electrospinning, the room temperature ionic conductivity of a polyacrylonitrile-LiClO 4 -based composite is increased 3 orders of magnitude to 1.31 × 10 –4 S/cm. Al-doped and Ta-doped LLZO nanowires are also synthesized and utilized as fillers, but the conductivity enhancement is similar as for the undoped LLZO nanowires. Solid-state nuclear magnetic resonance (NMR) studies show that LLZO NWs partially modify the PAN polymer matrix and create preferential pathways for Li + conduction through the modified polymer regions. CPEs with LLZO nanoparticles and Al 2 O 3 nanowire fillers are also studied to elucidate the role of filler type…

Metal–organic frameworks are a class of attractive materials for fluorescent sensing. Improvement of hydrolytic stability, sensitivity, and selectivity of function is the key to advance application of fluorescent MOFs in aqueous media. In this work, two stable MOFs, [Zr 6 O 4 (OH) 8 (H 2 O) 4 (L 1 ) 2 ] (BUT-14) and [Zr 6 O 4 (OH) 8 (H 2 O) 4 (L 2 ) 2 ] (BUT-15), were designed and synthesized for the detection of metal ions in water. Two new ligands utilized for construction of the MOFs, namely, 5′,5‴-bis(4-carboxyphenyl)-[1,1′:3′,1″:4″,1‴:3‴,1′′′′-quinquephenyl]-4,4′′′′-dicarboxylate (L 1 ) and 4,4′,4″,4‴-(4,4′-(1,4-phenylene)bis(pyridine-6,4,2-triyl))tetrabenzoate (L 2 ), are structurally similar with the only difference being that the latter is functionalized by pyridine N atoms. The two MOFs are isostructural with a sqc - a topological framework structure, and highly porous with the Brunauer–Emmett–Teller (BET) surface areas of 3595 and 3590 m 2 g –1, respectively. Interestingly, they show intense fluorescence in water, which can be solely quenched by trace amounts of Fe 3+…

The formation of lithium dendrites is suppressed using a Li 1.5 Al 0.5 Ge 1.5 (PO 4 ) 3 –poly(ethylene oxide) (LAGP-PEO) composite solid electrolyte and a PEO (lithium bis(trifluoromethane)sulfonimide) [PEO (LiTFSI)]-modified lithium metal anode in all-solid-state lithium batteries. The effects on the anode performance based on the PEO content in the composite solid electrolyte and the molecular weight of PEO used to modify the Li anode are studied. The structure, surface morphology, and stability of the composite solid electrolyte are examined by X-ray diffraction spectroscopy, scanning electron microscopy, and electrochemical tests. Results show that the presence of a PEO-500000(LiTFSI) film on a Li anode results in good mechanical properties and satisfactory interface contact features. The film can also prevent Li from reacting with LAGP. Furthermore, the formation of lithium dendrites can be effectively inhibited as the composite solid electrolyte is combined with the PEO film on the Li anode. The ratio of PEO in the composite solid electrolyte can be reduced to a low level of 1…

Nanotextured surfaces (NTSs) are critical to organisms as self-adaptation and survival tools. These NTSs have been actively mimicked in the process of developing bactericidal surfaces for diverse biomedical and hygiene applications. To design and fabricate bactericidal topographies effectively for various applications, understanding the bactericidal mechanism of NTS in nature is essential. The current mechanistic explanations on natural bactericidal activity of nanopillars have not utilized recent advances in microscopy to study the natural interaction. This research reveals the natural bactericidal interaction between E. coli and a dragonfly wing's (Orthetrum villosovittatum) NTS using advanced microscopy techniques and proposes a model. Contrary to the existing mechanistic models, this experimental approach demonstrated that the NTS of Orthetrum villosovittatum dragonfly wings has two prominent nanopillar populations and the resolved interface shows membrane damage occurred without direct contact of the bacterial cell membrane with the nanopillars. We propose that the bacterial…

The global fresh water shortage has driven enormous endeavors in seawater desalination and wastewater purification; among these, solar steam generation is effective in extracting fresh water by efficient utilization of naturally abundant solar energy. For solar steam generation, the primary focus is to design new materials that are biodegradable, sustainable, of low cost, and have high solar steam generation efficiency. Here, we designed a bilayer aerogel structure employing naturally abundant cellulose nanofibrils (CNFs) as basic building blocks to achieve sustainability and biodegradability as well as employing a carbon nanotube (CNT) layer for efficient solar utilization with over 97.5% of light absorbance from 300 to 1200 nm wavelength. The ultralow density (0.0096 g/cm 3 ) of the aerogel ensures that minimal material is required, reducing the production cost while at the same time satisfying the water transport and thermal-insulation requirements due to its highly porous structure (99.4% porosity). Owing to its rationally designed structure and thermal-regulation performance,…

Phytic acid, which is a naturally occurring component that is widely found in many plants, can strongly bond toxic mineral elements in the human body, because of its six phosphate groups. Some of the metal ions present the property of bonding with phytic acid to form insoluble coordination complexes aggregations, even at room temperature. Herein, a superhydrophobic cotton fabric was prepared using a novel and facile nature-inspired strategy that introduced phytic acid metal complex aggregations to generate rough hierarchical structures on a fabric surface, followed by PDMS modification. This superhydrophobic surface can be constructed not only on cotton fabric, but also on filter paper, polyethylene terephthalate (PET) fabric, and sponge. Ag I, Fe III, Ce III, Zr IV, and Sn IV are very commendatory ions in our study. Taking phytic acid–Fe III -based superhydrophobic fabric as an example, it showed excellent resistance to ultraviolet (UV) irradiation, high temperature, and organic solvent immersion, and it has good resistance to mechanical wear and abrasion. The…

Batteries and electrochemical double layer charging capacitors are two classical means of storing electrical energy. These two types of charge storage can be unambiguously distinguished from one another by the shape and scan-rate dependence of their cyclic voltammetric (CV) current–potential responses. The former shows peak-shaped current–potential responses, proportional to the scan rate v or to v 1/2, whereas the latter displays a quasi-rectangular response proportional to the scan rate. On the contrary, the notion of pseudocapacitance, popularized in the 1980s and 1990s for metal oxide systems, has been used to describe a charge storage process that is faradaic in nature yet displays capacitive CV signatures. It has been speculated that a quasi-rectangular CV response resembling that of a truly capacitive response arises from a series of faradaic redox couples with a distribution of potentials, yet this idea has never been justified theoretically. We address this problem by first showing theoretically that this distribution-of-potentials approach is closely equivalent to the more…

Abstract All-solid-state batteries (SSBs) have recently attracted much attention due to their potential application in electric vehicles. One key issue that is central to improve the function of SSBs is to gain a better understanding of the interfaces between the material components toward enhancing the electrochemical performance. In this work, the interfacial properties of a carbon-containing cathode composite, employing Li10GeP2S12 as the solid electrolyte, are investigated. A large interfacial charge-transfer resistance builds up upon the inclusion of carbon in the composite, which is detrimental to the resulting cycle life. Analysis by X-ray photoelectron spectroscopy reveals that carbon facilitates faster electrochemical decomposition of the thiophosphate solid electrolyte at the cathode/solid electrolyte interfaceby transferring the low chemical potential of lithium in the charged state deeper into the solid electrolyte and extending the decomposition region. The occurring accumulation of highly oxidized sulfur species at the interface is likely responsible for the large…

Luminescent bioprobes are powerful analytical means for biosensing and optical imaging. Luminogens featured with aggregation-induced emission (AIE) attributes have emerged as ideal building blocks for high-performance bioprobes. Bioprobes constructed with AIE luminogens have been identified to be a novel class of FL light-up probing tools. In contrast to conventional bioprobes based on the luminophores with aggregation-caused quenching (ACQ) effect, the AIE-based bioprobes enjoy diverse superiorities, such as lower background, higher signal-to-noise ratio and sensitivity, better accuracy, and more outstanding resistance to photobleaching. AIE-based bioprobes have been tailored for a vast variety of purposes ranging from biospecies sensing to bioimaging to theranostics (i.e., image-guided therapies). In this review, recent five years' advances in AIE-based bioprobes are briefly overviewed in a perspective distinct from other reviews, focusing on the most appealing trends and progresses in this flourishing research field. There are altogether 11 trends outlined, which have been…

