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Showing papers in "ACS Applied Materials & Interfaces in 2015"


Journal ArticleDOI
TL;DR: The results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations, and general principles for developing solid electrolytes materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries are provided.
Abstract: First-principles calculations were performed to investigate the electrochemical stability of lithium solid electrolyte materials in all-solid-state Li-ion batteries. The common solid electrolytes were found to have a limited electrochemical window. Our results suggest that the outstanding stability of the solid electrolyte materials is not thermodynamically intrinsic but is originated from kinetic stabilizations. The sluggish kinetics of the decomposition reactions cause a high overpotential leading to a nominally wide electrochemical window observed in many experiments. The decomposition products, similar to the solid-electrolyte-interphases, mitigate the extreme chemical potential from the electrodes and protect the solid electrolyte from further decompositions. With the aid of the first-principles calculations, we revealed the passivation mechanism of these decomposition interphases and quantified the extensions of the electrochemical window from the interphases. We also found that the artificial coating layers applied at the solid electrolyte and electrode interfaces have a similar effect of passivating the solid electrolyte. Our newly gained understanding provided general principles for developing solid electrolyte materials with enhanced stability and for engineering interfaces in all-solid-state Li-ion batteries.

1,155 citations


Journal ArticleDOI
TL;DR: Among the three Co/C composites obtained at different temperatures, co/C-500 obtained at 500 °C exhibited the best performance for electromagnetic wave absorption, ascribed to the synergetic effects between the highly porous structure and multiple components, which significantly improved impedance matching.
Abstract: Composites incorporating ferromagnetic metal nanopartices into a highly porous carbon matrix are promising as electromagnetic wave absorption materials. Such special composite nanomaterials are potentially prepared by the thermal decomposition of metal–organic framework (MOF) materials under controlled atmospheres. In this study, using Co-based MOFs (Co-MOF, ZIF-67) as an example, the feasibility of this synthetic strategy was demonstrated by the successful fabrication of porous Co/C composite nanomaterials. The atmosphere and temperature for the thermal decomposition of MOF precursors were crucial factors for the formation of the ferromagnetic metal nanopartices and carbon matrix in the porous Co/C composites. Among the three Co/C composites obtained at different temperatures, Co/C-500 obtained at 500 °C exhibited the best performance for electromagnetic wave absorption. In particular, the maximum reflection loss (RL) of Co/C-500 reached −35.3 dB, and the effective absorption bandwidth (RL ≤ −10 dB) was ...

666 citations


Journal ArticleDOI
TL;DR: Insight is provided into heterostructure photocatalysis and a novel way to design and fabricate high-performance semiconductor composites is described, which can greatly enhance the visible-light photocatalytic performance.
Abstract: The fabrication of multiple heterojunctions with tunable photocatalytic reactivity in full-range BiOBr–BiOI composites based on microstructure modulation and band structures is demonstrated. The multiple heterojunctions are constructed by precipitation at room temperature and characterized systematically. Photocatalytic experiments indicate that there are two types of heterostructures with distinct photocatalytic mechanisms, both of which can greatly enhance the visible-light photocatalytic performance for the decomposition of organic pollutants and generation of photocurrent. The large separation and inhibited recombination of electron–hole pairs rendered by the heterostructures are confirmed by electrochemical impedance spectra (EIS) and photoluminescence (PL). Reactive species trapping, nitroblue tetrazolium (NBT, detection agent of •O2–) transformation, and terephthalic acid photoluminescence (TA-PL) experiments verify the charge-transfer mechanism derived from the two types of heterostructures, as we...