The attachment and subsequent colonization of bacteria on the surfaces of synthetic materials and devices lead to serious problems in both human healthcare and industrial applications. Therefore, antibacterial surfaces that can prevent bacterial attachment and biofilm formation have been a long-standing focus of considerable interest and research efforts. Recently, a promising "kill-release" strategy has been proposed and applied to construct so-called smart antibacterial surfaces, which can kill bacteria attached to their surface and then undergo on-demand release of the dead bacteria and other debris to reveal a clean surface under an appropriate stimulus, thereby maintaining effective long-term antibacterial activity. This Review focuses on the recent progress (particularly over the past 5 years) on such smart antibacterial surfaces. According to the different design strategies, these surfaces can be divided into three categories: (i) "K + R"-type surfaces, which have both a killing unit and a releasing unit; (ii) "K → R"-type surfaces, which have a surface-immobilized killing…

Three-dimensional (3D) flexible foams consisting of reduced graphene oxides (rGO) and in situ grown SiC nanowires (NWs) were prepared using freeze-drying and carbothermal reduction processes. By means of incorporating SiC nanowires into rGO foams, both the thermostability and electromagnetic absorption of the composites were improved. It was demonstrated that rGO/SiC NW foams were thermostable beyond ∼630 °C (90% weight retention in air atmosphere). As expected, rGO/SiC NW foams in the poly(dimethylsiloxane) matrix achieved effective absorption in the entire X-band (8.2-12.4 GHz) with a thinner thickness (3 mm) in comparison with those of the pure rGO foams. It is revealed that SiC nanowires with abundant stacking faults, twinning interfaces, and bridged junctions play an important role in the enhanced electromagnetic absorption performance, in addition to the contribution of interconnected graphene networks. Hierarchical rGO/SiC NW foams not only are efficient absorbers in the critical environments but also can be applied in photocatalytic and thermal-management fields.

Phosphorus-doped graphitic carbon nitrides (P-g-C 3 N 4 ) have recently emerged as promising visible-light photocatalysts for both hydrogen generation and clean environment applications because of fast charge carrier transfer and increased light absorption. However, their photocatalytic performances on CO 2 reduction have gained little attention. In this work, phosphorus-doped g-C 3 N 4 nanotubes are synthesized through the one-step thermal reaction of melamine and sodium hypophosphite monohydrate (NaH 2 PO 2 ·H 2 O). The phosphine gas generated from the thermal decomposition of NaH 2 PO 2 ·H 2 O induces the formation of P-g-C 3 N 4 nanotubes from g-C 3 N 4 nanosheets, leads to an enlarged BET surface area and a unique mesoporous structure, and creates an amino-rich surface. The interstitial doping phosphorus also down shifts the conduction and valence band positions and narrows the band gap of g-C 3 N 4 . The photocatalytic activities are dramatically enhanced in the reduction both of CO 2 to produce CO and CH 4 and of water to produce H 2 because of the efficient suppression of…

Microwave absorbers with layered structures that can provide abundant interfaces are highly desirable for enhancing electromagnetic absorbing capability and decreasing the thickness. The atomically thin layers of two-dimensional (2D) transition-metal carbides (MXenes) make them a convenient precursor for synthesis of other 2D and layered structures. Here, laminated carbon/TiO 2 hybrid materials composed of well-aligned 2D carbon sheets with embedded TiO 2 nanoparticles were synthesized and showed excellent microwave absorption. Disordered 2D carbon layers with an unusual structure were obtained by annealing multilayer Ti 3 C 2 MXene in a CO 2 atmosphere. The minimum reflection coefficient of laminated carbon/TiO 2 composites reaches −36 dB, and the effective absorption bandwidth ranges from 3.6 to 18 GHz with the tunable thickness from 1.7 to 5 mm. The effective absorption bandwidth covers the whole Ku band (12.4–18 GHz) when the thickness of carbon/TiO 2 /paraffin composite is 1.7 mm. This study is expected to pave the way to the synthesis of carbon-supported absorbing materials…

All-solid-state batteries including a garnet ceramic as electrolyte are potential candidates to replace the currently used Li-ion technology, as they offer safer operation and higher energy storage performances. However, the development of ceramic electrolyte batteries faces several challenges at the electrode/electrolyte interfaces, which need to withstand high current densities to enable competing C-rates. In this work, we investigate the limits of the anode/electrolyte interface in a full cell that includes a Li-metal anode, LiFePO 4 cathode, and garnet ceramic electrolyte. The addition of a liquid interfacial layer between the cathode and the ceramic electrolyte is found to be a prerequisite to achieve low interfacial resistance and to enable full use of the active material contained in the porous electrode. Reproducible and constant discharge capacities are extracted from the cathode active material during the first 20 cycles, revealing high efficiency of the garnet as electrolyte and the interfaces, but prolonged cycling leads to abrupt cell failure. By using a combination of…

Zirconiumv (IV)-carboxylate metal-organic framework (MOF) UiO-66 nanoparticles were successfully synthesized and incorporated in the polyamide (PA) selective layer to fabricate novel thin-film nanocomposite (TFN) membranes. Compared to unmodified pure polyamide thin-film composite (TFC) membranes, the incorporation of UiO-66 nanoparticles significantly changes the membrane morphology and chemistry, leading to an improvement of intrinsic separation properties due to the molecular sieving and superhydrophilic nature of UiO-66 particles. The best performing TFN-U2 (0.1 wt % particle loading) membrane not only shows a 52% increase of water permeability but also maintains salt rejection levels (∼95%) similar to the benchmark. The effects of UiO-66 loading on the forward osmosis (FO) performance were also investigated. Incorporation of 0.1 wt % UiO-66 produced a maximum water flux increase of 40% and 25% over the TFC control under PRO and FO modes, when 1 M NaCl was used as the draw solution against deionized water feed. Meanwhile, solute reverse flux was maintained at a relatively low…

The continuous evolution toward semiconductor technology in the "more-than-Moore" era and rapidly increasing power density of modern electronic devices call for advanced thermal interface materials (TIMs). Here, we report a novel strategy to construct flexible polymer nanocomposite TIMs for advanced thermal management applications. First, aligned polyvinyl alcohol (PVA) supported and interconnected 2D boron nitride nanosheets (BNNSs) composite fiber membranes were fabricated by electrospinning. Then, the nanocomposite TIMs were constructed by rolling the PVA/BNNS composite fiber membranes to form cylinders and subsequently vacuum-assisted impregnation of polydimethylsiloxane (PDMS) into the porous cylinders. The nanocomposite TIMs not only exhibit a superhigh through-plane thermal conductivity enhancement of about 10 times at a low BNNS loading of 15.6 vol % in comparison with the pristine PDMS but also show excellent electrical insulating property (i.e., high volume electrical resistivity). The outstanding thermal management capability of the nanocomposite TIMs was practically…

The construction of exceptionally robust and high-quality semiconductor–cocatalyst heterojunctions remains a grand challenge toward highly efficient and durable solar-to-fuel conversion. Herein, novel graphitic carbon nitride (g-C 3 N 4 ) nanosheets decorated with multifunctional metallic Ni interface layers and amorphous NiS cocatalysts were fabricated via a facile three-step process: the loading of Ni(OH) 2 nanosheets, high-temperature H 2 reduction, and further deposition of amorphous NiS nanosheets. The results demonstrated that both robust metallic Ni interface layers and amorphous NiS can be utilized as electron cocatalysts to markedly boost the visible-light H 2 evolution over g-C 3 N 4 semiconductor. The optimized g-C 3 N 4 -based photocatalyst containing 0.5 wt % Ni and 1.0 wt % NiS presented the highest hydrogen evolution of 515 μmol g –1 h –1, which was about 2.8 and 4.6 times as much as those obtained on binary g-C 3 N 4 -1.0%NiS and g-C 3 N 4 -0.5%Ni, respectively. Apparently, the metallic Ni interface layers play multifunctional roles in enhancing the visible-light H 2…

Three-dimensional (3D) printing is an emerging approach for rapid fabrication of complex tissue structures using cell-loaded bioinks. However, 3D bioprinting has hit a bottleneck in progress because of the lack of suitable bioinks that are printable, have high shape fidelity, and are mechanically resilient. In this study, we introduce a new family of nanoengineered bioinks consisting of kappa-carrageenan (κCA) and two-dimensional (2D) nanosilicates (nSi). κCA is a biocompatible, linear, sulfated polysaccharide derived from red algae and can undergo thermo-reversible and ionic gelation. The shear-thinning characteristics of κCA were tailored by nanosilicates to develop a printable bioink. By tuning κCA-nanosilicate ratios, the thermo-reversible gelation of the bioink can be controlled to obtain high printability and shape retention characteristics. The unique aspect of the nanoengineered κCA-nSi bioink is its ability to print physiologically-relevant-scale tissue constructs without requiring secondary supports. We envision that nanoengineered κCA-nanosilicate bioinks can be used to…