651 citations


Journal ArticleDOI
TL;DR: The sample of NG-700, obtained at a calcination temperature of 700 °C, showed the highest efficiency in degradation of phenol solutions by metal-free catalytic activation of peroxymonosulfate (PMS).
Abstract: N-Doped graphene (NG) nanomaterials were synthesized by directly annealing graphene oxide (GO) with a novel nitrogen precursor of melamine. A high N-doping level, 8–11 at. %, was achieved at a moderate temperature. The sample of NG-700, obtained at a calcination temperature of 700 °C, showed the highest efficiency in degradation of phenol solutions by metal-free catalytic activation of peroxymonosulfate (PMS). The catalytic activity of the N-doped rGO (NG-700) was about 80 times higher than that of undoped rGO in phenol degradation. Moreover, the activity of NG-700 was 18.5 times higher than that of the most popular metal-based catalyst of nanocrystalline Co3O4 in PMS activation. Theoretical calculations using spin–unrestricted density functional theory (DFT) were carried out to probe the active sites for PMS activation on N-doped graphene. In addition, experimental detection of generated radicals using electron paramagnetic resonance (EPR) and competitive radical reactions was performed to reveal the PMS...

622 citations


Journal ArticleDOI
TL;DR: This review will cover amine-based technology developed and published in and after the year 2013, which are well-known for their reversible reactions with CO2, which make them ideal for the separation of CO2 from many CO2-containing gases, including flue gas.
Abstract: It is generally accepted by the scientific community that anthropogenic CO2 emissions are leading to global climate change, notably an increase in global temperatures commonly referred to as global warming. The primary source of anthropogenic CO2 emissions is the combustion of fossil fuels for energy. As society’s demand for energy increases and more CO2 is produced, it becomes imperative to decrease the amount emitted to the atmosphere. One promising approach to do this is to capture CO2 at the effluent of the combustion site, namely, power plants, in a process called postcombustion CO2 capture. Technologies to achieve this are heavily researched due in large part to the intuitive nature of removing CO2 from the stack gas and the ease in retrofitting existing CO2 sources with these technologies. As such, several reviews have been written on postcombustion CO2 capture. However, it is a fast-developing field, and the most recent review papers already do not include the state-of-the-art research. Notable am...

617 citations


Journal ArticleDOI
TL;DR: This review focuses especially on the structural aspects of these novel dye anchors for TiO2-based DSSCs, including pyridine, phosphonic acid, tetracyanate, perylene dicarboxylic acid anhydride, 2-hydroxylbenzonitrile, 8-Hydroxylquinoline, pyrsidine-N-oxide, hydroxylpyridium, and salicylic acid substituents.
Abstract: The dyes in dye-sensitized solar cells (DSSCs) require one or more chemical substituents that can act as an anchor, enabling their adsorption onto a metal oxide substrate. This adsorption provides a means for electron injection, which is the process that initiates the electrical circuit in a DSSC. Understanding the structure of various DSSC anchors and the search for new anchors are critical factors for the development of improved DSSCs. Traditionally, carboxylic acid and cyanoacrylic acid groups are employed as dye anchors in DSSCs. In recent years, novel anchor groups have emerged, which make a larger pool of materials available for DSSC dyes, and their associated physical and chemical characteristics offer interesting effects at the interface between dye and metal oxide. This review focuses especially on the structural aspects of these novel dye anchors for TiO2-based DSSCs, including pyridine, phosphonic acid, tetracyanate, perylene dicarboxylic acid anhydride, 2-hydroxylbenzonitrile, 8-hydroxylquinoline, pyridine-N-oxide, hydroxylpyridium, catechol, hydroxamate, sulfonic acid, acetylacetanate, boronic acid, nitro, tetrazole, rhodanine, and salicylic acid substituents. We anticipate that further exploration and understanding of these new types of anchoring groups for TiO2 substrates will not only contribute to the development of advanced DSSCs, but also of quantum dot-sensitized solar cells, water splitting systems, and other self-assembled monolayer-based technologies.

612 citations


Journal ArticleDOI
TL;DR: In this article, phosphorus-doped graphitic carbon nitride nanostructured flowers of in-plane mesopores are synthesized by a co-condensation method in the absence of any templates.
Abstract: Graphitic carbon nitride (g-C3N4) has been deemed a promising heterogeneous metal-free catalyst for a wide range of applications, such as solar energy utilization toward water splitting, and its photocatalytic performance is reasonably adjustable through tailoring its texture and its electronic and optical properties. Here phosphorus-doped graphitic carbon nitride nanostructured flowers of in-plane mesopores are synthesized by a co-condensation method in the absence of any templates. The interesting structures, together with the phosphorus doping, can promote light trapping, mass transfer, and charge separation, enabling it to perform as a more impressive catalyst than its pristine carbon nitride counterpart for catalytic hydrogen evolution under visible light irradiation. The catalyst has low cost, is environmentally friendly, and represents a potential candidate in photoelectrochemistry.

599 citations


Journal ArticleDOI
TL;DR: This article highlights carbon dots, which are small carbon nanoparticles with some form of surface passivation, and graphene quantum dots in various configurations by focusing on their syntheses, on their photoexcited state properties and redox processes, and on their applications as photocatalysts in visible-light carbon dioxide reduction and in water-splitting.
Abstract: Quantum dots (QDs) generally refer to nanoscale particles of conventional semiconductors that are subject to the quantum-confinement effect, though other nanomaterials of similar optical and redox properties are also named as QDs even in the absence of strictly defined quantum confinement. Among such nanomaterials that have attracted tremendous recent interest are carbon dots, which are small carbon nanoparticles with some form of surface passivation, and graphene quantum dots in various configurations. In this article, we highlight these carbon-based QDs by focusing on their syntheses, on their photoexcited state properties and redox processes, and on their applications as photocatalysts in visible-light carbon dioxide reduction and in water-splitting, as well as on their mechanistic similarities and differences.

566 citations


Journal ArticleDOI
Jinjuan Xue1, Shuaishuai Ma1, Yuming Zhou1, Zewu Zhang1, Man He1 
TL;DR: A novel plasmonic photocatalyst, Au/Pt/g-C3N4, was prepared by a facile calcination-photodeposition technique and enhanced photocatalytic activity for antibiotic tetracycline hydrochloride (TC-HCl) degradation was attributed to the surface plAsmon resonance effect of Au and electron-sink function of Pt nanoparticles, synergistically facilitating the photocatalysis process.
Abstract: A novel plasmonic photocatalyst, Au/Pt/g-C3N4, was prepared by a facile calcination-photodeposition technique. The samples were characterized by X-ray diffraction, energy-dispersive spectroscopy, transmission electron microscopy, and UV–vis diffuse reflectance spectroscopy, and the results demonstrated that the Au and Pt nanoparticles (7–15 nm) were well-dispersed on the surfaces of g-C3N4. The Au/Pt codecorated g-C3N4 heterostructure displayed enhanced photocatalytic activity for antibiotic tetracycline hydrochloride (TC-HCl) degradation, and the degradation rate was 3.4 times higher than that of pure g-C3N4 under visible light irradiation. The enhancement of photocatalytic activity could be attributed to the surface plasmon resonance effect of Au and electron-sink function of Pt nanoparticles, which improve the optical absorption property and photogenerated charge carriers separation of g-C3N4, synergistically facilitating the photocatalysis process. Finally, a possible photocatalytic mechanism for degr...

553 citations


Journal ArticleDOI
TL;DR: Wearable electronics are fabricated with implanted sensors that can monitor diverse human motions, including joint movement, phonation, swallowing, and breathing, and can detect both large- and small-scale human motions.
Abstract: Because of their outstanding electrical and mechanical properties, graphene strain sensors have attracted extensive attention for electronic applications in virtual reality, robotics, medical diagnostics, and healthcare Although several strain sensors based on graphene have been reported, the stretchability and sensitivity of these sensors remain limited, and also there is a pressing need to develop a practical fabrication process This paper reports the fabrication and characterization of new types of graphene strain sensors based on stretchable yarns Highly stretchable, sensitive, and wearable sensors are realized by a layer-by-layer assembly method that is simple, low-cost, scalable, and solution-processable Because of the yarn structures, these sensors exhibit high stretchability (up to 150%) and versatility, and can detect both large- and small-scale human motions For this study, wearable electronics are fabricated with implanted sensors that can monitor diverse human motions, including joint mov