The development of pressure sensors that are effective over a broad range of pressures is crucial for the future development of electronic skin applicable to the detection of a wide pressure range from acoustic wave to dynamic human motion. Here, we present flexible capacitive pressure sensors that incorporate micropatterned pyramidal ionic gels to enable ultrasensitive pressure detection. Our devices show superior pressure-sensing performance, with a broad sensing range from a few pascals up to 50 kPa, with fast response times of <20 ms and a low operating voltage of 0.25 V. Since high-dielectric-constant ionic gels were employed as constituent sensing materials, an unprecedented sensitivity of 41 kPa –1 in the low-pressure regime of <400 Pa could be realized in the context of a metal–insulator–metal platform. This broad-range capacitive pressure sensor allows for the efficient detection of pressure from a variety of sources, including sound waves, a lightweight object, jugular venous pulses, radial artery pulses, and human finger touch. This platform offers a simple, robust…

Lead-free dielectric ceramics with high recoverable energy density are highly desired to sustainably meet the future energy demand. AgNbO 3 -based lead-free antiferroelectric ceramics with double ferroelectric hysteresis loops have been proved to be potential candidates for energy storage applications. Enhanced energy storage performance with recoverable energy density of 3.3 J/cm 3 and high thermal stability with minimal energy density variation (<10%) over a temperature range of 20–120 °C have been achieved in W-modified AgNbO 3 ceramics. It is revealed that the W 6+ cations substitute the B-site Nb 5+ and reduce the polarizability of B-site cations, leading to the enhanced antiferroelectricity, which is confirmed by the polarization hysteresis and dielectric tunability. It is believed that the polarizability of B-site cations plays a dominant role in stabilizing the antiferroelectricity in AgNbO 3 system, in addition to the tolerance factor, which opens up a new design approach to achieve stable antiferroelectric materials.

Graphene oxide quantum dots (GOQDs), novel carbon-based nanomaterials, have attracted tremendous research interest due to their unique properties associated with both graphene and quantum dots. In the present study, thin film nanocomposite (TFN) membranes comprising GOQDs dispersed within a tannic acid (TA) film were fabricated by an interfacial polymerization reaction for low-pressure nanofiltration (NF). The resultant TA/GOQDs TFN membranes had measurably smoother and more hydrophilic, negatively charged surfaces compared to the similarly formed TA thin film composite (TFC) membrane. Owing to the loose active layer structure and the combination of Donnan exclusion and steric hindrance, the TA/GOQDs TFN membrane showed a pure water flux up to 23.33 L/m 2 ·h (0.2 MPa), which was 1.5 times more than that of pristine TA TFC membrane, while high dye rejection to Congo red (99.8%) and methylene blue (97.6%) was kept. In addition, the TA/GOQDs TFN membrane presented better antifouling properties, which was ascribed to the favorable changes in membrane hydrophilicity, ζ-potential, and…

pH and glucose dual-responsive injectable hydrogels were prepared through the cross-linking of Schiff's base and phenylboronate ester using phenylboronic-modified chitosan, poly(vinyl alcohol) and benzaldehyde-capped poly(ethylene glycol). Protein drugs and live cells could be incorporated into the hydrogels during the in situ cross-linking, displaying sustained and pH/glucose-triggered drug release from the hydrogels and cell viability and proliferation in the three-dimensional hydrogel matrix as well. Hence, the hydrogels with insulin and fibroblasts were considered as bioactive dressings for diabetic wound healing. A streptozotocin-induced diabetic rat model was used to evaluate the efficacy of hydrogel dressings in wound repair. The results revealed that the incorporation of insulin and L929 in the hydrogels could promote neovascularization and collagen deposition and enhance the wound-healing process of diabetic wounds. Thus, the drug- and cell-loaded hydrogels have promising potential in wound healing as a medicated system for various therapeutic proteins and live cells.

Ni-rich materials are appealing to replace LiCoO 2 as cathodes in Li-ion batteries due to their low cost and high capacity. However, there are also some disadvantages for Ni-rich cathode materials such as poor cycling and rate performance, especially under high voltage. Here, we demonstrate the effect of dual-conductive layers composed of Li 3 PO 4 and PPy for layered Ni-rich cathode material. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy show that the coating layers are composed of Li 3 PO 4 and PPy. (NH 4 ) 2 HPO 4 transformed to Li 3 PO 4 after reacting with surface lithium residuals and formed an inhomogeneous coating layer which would remarkably improve the ionic conductivity of the cathode materials and reduce the generation of HF. The PPy layer could form a uniform film which can make up for the Li 3 PO 4 coating defects and enhance the electronic conductivity. The stretchy PPy capsule shell can reduce the generation of internal cracks by resisting the internal pressure as well. Thus, ionic and electronic conductivity, as well as surface…

Large-scale core–sheath heterostructural SiC nanowires were facilely grown on the surface of carbon fibers using a one-step chemical vapor infiltration process. The as-synthesized SiC nanowires consist of single crystalline SiC cores with a diameter of ∼30 nm and polycrystalline SiC sheaths with an average thickness of ∼60 nm. The formation mechanisms of core–sheath heterostructural SiC nanowires (SiC nws ) were discussed in detail. The SiC nws -CF shows strong electromagnetic (EM) wave absorption performance with a maximum reflection loss value of −45.98 dB at 4.4 GHz. Moreover, being coated with conductive polymer polypyrrole (PPy) by a simple chemical polymerization method, the SiC nws -CF/PPy nanocomposites exhibited superior EM absorption abilities with maximum RL value of −50.19 dB at 14.2 GHz and the effective bandwidth of 6.2 GHz. The SiC nws -CF/PPy nanocomposites in this study are very promising as absorber materials with strong electromagnetic wave absorption performance.

Design of an interface to arouse interface polarization is an efficient route to attenuate high-frequency electromagnetic waves. The attenuation intensity is highly related to the contact area. To achieve stronger interface polarization, growing metal oxide granular film on graphene with a larger surface area seems to be an efficient strategy due to the high charge carrier concentration of graphene. This study is devoted to fabricating the filmlike composite by a facile thermal decomposition method and investigating the relationship among contact area, polarization intensity, and the type of metal oxide. Because of the high-frequency polarization effect, the composites presented excellent electromagnetic wave attenuation ability. It is shown that the optimal effective frequency bandwidth of graphene/metal oxide was close to 7.0 GHz at a thin coating layer of 2.0 mm. The corresponding reflection loss value was nearly -22.1 dB. Considering the attenuation mechanism, interface polarization may play a key role in the microwave-absorbing ability.

Red emissive carbon dots (CDs) have drawn more and more attention due to their good organ penetration depth and slight biological tissue photodamage. Herein, the fluorescent CDs with red emission were synthesized by the facile one-pot hydrothermal treatment of citric acid and neutral red and they show red fluorescence both in aqueous solution and solid state. The solution of CDs exhibits the quantum yield of 12.1%, good stability against photobleaching, and low cytotoxicity. As-prepared CDs can be used as a fluorescent probe for peculiar detection of Pt 2+, Au 3+, and Pd 2+ . Furthermore, the CDs show excellent biocompatibility, which were successfully used as hopeful bioimaging and biosensing of noble metal ions in PC12 cells and zebrafish.