504 citations


Journal ArticleDOI
TL;DR: An easy and flexible two-step method consisting of hydrothermal and subsequent annealing process have been developed to synthesize the porous 3-D flower-like Co/CoO and it is found that the suitable heat treatment temperature played a vital role on the flower- like structure, composition, and electromagnetic absorption properties.
Abstract: The porous three-dimensional (3-D) flower structures assembled by numerous ultrathin flakes were favor for strengthen electromagnetic absorption capability. However, it still remains a big challenge to fabricate such kind of materials. In this study, an easy and flexible two-step method consisting of hydrothermal and subsequent annealing process have been developed to synthesize the porous 3-D flower-like Co/CoO. Interestingly, we found that the suitable heat treatment temperature played a vital role on the flower-like structure, composition, and electromagnetic absorption properties. In detail, only in the composite treated with 400 °C can we gain the porous 3-D flower structure. If the annealing temperature were heated to 300 °C, the Co element was unable to generate. Moreover, when the annealing temperature increased from 400 to 500 °C, these flower-like structures were unable to be kept because the enlarged porous diameter would wreck the flower frame. Moreover, these 3-D porous flower-like structures...

Journal ArticleDOI
TL;DR: This successful fabrication of a robust, anti-icing, UV-durable, and anticorrosion superhydrophobic surface could yield a prospective candidate for various practical applications.
Abstract: A superhydrophobic steel surface was prepared through a facile method: combining hydrogen peroxide and an acid (hydrochloric acid or nitric acid) to obtain hierarchical structures on steel, followed by a surface modification treatment. Empirical grid maps based on different volumes of H2O2/acid were presented, revealing a wettability gradient from “hydrophobic” to “rose effect” and finally to “lotus effect”. Surface grafting has been demonstrated to be realized only on the oxidized area. As-prepared superhydrophobic surfaces exhibited excellent anti-icing properties according to the water-dripping test under overcooled conditions and the artificial “steam-freezing” (from 50 °C with 90% humidity to the −20 °C condition) test. In addition, the surfaces could withstand peeling with 3M adhesive tape at least 70 times with an applied pressure of 31.2 kPa, abrasion by 400 grid SiC sandpaper for 110 cm under 16 kPa, or water impacting for 3 h without losing superhydrophobicity, suggesting superior mechanical dur...

Journal ArticleDOI
TL;DR: The established heterojunction between the interfaces of TiO2 nanoparticles and g-C3N4 nanosheets as well as introduced Ti(3+) led to the rapid electron transfer rate and improved photoinduced electron-hole pair's separation efficiency, resulting in the improved photocatalytic performance of the Ti( 3+) self-doped TiO 2/g-C 3N4 heterojunctions.
Abstract: A simple one-step calcination route was used to prepare Ti3+ self-doped TiO2/g-C3N4 heterojunctions by mixture of H2Ti3O7 and melamine. X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), electron spin resonance (ESR) spectroscopy, and UV–Vis diffuse reflectance spectroscopy (UV–vis DRS) technologies were used to characterize the structure, crystallinity, morphology, and chemical state of the as-prepared samples. The absorption of the prepared Ti3+ self-doped TiO2/g-C3N4 heterojunctions shifted to a longer wavelength region in comparison with pristine TiO2 and g-C3N4. The photocatalytic activities of the heterojunctions were studied by degrading methylene blue under a 30 W visible-light-emitting diode irradiation source. The visible-light photocatalytic activities enhanced by the prepared Ti3+ self-doped TiO2/g-C3N4 heterojunctions were observed and proved to be better than that of pure TiO2 and ...