Abstract Metals are excellent choices for electrical- and thermal-current conducting. However, either the stiffness of solid metals or the fluidity of liquid metals could be troublesome when flexibility and formability are both desired. To address this problem, a reliable two-stage route to improve the functionalities of gallium-based liquid metals is proposed. A series of stable semiliquid/semisolid gallium-based liquid metal amalgams with well-controlled particle packing ratios, which we call TransM2ixes, are prepared and characterized. Through effectively packing the liquid metal with copper particles (which are found to turn into intermetallic compound, CuGa2, after dispersing), remarkable enhancements in electrical conductivity (6 × 106 S m–1, ∼80% increase) and thermal conductivity (50 W m–1 K–1, ∼100% increase) are obtained, making the TransM2ixes stand out from current conductive soft materials. The TransM2ixes also exhibit appealing semiliquid/semisolid mechanical behaviors such as excellent adhesion, tunable formability, and self-healing ability. As a class of highly…

The quest for the development of new porous materials addressing both CO 2 capture from various sources and its conversion into useful products is a very active research area and also critical in order to develop a more sustainable and environmentally-friendly society. Here, we present the first charged covalent triazine framework (cCTF) prepared by simply heating nitrile functionalized dicationic viologen derivatives under ionothermal reaction conditions using ZnCl 2 as both solvent and trimerization catalyst. It has been demonstrated that the surface area, pore volume/size of cCTFs can be simply controlled by varying the synthesis temperature and the ZnCl 2 content. Specifically, increasing the reaction temperature led to controlled increase in the mesopore content and facilitated the formation of hierarchical porosity, which is critical to ensure efficient mass transport within porous materials. The resulting cCTFs showed high specific surface areas up to 1247 m 2 g –1, and high physicochemical stability. The incorporation of ionic functional moieties to porous organic polymers…

Mn 4+ -activated oxide phosphors La(MgTi) 1/2 O 3 (LMT) with far-red emitting were prepared via a sol–gel route. The structures of samples were determined by X-ray diffraction (XRD) and Reitveld refinement. The occupied sites of Mn 4+ ( d 3 electronic configuration) in host La(MgTi) 1/2 O 3 were confirmed by ab initio calculations in which the system has the lower formation energy, stable lattice structure, and strong bonding state as Mn 4+ enters into Ti site. The luminescent properties of Mn 4+ -doped samples were investigated; the samples emit far-red light centered at 708 nm with ultraviolet light (345 nm) or blue light (487 nm) excitation. According to the photoluminescence (PL) and excitation (PLE) spectra, the crystal field strength of the Mn 4+ -occupied environment was estimated. The thermal stability of phosphor was also evaluated through temperature-dependent PL intensity in a heating and cooling cycle process. The emission band is well-matched with the absorption band of phytochrome P FR under the excitation of light in near-ultraviolet to blue, which suggests that the…

Constructing 0D/2D Z-scheme photocatalysts is a great promising path to improve photocatalytic activity by efficiently enhancing charge separation. Herein, we fabricated a visible-light-responsive Bi 3 TaO 7 quantum dots (QDs)/g-C 3 N 4 nanosheets (NSs) 0D/2D Z-scheme composite via a facile ultrasound method, and Bi 3 TaO 7 QDs could be interspersed on the surface of g-C 3 N 4 NSs uniformly. Furthermore, the strong interaction between Bi 3 TaO 7 QDs and g-C 3 N 4 NSs disturbed the CN heterocycles by forming C═O bonds between C atoms of the N-(C) 3 group and O atoms of the Ta–O bond. The optimum composite with 20 wt % g-C 3 N 4 NSs showed the superior photocatalytic activity for degradation of ciprofloxacin (CIP) over the composites prepared by mechanical mixing and solid-state methods, the photocatalytic efficiency of which were 4 and 12.2 times higher than those of bare Bi 3 TaO 7 and g-C 3 N 4 . Photoluminescence (PL), time-resolved transient PL decay spectra, and photocurrent together verify that the photogenerated hole–electron pairs in this 0D/2D Z-scheme composite have been…

Enrichment of uranyl from seawater is crucial for the sustainable development of nuclear energy, but current uranium extraction technology suffers from multiple drawbacks of low sorption efficiency, slow uptake kinetics, or poor extraction selectivity. Herein, we prepared the first example of amidoxime appended metal-organic framework UiO-66-AO by a postsynthetic modification method for rapid and efficient extraction of uranium from seawater. UiO-66-AO can remove 94.8% of uranyl ion from Bohai seawater within 120 min and 99% of uranyl ion from Bohai seawater containing extra 500 ppb uranium within 10 min. The uranyl sorption capacity in a real seawater sample was determined to be 2.68 mg/g. In addition, the recyclability of the UiO-66-AO framework was demonstrated for at least three adsorption/desorption cycles. The origin for the superior sorption capability was further probed by extended X-ray absorption fine structure (EXAFS) analysis on the uranium-sorbed sample, suggesting multiple amidoxime ligands are able to chelate uranyl(VI) ions, forming a hexagonal bipyramid coordination…

We describe herein a nanocellulose-alginate hydrogel suitable for 3D printing. The composition of the hydrogel was optimized based on material characterization methods and 3D printing experiments, and its behavior during the printing process was studied using computational fluid dynamics simulations. The hydrogel was biofunctionalized by the covalent coupling of an enhanced avidin protein to the cellulose nanofibrils. Ionic cross-linking of the hydrogel using calcium ions improved the performance of the material. The resulting hydrogel is suitable for 3D printing, its mechanical properties indicate good tissue compatibility, and the hydrogel absorbs water in moist conditions, suggesting potential in applications such as wound dressings. The biofunctionalization potential was shown by attaching a biotinylated fluorescent protein and a biotinylated fluorescent small molecule via avidin and monitoring the material using confocal microscopy. The 3D-printable bioactivated nanocellulose-alginate hydrogel offers a platform for the development of biomedical devices, wearable sensors, and…

Even though the nonlinear optical effects of solution processed organic-inorganic perovskite films have been studied, the nonlinear optical properties in two-dimensional (2D) perovskites, especially their applications for ultrafast photonics, are largely unexplored. In comparison to bulk perovskite films, 2D perovskite nanosheets with small thicknesses of a few unit cells are more suitable for investigating the intrinsic nonlinear optical properties because bulk recombination of photocarriers and the nonlinear scattering are relatively small. In this research, we systematically investigated the nonlinear optical properties of 2D perovskite nanosheets derived from a combined solution process and vapor phase conversion method. It was found that 2D perovskite nanosheets have stronger saturable absorption properties with large modulation depth and very low saturation intensity compared with those of bulk perovskite films. Using an all dry transfer method, we constructed a new type of saturable absorber device based on single piece 2D perovskite nanosheet. Stable soliton state…

High porosities, large surface areas, and tunable functionalities made metal-organic frameworks (MOFs) as effective carriers for drug delivery. One of the most promising MOFs is the zeolitic imidazolate framework (ZIF-8) crystal, an advanced functional material for small-molecule delivery, due to its high loading ability and pH-sensitive degradation. As a novel carrier, ZIF-8 nanoparticles were used in this work to control the release of an autophagy inhibitor, 3-methyladenine (3-MA), and prevent it from dissipating in a large quantity before reaching the target. The cellular uptake in HeLa cells of 3-MA encapsulated in ZIF-8 (3-MA@ZIF-8 NPs) is facilitated through the nanoparticle internalization with reference to TEM observations and the quantitative analyses of zinc by ICP-MS. The autophagy-related proteins and autophagy flux in HeLa cells treated with 3-MA@ZIF-8 NPs show that the autophagosome formation is significantly blocked, which reveals that the pH-sensitive dissociation increases the efficiency of autophagy inhibition at the equivalent concentration of 3-MA. In vivo…

Nanocomposites of poly(methyl methacrylate)/reduced graphene oxide (PMMA/rGO) without and with decorated magnetite nanoparticles with a segregated structure were prepared using emulsifier-free emulsion polymerization. Various characterization techniques were employed to validate the presence of the nanofillers and the formation of the segregated structure within the nanocomposites. The percolation threshold of the nanocomposites was found to be 0.3 vol %, while a maximum electrical conductivity of 91.2 S·m –1 and electromagnetic interference shielding effectiveness (EMI SE) of 63.2 dB (2.9 mm thickness) were achieved for the PMMA/rGO nanocomposites at a loading of 2.6 vol % rGO. It was also observed that decorating rGO with magnetite nanoparticles (hybrid nanocomposites) led to a tremendous increase in EMI SE. For instance, 1.1 vol % PMMA/rGO nanocomposites indicated an EMI SE of 20.7 dB, while adding 0.5 vol % magnetite nanoparticles enhanced EMI SE to 29.3 dB. The excellent electrical properties obtained for these nanocomposites were ascribed to both superiorities of the…

The recent discovery of ferroelectricity in thin hafnium oxide films has led to a resurgence of interest in ferroelectric memory devices. Although both experimental and theoretical studies on this new ferroelectric system have been undertaken, much remains to be unveiled regarding its domain landscape and switching kinetics. Here we demonstrate that the switching of single domains can be directly observed in ultrascaled ferroelectric field effect transistors. Using models of ferroelectric domain nucleation we explain the time, field and temperature dependence of polarization reversal. A simple stochastic model is proposed as well, relating nucleation processes to the observed statistical switching behavior. Our results suggest novel opportunities for hafnium oxide based ferroelectrics in nonvolatile memory devices.

Dispersion of graphene in water and its incorporation into waterborne resin have been rarely researched and hardly achieved owing to its hydrophobicity. Furthermore, it has largely been reported that graphene with impermeability contributed to the improved anticorrosion property. Here, we show that highly concentrated graphene aqueous solution up to 5 mg/mL can be obtained by synthesizing hydrophilic polypyrrole (PPy) nanocolloids as intercalators and ultrasonic vibration. On the basis of π-π interaction between PPy and graphene, stacked graphene sheets are exfoliated to the thickness of three to five layers without increasing defects. The corrosion performance of coatings without and with PPy and graphene is obtained by potential and impedance measurements, Tafel curves, and fitted pore resistance by immersing in a 3.5 wt % NaCl solution. It turns out that composite coating with 0.5 wt % graphene additive exhibits superior anticorrosive ability. The mechanism of intercalated graphene-based coating is interpreted as the synergistic protection of impermeable graphene sheets and…

In this work, a new type of ultrasmall Pt nanoclusters (Pt NCs) was prepared via a facile one-pot approach by using yeast extract as the reductant and stabilizer. Besides their excellent water solubility, these yeast extract-stabilized Pt NCs also possess attractive peroxidase mimicking property. They can efficiently catalyze the oxidation of 3,3,5,5-tetramethylbenzidine (TMB) in the coexistence of hydrogen peroxide (H 2 O 2 ). Catalytic mechanism analysis suggested that the peroxidase mimicking activity of these Pt NCs might originate from their characteristic of accelerating electron transfer between TMB and H 2 O 2, and their enzymatic kinetics followed typical Michaelis–Menten theory. On the basis of these findings, we developed a new highly sensitive colorimetric method for glucose detection, and the limit of detection was calculated as low as 0.28 μM (S/N = 3). Further application of the present system for glucose detection in human serum has been successfully demonstrated, suggesting its promising utilization as robust peroxidase mimics in the clinical diagnosis,…

Brightly red fluorescent carbon dots are synthesized hydrothermally and dissolved in diluted hydrochloric acid solution. Such carbon dots exhibit excitation-independent emission at about 620 nm with quantum yield over 10%, which is visible in daylight. After the carbon dots solution is sprayed to the fingerprints on various solid substrates and dried in air, clear fingerprints can be seen under an ultraviolet lamp and stay stable for 1 day. Detailed characterizations suggest that during the drying process, the coffee-ring effect and the electrostatic interactions between the carbon dots and the fingerprint residues prevent the typical aggregation-induced fluorescence quenching of carbon dots.

All inorganic perovskites quantum dots (PeQDs) have attracted much attention for used in thin film display applications and solid-state lighting applications, owing to their narrow band emission with high photoluminescence quantum yields (PLQYs), color tunability, and solution processability. Here, we fabricated low-driving-voltage and high-efficiency CsPbBr 3 PeQDs light-emitting devices (PeQD-LEDs) using a PeQDs washing process with an ester solvent containing butyl acetate (AcOBu) to remove excess ligands from the PeQDs. The CsPbBr 3 PeQDs film washed with AcOBu exhibited a PLQY of 42%, and a narrow PL emission with a full width at half-maximum of 19 nm. We also demonstrated energy level alignment of the PeQD-LED in order to achieve effective hole injection into PeQDs from the adjacent hole injection layer. The PeQD-LED with AcOBu-washed PeQDs exhibited a maximum power efficiency of 31.7 lm W –1 and EQE of 8.73%. Control of the interfacial PeQDs through ligand removal and energy level alignment in the device structure are promising methods for obtaining high PLQYs in film state…

Porous g-C 3 N 4 nanosheet (PCNS) photocatalyst with a thickness of 2.0 nm, pore volume of 0.61 cm 3 g –1, and surface area of 190.1 m 2 g –1 was prepared by a simple two-step template-free approach without the addition of extra reagents. Compared with the bulk g-C 3 N 4 (BCN), PCNS possesses a greater number of surface reactive sites, improved efficiency of charge transfer, and accelerated separation of photogenerated electron–hole pairs. Accordingly, the visible-light-driven photocatalytic disinfection performance and organic pollutant degradation activity of PCNS are significantly enhanced. Escherichia coli ( E. coli ) cells can be killed completely by PCNS within 4 h, whereas only 77.1% of E. coli cells can be killed by BCN. The photodegradation rates of PCNS on methylene blue, Acid Red 27, and bisphenol A are almost 6.4, 4.0, and 1.9 times as fast as that of BCN, respectively. The photocurrent intensity of PCNS is about 3.7 times in comparison with that of BCN. Considering the easy preparation and excellent performance, PCNS could be a promising and competitive…

Lithium (Li) ion battery has penetrated almost every aspect of human life, from portable electronics, vehicles, to grids, and its operation stability in extreme environments is becoming increasingly important. Among these, subzero temperature presents a kinetic challenge to the electrochemical reactions required to deliver the stored energy. In this work, we attempted to identify the rate-determining process for Li + migration under such low temperatures, so that an optimum electrolyte formulation could be designed to maximize the energy output. Substantial increase in the available capacities from graphite∥LiNi 0.80 Co 0.15 Al 0.05 O 2 chemistry down to −40 °C is achieved by reducing the solvent molecule that more tightly binds to Li + and thus constitutes a high desolvation energy barrier. The fundamental understanding is applicable universally to a wide spectrum of electrochemical devices that have to operate in similar environments.

In this study, we fabricated conductive poly(vinylidene fluoride) (PVDF)/carbon composites simply by dispersing multiwalled carbon nanotubes (MWCNTs) and graphene nanoplatelets into a PVDF solution. The electrical conductivity and the electromagnetic interference (EMI) shielding of the PVDF/carbon composites were increased by increasing the conductive carbon filler amounts. Moreover, we also found that the EMI shielding properties of the PVDF/CNT/graphene composites were higher than those of PVDF/CNT and PVDF/graphene composites. The mean EMI shielding values of PVDF/5 wt %-CNT, PVDF/10 wt %-graphene, and PVDF/CNT/graphene composite films with a thickness of 0.1 mm were 22.41, 18.70, and 27.58 dB, respectively. An analysis of the shielding mechanism showed that the main contribution to the EMI shielding came from the absorption mechanism, and that the EMI shielding could be tuned by controlling the films’ thickness. The total shielding of the PVDF/CNT/graphene films increased from 21.90 to 36.46 dB as the thickness was increased from 0.06 mm to 0.25 mm. In particular, the…

This comprehensive review surveys the up-to-date development of aggregation-induced emission/aggregation-induced emission enhancement (AIE/AIEE) active naphthalimide (NI)-based smart materials with potential for wide and real-world applications and that serves as a highly versatile building block with tunable absorption and emission in the complete visible region. The review article commences with a precise description of the importance of NI moiety and its several restricted area of applications owing to its aggregation caused quenching (ACQ) properties, followed by the discovery and importance of AIE/AIEE-active NIs. The introduction section tracked an overview of the state of the art in NI luminogens in multiple applications. It also includes a few mechanistic studies on the structure-property correlation of NIs and provides more insights into the condensed-state photophysical properties of small aggregation-prone systems. The review aims to ultimately accomplish current and forthcoming views comprising the use of the NIs for the detection of biologically active molecules, such…

Developing lightweight and highly efficient electromagnetic wave (EMW) absorbing materials is crucial but challenging for anti-electromagnetic irradiation and interference. Herein, we used multiwalled carbon nanotubes (MWCNTs) as templates for growth of Co-based zeolitic imidazolate frameworks (ZIFs) and obtained a Co-C/MWCNTs composite by postpyrolysis. The MWCNTs interconnected the ZIF-derived Co-C porous particles, constructing a conductive network for electron hopping and migration. Moreover, the Co-C/MWCNTs composite was aligned in paraffin matrix under an external magnetic field, which led to a stretch of the MWCNTs along the magnetic field direction. Due to the anisotropic permittivity of MWCNTs, the magnetic alignment considerably increased the dielectric loss of the Co-C/MWCNTs composite. Benefiting from the conductive network, the orientation-enhanced dielectric loss, and the synergistic effect between magnetic and dielectric components, the magnetically aligned Co-C/MWCNTs composite exhibited extremely strong EMW absorption, with a minimum reflection loss (RL) of -48.9 dB…

Inspired by the diverse drug compounds with various heteroatoms (such as N, S, and P) in the drug library, facile synthesis of a new kind of bright and color-tunable N-doped carbon dots (NCDs) has been reported by using a popular antibiotic—aminosalicylic acid—as precursor. The N doping of CDs not only enable great improvement of photoluminescence (PL) efficiency and tunability of PL emission, but also enrich surface functional groups to broaden its application. The as-prepared NCDs possess tunable PL and show a quantum yield of 16.4%, which is the result of PL improvement effect of introduced nitrogen atoms among CDs. The cellular toxicity on H1299 cancer cells indicates that the NCDs have negligible cytotoxicity, excellent biocompatibility, and great resistance to photobleaching. Moreover, the drug-derived NCDs showed excellent sensitivity in detection of Fe 3+ in living cells, which indicates the potential application in diagnosis and related biological study.