Journal ArticleDOI
TL;DR: The study widens the application of monolayer Ti2CO2 not only as the battery material, but also as the potential gas sensor or capturer of NH3 with high sensitivity and selectivity.
Abstract: Ti2C is one of the thinnest layers in MXene family with high potential for applications. In the present study, the adsorption of NH3, H2, CH4, CO, CO2, N2, NO2, and O2 on monolayer Ti2CO2 was investigated by using first-principles simulations to exploit its potential applications as gas sensor or capturer. Among all the gas molecules, only NH3 could be chemisorbed on Ti2CO2 with apparent charge transfer of 0.174 e. We further calculated the current–voltage (I–V) relation using the nonequilibrium Green’s function (NEGF) method. The transport feature exhibits distinct responses with a dramatic change of I–V relation before and after NH3 adsorption on Ti2CO2. Thus, we predict that Ti2CO2 could be a promising candidate for the NH3 sensor with high selectivity and sensitivity. On the other hand, the adsorption of NH3 on Ti2CO2 could be further strengthened with the increase of applied strain on Ti2CO2, while the adsorption of other gases on Ti2CO2 is still weak under the same strain, indicating that the captur...

Journal ArticleDOI
TL;DR: Centrifugally cast films retain bright photoluminescence and achieve dense and homogeneous morphologies and offer a platform for optoelectronic applications of perovskite quantum dot solids.
Abstract: Nanocrystals of CsPbX3 perovskites are promising materials for light-emitting optoelectronics because of their colloidal stability, optically tunable bandgap, bright photoluminescence, and excellent photoluminescence quantum yield. Despite their promise, nanocrystal-only films of CsPbX3 perovskites have not yet been fabricated; instead, highly insulating polymers have been relied upon to compensate for nanocrystals’ unstable surfaces. We develop solution chemistry that enables single-step casting of perovskite nanocrystal films and overcomes problems in both perovskite quantum dot purification and film fabrication. Centrifugally cast films retain bright photoluminescence and achieve dense and homogeneous morphologies. The new materials offer a platform for optoelectronic applications of perovskite quantum dot solids.

Journal ArticleDOI
TL;DR: This work designs, fabricate, and characterize photopatterned, self-folding functional microgrippers that combine a swellable, photo-cross-linked pNIPAM-AAc soft-hydrogel with a nonswellable and stiff segmented polymer (polypropylene fumarate, PPF).
Abstract: Hydrogels such as poly(N-isopropylacrylamide-co-acrylic acid) (pNIPAM-AAc) can be photopatterned to create a wide range of actuatable and self-folding microstructures. Mechanical motion is derived from the large and reversible swelling response of this cross-linked hydrogel in varying thermal or pH environments. This action is facilitated by their network structure and capacity for large strain. However, due to the low modulus of such hydrogels, they have limited gripping ability of relevance to surgical excision or robotic tasks such as pick-and-place. Using experiments and modeling, we design, fabricate, and characterize photopatterned, self-folding functional microgrippers that combine a swellable, photo-cross-linked pNIPAM-AAc soft-hydrogel with a nonswellable and stiff segmented polymer (polypropylene fumarate, PPF). We also show that we can embed iron oxide (Fe2O3) nanoparticles into the porous hydrogel layer, allowing the microgrippers to be responsive and remotely guided using magnetic fields. Usi...