Hf 0.5 Zr 0.5 O 2 thin films are one of the most appealing HfO 2 -based ferroelectric thin films, which have been researched extensively for their applications in ferroelectric memory devices. In this work, a 1 mol % La-doped Hf 0.5 Zr 0.5 O 2 thin film was grown by plasma-assisted atomic layer deposition and annealed at temperatures of 450 and 500 °C to crystallize the film into the desired orthorhombic phase. Despite the use of a lower temperature than that used in previous reports, the film showed highly promising ferroelectric properties—a remnant polarization of ∼30 μC/cm 2 and switching cycle endurance up to 4 × 10 10 . The performance was much better than that of undoped Hf 0.5 Zr 0.5 O 2 thin films, demonstrating the positive influence of La doping. Such improvements were mainly attributed to the decreased coercive field (by ∼30% compared to the undoped film), which allowed for the use of a lower applied field to drive the cycling tests while maintaining a high polarization value. La doping also decreased the leakage current by ∼3 orders of magnitude compared to the undoped…

Bimetallic phosphides have attracted research interest for their synergistic effect and superior electrocatalytic activities for electrocatalytic water splitting. Herein, a MOF-derived phosphorization approach was developed to produce Ni 2 P–CoP bimetallic phosphides as bifunctional electrocatalysts for both hydrogen and oxygen evolution reactions (HER and OER). Ni 2 P–CoP shows superior electrocatalytic activities to both pure Ni 2 P and CoP toward HER and OER, revealing a strong synergistic effect. High-resolution transmission electron microscopy and energy dispersive X-ray spectroscopy elemental mapping analysis show that, in the sample Ni 2 P–CoP, the Ni 2 P and CoP nanoparticles with an average particle size 10–20 nm were mixed closely on the nanoscale, creating numerous Ni 2 P/CoP interfaces. By comparison with the sample Ni 2 P+CoP, in which seldom Ni 2 P/CoP interfaces exist, we documented that the Ni 2 P/CoP interface is an essential prerequisite to realize the synergistic effect and to achieve the enhanced electrocatalytic activities in Ni 2 P–CoP bimetallic phosphides.…

Novel g-C 3 N 4 /CoO nanocomposite application for photocatalytic H 2 evolution were designed and fabricated for the first time in this work. The structure and morphology of g-C 3 N 4 /CoO were investigated by a wide range of characterization methods. The obtained g-C 3 N 4 /CoO composites exhibited more-efficient utilization of solar energy than pure g-C 3 N 4 did, resulting in higher photocatalytic activity for H 2 evolution. The optimum photoactivity in H 2 evolution under visible-light irradiation for g-C 3 N 4 /CoO composites with a CoO mass content of 0.5 wt % (651.3 μmol h –1 g –1 ) was up to 3 times as high as that of pure g-C 3 N 4 (220.16 μmol h –1 g –1 ). The remarkably increased photocatalytic performance of g-C 3 N 4 /CoO composites was mainly attributed to the synergistic effect of the junction or interface formed between g-C 3 N 4 and CoO.

The unique structure of a vertically aligned carbon nanotube (VACNT) array makes it behave most similarly to a blackbody. It is reported that the optical absorptivity of an extremely black VACNT array is about 0.98-0.99 over a large spectral range of 200 nm-200 μm, inspiring us to explore the performance of VACNT arrays in solar energy harvesting. In this work, we report the highly efficient steam generation simply by laminating a layer of VACNT array on the surface of water to harvest solar energy. It is found that under solar illumination the temperature of upper water can significantly increase with obvious water steam generated, indicating the efficient solar energy harvesting and local temperature rise by the thin layer of VACNTs. We found that the evaporation rate of water assisted by VACNT arrays is 10 times that of bare water, which is the highest ratio for solar-thermal-steam generation ever reported. Remarkably, the solar thermal conversion efficiency reached 90%. The excellent performance could be ascribed to the strong optical absorption and local temperature rise…

Future electronics are expected to develop into wearable forms, and an adequate stretchability is required for the forthcoming wearable electronics considering various motions occurring in human body. Along with stretchability, transparency can increase both the functionality and esthetic features in future wearable electronics. In this study, we demonstrate, for the first time, a highly stretchable and transparent electromagnetic interference shielding layer for wearable electronic applications with silver nanowire percolation network on elastic poly(dimethylsiloxane) substrate. The proposed stretchable and transparent electromagnetic interference shielding layer shows a high electromagnetic wave shielding effectiveness even under a high tensile strain condition. It is expected for the silver nanowire percolation network-based electromagnetic interference shielding layer to be beyond the conventional electromagnetic interference shielding materials and to broaden its application range to various fields that require optical transparency or nonplanar surface environment, such as…

In the present work, we have synthesized three-dimensional (3D) reduced graphene oxide nanosheets (rGO NSs) containing iron oxide nanoparticles (Fe 3 O 4 NPs) hybrids (3D Fe 3 O 4 /rGO) by one-pot microwave approach. Structural and morphological studies reveal that the as-synthesized Fe 3 O 4 /rGO hybrids were composed of faceted Fe 3 O 4 NPs induced into the interconnected network of rGO NSs. The morphologies and structures of the 3D hybrids have been characterized using scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Raman spectroscopy and X-ray photoelectron spectrometer (XPS). The electrochemical studies were analyzed by cyclic voltammetry, galvanostatic charge/discharge measurements, and electrochemical impedance spectroscopy, which demonstrate superior electrochemical performance as supercapacitors electrode application. The specific capacitances of 3D hybrid materials was 455 F g –1 at the scan rate of 8 mV s –1, which is superior to that of bare Fe 3 O 4 NPs. Additionally, the 3D hybrid shows good cycling stability with a…

Electrochemical reduction of CO 2 to chemical feedstocks is an attractive solution that prevents CO 2 accumulation in the atmosphere, but it remains a great challenge to develop the cost-effective catalysts. Herein, we synthesized oxide-derived Cu/carbon (OD Cu/C) catalysts by a facile carbonization of Cu-based MOF (HKUST-1). The resulting materials exhibited highly selective CO 2 reduction to alcohol compounds with total faradic efficiencies of 45.2–71.2% at −0.1 to −0.7 V versus reversible hydrogen electrode (RHE). High-yield methanol and ethanol has been achieved on OD Cu/C-1000 with the production rates of 5.1–12.4 and 3.7–13.4 mg L –1 h –1, respectively. Notably, the onset potential for C 2 H 5 OH formation is near −0.1 V (versus RHE), corresponding to ∼190 mV of overpotential, which is among the lowest overpotentials reported to date for the reduction of CO 2 to C 2 H 5 OH. The improvements in activity and selectivity of the oxide-derived Cu/carbon might be attributed to the synergistic effect between the highly dispersed copper and the matrix of porous carbon. These findings…

Flexible pressure sensors have attracted increasing research interest because of their potential applications for wearable sensing devices. Herein, a highly sensitive flexible pressure sensor is exhibited based on the elastomeric electrodes and a microarray architecture. Polydimethylsiloxane (PDMS) substrate, coated with silver nanowires (AgNWs), is used as the top electrode, while polyvinylidene fluoride (PVDF) as the dielectric layer. Several transfer processes are applied on seeking facile strategy for the preparation of the bottom electrode via embedding AgNWs into the PDMS film of microarray structure. The flexible pressure sensor integrates the top electrode, dielectric layer, and microarray electrode in a sandwich structure. It is demonstrated that such sensors possess the superiorities of high sensitivity (2.94 kPa –1 ), low detection limit (<3 Pa), short response time (<50 ms), excellent flexibility, and long-term cycle stability. This simple process for preparing such sensors can also be easily scaled up to construct pressure sensor arrays for detecting the intensity and…

Multifunctional graphene oxide (GO)/chitosan (CS) aerogel microspheres (GCAMs) with honeycomb-cobweb and radially oriented microchannel structures are prepared by combining electrospraying with freeze-casting to optimize adsorption performances of heavy metal ions and soluble organic pollutants. The GCAMs exhibit superior adsorption capacities of heavy metal ions of Pb(II), Cu(II), and Cr(VI), cationic dyes of methylene blue (MB) and Rhodamine B, anionic dyes of methyl orange and Eosin Y, and phenol. It takes only 5 min to reach 82 and 89% of equilibrium adsorption capacities for Cr(VI) (292.8 mg g –1 ) and MB (584.6 mg g –1 ), respectively, much shorter than the adsorption equilibrium time (75 h) of a GO/CS monolith. More importantly, the GCAMs maintain excellent adsorption capacity for six cycles of adsorption–desorption. The broad-spectrum, rapid, and reusable adsorption performance makes the GCAMs promising for highly efficient water treatments.

Cu-MOF nanoparticles with an average diameter of 550 nm were synthesized from 2-aminoterephthalic acid and Cu(NO 3 ) 2 by a mixed solvothermal method. The Cu-MOF nanoparticles can show peroxidase-like activity that can catalyze 3,3′,5,5′-tetramethylbenzidine to produce a yellow chromogenic reaction in the presence of H 2 O 2 . The presence of abundant amine groups on the surfaces of Cu-MOF nanoparticles enables facile modification of Staphylococcus aureus ( S. aureus ) aptamer on Cu-MOF nanoparticles. By combining Cu-MOF-catalyzed chromogenic reaction with aptamer recognition and magnetic separation, a simple, sensitive, and selective colorimetric method for the detection of S. aureus was developed.

An anisotropic thermally conductive film with tailorable microstructures and macroproperties is fabricated using a layer-by-layer (LbL) assembly of graphene oxide (GO) and nanofibrillated cellulose (NFC) on a flexible NFC substrate driven by hydrogen bonding interactions, followed by chemical reduction process. The resulting NFC/reduced graphene oxide (RGO) hybrid film reveals an orderly hierarchical structure in which the RGO nanosheets exhibit a high degree of orientation along the in-plane direction. The assembly cycles dramatically increase the in-plane thermal conductivity (λ X ) of the hybrid film to 12.6 W·m –1 ·K –1, while the cross-plane thermal conductivity (λ Z ) shows a lower value of 0.042 W·m –1 ·K –1 in the hybrid film with 40 assembly cycles. The thermal conductivity anisotropy reaches up to λ X /λ Z = 279, which is substantially larger than that of similar polymeric nanocomposites, indicating that the LbL assembly on a flexible NFC substrate is an efficient technique for the preparation of polymeric nanocomposites with improved heat conducting property. Moreover,…

Lightweight, biodegradable, thermally insulating, and electrically conductive materials play a vital role in achieving the sustainable development of our society. The fabrication of such multifunctional materials is currently very challenging. Here, we report a general, facile, and eco-friendly way for the large-scale fabrication of ultralow-threshold and biodegradable porous polylactic acid (PLA)/multiwalled carbon nanotube (MWCNT) for high-performance thermal insulation and electromagnetic interference (EMI) shielding applications. Thanks to the unique structure of the microporous PLA matrix embedded by conductive 3D MWCNT networks, the lightweight porous PLA/MWCNT with a density of 0.045 g/cm 3 possesses a percolation threshold of 0.00094 vol %, which, to our knowledge, is the minimum value reported so far. Furthermore, the material exhibits excellent thermal insulation performance with a thermal conductivity of 27.5 mW·m –1 ·K –1, which is much lower than the best value of common thermal insulation materials. Moreover, it also shows outstanding EMI shielding performance…

Metal–organic frameworks (MOFs) with Fe content are gradually developing into an independent branch in environmental remediation, requiring economical, effective, low-toxicity strategies to the complete procedure. In this review, recent advancements in the structure, synthesis, and environmental application focusing on the mechanism are presented. The unique structure of novel design proposed specific characteristics of different iron-containing MOFs with potential innovation. Synthesis of typical MILs, NH 2 -MILs and MILs based materials reveal the basis and defect of the current method, indicating the optimal means for the actual requirements. The adsorption of various contamination with multiple interaction as well as the catalytic degradation over radicals or electron–hole pairs are reviewed. This review implied considerable prospects of iron-containing MOFs in the field of environment and a more comprehensive cognition into the challenges and potential improvement.

Boron nitride nanosheet (BNNS) films receive wide attention in both academia and industry because of their high thermal conductivity (TC) and good electrical insulation capability. However, the brittleness and low strength of the BNNS film largely limit its application. Herein, functionalized BNNSs (f-BNNSs) with a well-maintained in-plane crystalline structure were first prepared utilizing urea in the aqueous solution via ball-milling for the purpose of improving their stability in water and enhancing the interaction with the polymer matrix. Then, a biodegradable and highly thermally conductive film with an orderly oriented structure based on cellulose nanofibers (CNFs) and f-BNNSs was prepared just by simple vacuum-assisted filtration. The modification of the BNNS and the introduction of the CNF result in a better orientation of the f-BNNS, sufficient connection between f-BNNS themselves, and strong interaction between f-BNNS and CNF, which not only make the prepared composite film strong and tough but also possess higher in-plane TC. An increase of 70% in-plane TC, 63.2% tensile…

When it comes to underwater adhesion, shellfish are the true experts. Mussels, barnacles, and oysters attach to rocks with apparent ease. Yet our man-made glues often fail when trying to stick in wet environments. Results described herein focus on a copolymer mimic of mussel adhesive proteins, poly(catechol-styrene). Underwater bonding was examined as a function of parameters including polymer molecular weight and composition. In doing so, several surprising results emerged. Poly(catechol-styrene) may be the strongest underwater adhesive found to date. Bonding even exceeded that of the reference biological system, live mussels. Adhesion was also found to be stronger under salt water than deionized water. Such unexpected findings may contradict an earlier proposal in which charged amino acids were suggested to be key for mussel adhesive function. Taken together, these discoveries are helping us to both understand biological adhesion as well as develop new materials with properties not accessed previously.

The design of efficient, low-cost, and stable electrocatalyst systems toward energy conversion is highly demanding for their practical use. Large scale electrolytic water splitting is considered as a promising strategy for clean and sustainable energy production. Herein, we report a self-supported NiFe layered double hydroxide (LDH)-NiSe electrocatalyst by stepwise surface-redox-etching of Ni foam (NF) through a hydrothermal process. The as-prepared NiFe LDH-NiSe/NF catalyst exhibits far better performance in alkaline water oxidation, proton reduction, and overall water splitting compared to NiSe x /NF or NiFe LDH/NF. Only 240 mV overpotential is required to obtain a water oxidation current density of 100 mA cm –2, whereas the same for the hydrogen evolution reaction is 276 mV in 1.0 M KOH. The synergistic effect from NiSe and NiFe LDH leads to the evolution of a highly efficient catalyst system for water splitting by achieving 10 mA cm –2 current density at only 1.53 V in a two-electrode alkaline electrolyzer. In addition, the designed electrode produces stable performance for a…

To improve the utilization of visible light and reduce photogenerated electron/hole recombination, Ti 3+ self-doped TiO 2 /oxygen-doped graphitic carbon nitride (Ti 3+ -TiO 2 /O-g-C 3 N 4 ) heterojunctions were prepared via hydrothermal treatment of a mixture of g-C 3 N 4 and titanium oxohydride sol obtained from the reaction of TiH 2 with H 2 O 2 . In this way, exfoliated O-g-C 3 N 4 and Ti 3+ -TiO 2 nanoparticles were obtained. Simultaneously, strong bonding was formed between Ti 3+ -TiO 2 nanoparticles and exfoliated O-g-C 3 N 4 during the hydrothermal process. Charge transfer and recombination processes were characterized by transient photocurrent responses, electrochemical impedance test, and photoluminescence spectroscopy. The photocatalytic performances were investigated through rhodamine B degradation test under an irradiation source based on 30 W cold visible-light-emitting diode. The highest visible-light photoelectrochemical and photocatalytic activities were observed from the heterojunction with 1:2 mass ratio of Ti 3+ -TiO 2 to O-g-C 3 N 4 . The photodegradation…