Journal ArticleDOI
TL;DR: GO-Ag nanocomposite, as a kind of antibacterial material, had a great promise for application in a wide range of biomedical applications and was demonstrated to have good cytocompatibility and antibacterial properties.
Abstract: In this work, we report a facile and green approach to prepare a uniform silver nanoparticles (AgNPs) decorated graphene oxide (GO) nanocomposite (GO-Ag). The nanocomposite was fully characterized by transmission electron microscopy (TEM), Fourier transform infrared (FTIR) spectra, ultraviolet–visible (UV–vis) absorption spectra, and X-ray photoelectron spectroscopy (XPS), which demonstrated that AgNPs with a diameter of approximately 22 nm were uniformly and compactly deposited on GO. To investigate the silver ion release behaviors, HEPES buffers with different pH (5.5, 7, and 8.5) were selected and the mechanism of release actions was discussed in detail. The cytotoxicity of GO-Ag nanocomposite was also studied using HEK 293 cells. GO-Ag nanocomposite displayed good cytocompatibility. Furthermore, the antibacterial properties of GO-Ag nanocomposite were studied using Gram-negative E. coli ATCC 25922 and Gram-positive S. aureus ATCC 6538 by both the plate count method and disk diffusion method. The nanoc...

Journal ArticleDOI
Yulong Ying1, Yu Liu1, Xinyu Wang1, Yiyin Mao1, Wei Cao1, Pan Hu1, Xinsheng Peng1 
TL;DR: These reductive 2-D Ti3C2Tx nanosheets are generally explored to remove other oxidant agents, such as K3[Fe(CN)6], KMnO4, and NaAuCl4 solutions, by converting them to low oxidation states.
Abstract: Two dimensional (2-D) Ti3C2Tx nanosheets are obtained by etching bulk Ti3C2Tx powders in HF solution and delaminating ultrasonically, which exhibit excellent removal capacity for toxic Cr(VI) from water, due to their high surface area, well dispersibility, and reductivity. The Ti3C2Tx nanosheets delaminated by 10% HF solution present more efficient Cr(VI) removal performance with capacity of 250 mg g–1, and the residual concentration of Cr(VI) in treated water is less than 5 ppb, far below the concentration (0.05 ppm) of Cr(VI) in the drinking water standard recommended by the World Health Organization. This kind of 2-D Ti3C2Tx nanosheet can not only remove Cr(VI) rapidly and effectively in one step from aqueous solution by reducing Cr(VI) to Cr(III) but also adsorb the reduced Cr(III) simultaneously. Furthermore, these reductive 2-D Ti3C2Tx nanosheets are generally explored to remove other oxidant agents, such as K3[Fe(CN)6], KMnO4, and NaAuCl4 solutions, by converting them to low oxidation states. These...

Journal ArticleDOI
TL;DR: This work demonstrates the versatile and single-step synthesis of ZnO-T with different arm morphologies by a simple flame transport synthesis (FTS) approach, forming a network that will be of interest for various advanced applications.
Abstract: Growth of freestanding nano- and microstructures with complex morphologies is a highly desired aspect for real applications of nanoscale materials in various technologies. Zinc oxide tetrapods (ZnO-T), which exhibit three-dimensional (3D) shapes, are of major importance from a technological applications point of view, and thus efficient techniques for growth of different varieties of tetrapod-based networks are demanded. Here, we demonstrate the versatile and single-step synthesis of ZnO-T with different arm morphologies by a simple flame transport synthesis (FTS) approach, forming a network. Morphological evolutions and structural intactness of these tetrapods have been investigated in detail by scanning electron microscopy, X-ray diffraction, and micro-Raman measurements. For a deeper understanding of the crystallinity, detailed high-resolution transmission electron microscopic studies on a typical ZnO tetrapod structure are presented. The involved growth mechanism for ZnO tetrapods with various arm mor...

Journal ArticleDOI
TL;DR: Nitrogen and sulfur codoped carbon dots prepared from garlic by a hydrothermal method demonstrated to possess good water dispersibility, strong blue fluorescence emission, and excellent photo and pH stabilities, and could be used as an excellent fluorescent probe for cellular multicolor imaging.
Abstract: Nitrogen and sulfur codoped carbon dots (CDs) were prepared from garlic by a hydrothermal method. The as-prepared CDs possess good water dispersibility, strong blue fluorescence emission with a fluorescent quantum yield of 17.5%, and excellent photo and pH stabilities. It is also demonstrated that the fluorescence of CDs are resistant to the interference of metal ions, biomolecules, and high ionic strength environments. Combining with low cytotoxicity properties, CDs could be used as an excellent fluorescent probe for cellular multicolor imaging. Moreover, the CDs were also demonstrated to exhibit favorable radical scavenging activity.