A new fluorescent polyimide covalent organic framework (PI-COF) has been successfully synthesized through solvothermal route using tetra(4-aminophenyl) porphyrin and perylenetracarboxylic dianhydride, which possesses porous crystalline and excellent thermal stability (>500 °C). Furthermore, few-layered PI covalent organic nanosheets (PI-CONs) can be easily obtained from the fluorescent PI-COF through a facile liquid phase exfoliation approach, which were confirmed by atomic force microscopy and transmission electron microscopy analysis. It is interesting that the fluorescent intensity of PI-CONs is obviously enhanced relative to that of PI-COF. The PI-CONs have been successfully utilized as an efficient fluorescent probe for the highly sensitive and selective detection of 2,4,6-trinitrophenol (TNP). The mechanism might be attributed to the combination of electron transfer and inner filter effect based on DFT calculations and spectral overlap data. The system exhibits a good linear response toward TNP over the range from 0.5 to 10 μM with a detection limit of 0.25 μM.

High crystallinity of covalent organic frameworks (COFs) with dual fluorescence emissions has not been reported so far. Here, we show the rational design and preparation of high-crystallinity COF TzDa via the synergetic interaction of docking sites and hydrogen bonds: 4,4',4″-(1,3,5-Triazine-2,4,6-triyl)trianiline (Tz) with the docking site and 2,5-dihydroxyterephthalaldehyde (Da) with the OH group are employed to synthesize the imine-linked two-dimensional high-crystallinity layered structure TzDa. The prepared mesoporous TzDa (ca. 36 Å) exhibits high thermal and chemical stability. The intramolecular charge transfer (ICT) and excited-state intramolecular proton transfer (ESIPT) effects bring TzDa two main fluorescence emissions around 500 and 590 nm. Water molecules can interfere with the ICT and ESIPT effects, allowing the development of a ratiometric fluorescent sensor for water in organic solvents. The proposed sensor shows high sensitivity to trace water in conventional organic solvents. The high stability of TzDa allows its recyclable uses for trace water detection. This work…

Highly flexible and deformable electrically conductive materials are vital for the emerging field of wearable electronics. To address the challenge of flexible materials with a relatively high electrical conductivity and a high elastic limit, we report a new and facile method to prepare porous polydimethylsiloxane/carbon nanofiber composites (denoted by p-PDMS/CNF). This method involves using sugar particles coated with carbon nanofibers (CNFs) as the templates. The resulting three-dimensional porous nanocomposites, with the CNFs embedded in the PDMS pore walls, exhibit a greatly increased failure strain (up to ∼94%) compared to that of the solid, neat PDMS (∼48%). The piezoresistive response observed under cyclic tension indicates that the unique microstructure provides the new nanocomposites with excellent durability. The electrical conductivity and the gauge factor of this new nanocomposite can be tuned by changing the content of the CNFs. The electrical conductivity increases, while the gauge factor decreases, upon increasing the content of CNFs. The gauge factor of the newly…

Electrocatalytic water-splitting, a combination of oxygen and hydrogen evolution reactions (OER and HER), is highly attractive in clean energy technologies, especially for high-purity hydrogen production, whereas developing stable, earth-abundant, bifunctional catalysts has continued to pose major challenges. Herein, a mesoporous NiFe-oxide nanocube (NiFe-NC) system is developed from a NiFe Prussian blue analog metal–organic framework as an efficient bifunctional catalyst for overall water-splitting. The NiFe-NCs with ∼200 nm side length have a Ni/Fe molar ratio of 3:2 and is a composite of NiO and α/γ-Fe 2 O 3 . The NCs demonstrate overpotentials of 271 and 197 mV for OER and HER, respectively, in 1 M KOH at 10 mA cm –2, which outperform those of 339 and 347 mV for the spherical NiFe-oxide nanoparticles having a similar composition. The electrolyzer constructed using NiFe-NCs requires an impressive cell voltage of 1.67 V to deliver a current density of 10 mA cm –2 . Along with a mesoporous structure with a broad pore size distribution, the NiFe-NCs demonstrate the qualities of a…

Nanozymes are an excellent class of optical reporters for the development of sensitive biosensors for widespread applications. In this study, mesoporous core-shell palladium@platinum (Pd@Pt) nanoparticles were synthesized and then applied as signal amplifier in a dual lateral flow immunoassay (LFIA) and integrated with a smartphone-based device for use in simultaneous detection of Salmonella Enteritidis and Escherichia coli O157:H7. After optimization, the limit of detections were calculated to be ∼20 cfu/mL for S. Enteritidis and ∼34 cfu/mL for E. coli O157:H7, respectively. The greatly improved sensitivity was contributed by the peroxidase-like catalytic activity of the Pd@Pt nanoparticles for signal enhancement and the parallel design of dual detection for eliminating the cross-interference. The estimated recoveries of the dual LFIA range from 91.44 to 117.00%, which indicated that the developed method is capable of detecting live bacteria in food samples. This approach provides an attractive platform for S. Enteritidis and E. coli O157:H7 detection using a smartphone-based…

Superhydrophobic coatings are highly promising for protecting material surfaces and for wide applications. In this study, superhydrophobic composites, comprising a rhombic-dodecahedral zeolitic imidazolate framework (ZIF-8@SiO 2 ), have been manufactured onto AZ31 magnesium alloy via chemical etching and dip-coating methods to enhance stability and corrosion resistance. Herein, we report on a simple strategy to modify hydrophobic hexadecyltrimethoxysilan (HDTMS) on ZIF-8@SiO 2 to significantly improve the property of repelling water. We show that various liquids can be stable on its surface and maintain a contact angle higher than 150°. The morphologies and chemical composition were characterized by means of scanning electron microscopy (SEM) and Fourier transform infrared spectroscopy (FI-IR). In addition, the anticorrosion and antiattrition properties of the film were assessed by electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization and HT, respectively. Such a coating shows promising potential as a material for large-scale fabrication.

Abstract Metal–organic frameworks (MOFs) have shown promising performance in separation, adsorption, reaction, and storage of various industrial gases; however, their large-scale applications have been hampered by the lack of a proper strategy to formulate them into scalable gas–solid contactors. Herein, we report the fabrication of MOF monoliths using the 3D printing technique and evaluation of their adsorptive performance in CO2 removal from air. The 3D-printed MOF-74­(Ni) and UTSA-16­(Co) monoliths with MOF loadings as high as 80 and 85 wt %, respectively, were developed, and their physical and structural properties were characterized and compared with those of MOF powders. Our adsorption experiments showed that, upon exposure to 5000 ppm (0.5%) CO2 at 25 °C, the MOF-74­(Ni) and UTSA-16­(Co) monoliths can adsorb CO2 with uptake capacities of 1.35 and 1.31 mmol/g, respectively, which are 79% and 87% of the capacities of their MOF analogues under the same conditions. Furthermore, a stable performance was obtained for self-standing 3D-printed monolithic structures with relatively…

Driven by the urgent need to detect trace heavy metal ions in various real water samples, this article demonstrates for the first time an electrochemical biosensor based on DNA modified Fe 3 O 4 @Au magnetic nanoparticles (NPs). Three DNA probes are designed to contain certain mismatched base pairs. One is thiolated and modified on the surface of Fe 3 O 4 @Au NPs (DNA 1). The other two probes (DNA 2 and 3) are labeled with two independent electrochemical species. Stable structures of cytosine–Ag + –cytosine and thymine–Hg 2+ –thymine formed in the presence of Ag + and Hg 2+ can assist the hybridization of DNA 1/DNA 2 and DNA 1/DNA 3, which locate corresponding electrochemical species onto the surface of the magnetic NPs. The achieved nanocomposites are then used as selective electrochemical probes for the detection of heavy metal ions by recording the square wave voltammetry signals. Simultaneous detection of Ag + and Hg 2+ is demonstrated without significant interference, and their individual high sensitivities are fundamentally preserved, which meet the requirements of U.S.…