Journal ArticleDOI
TL;DR: Although PPy@PANI composites herein consume the incident electromagnetic wave by absolute dielectric loss, their performances are still superior or comparable to most PANI-based composites ever reported, indicating that they can be taken as a new kind of promising lightweight microwave absorbers.
Abstract: Highly uniform core–shell composites, polypyrrole@polyaniline (PPy@PANI), have been successfully constructed by directing the polymerization of aniline on the surface of PPy microspheres. The thickness of PANI shells, from 30 to 120 nm, can be well controlled by modulating the weight ratio of aniline and PPy microspheres. PPy microspheres with abundant carbonyl groups have very strong affinity to the conjugated chains of PANI, which is responsible for the spontaneous formation of uniform core–shell microstructures. However, the strong affinity between PPy microspheres and PANI shells does not promote the diffusion or reassembly of two kinds of conjugated chains. Coating PPy microspheres with PANI shells increases the complex permittivity and creates the mechanism of interfacial polarization, where the latter plays an important role in increasing the dielectric loss of PPy@PANI composites. With a proper thickness of PANI shells, the moderate dielectric loss will produce well matched characteristic impedanc...

Journal ArticleDOI
TL;DR: Both G-CNTm and GNm possessed excellent antifouling performance for SA and HA but inferior for BSA because of the strong interaction between protein and graphene sheets.
Abstract: A sort of novel high-flux nanofiltration membrane was fabricated by synergistic assembling of graphene and multiwalled carbon nanotubes (MWNTs), in which graphene played the role of molecular sieving and MWNTs expanded the interlayer space between neighbored graphene sheets. The MWNT-intercalated graphene nanofiltration membrane (G-CNTm) showed a water flux up to 11.3 L m(-2) h(-1) bar(-1), more than 2 times that of the neat graphene nanofiltration membrane (GNm), while keeping high dye rejection (>99% for Direct Yellow and >96% Methyl Orange). The G-CNTm also showed good rejection ratio for salt ions (i.e., 83.5% for Na2SO4, 51.4% for NaCl). We also explored the antifouling performance of G-CNTm and GNm with bovine serum albumin (BSA), sodium alginate (SA) and humic acid (HA). Both G-CNTm and GNm possessed excellent antifouling performance for SA and HA but inferior for BSA because of the strong interaction between protein and graphene sheets.

Journal ArticleDOI
TL;DR: The calculations show that free-standing α and β allotropes of antimonene are stable and semiconducting, which opens up the possibility of their applications in optoelectronics.
Abstract: Group V elemental monolayers including phosphorene are emerging as promising 2D materials with semiconducting electronic properties. Here, we present the results of first-principles calculations on stability, mechanical and electronic properties of 2D antimony (Sb), antimonene. Our calculations show that free-standing α and β allotropes of antimonene are stable and semiconducting. The α-Sb has a puckered structure with two atomic sublayers and β-Sb has a buckled hexagonal lattice. The calculated Raman spectra and STM images have distinct features thus facilitating characterization of both allotropes. The β-Sb has nearly isotropic mechanical properties, whereas α-Sb shows strongly anisotropic characteristics. An indirect–direct band gap transition is expected with moderate tensile strains applied to the monolayers, which opens up the possibility of their applications in optoelectronics.

Journal ArticleDOI
TL;DR: A facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors is reported, which provides an alternative route toward high efficient solution-processed perovSkite-based light-emitting diodes.
Abstract: We report a facile nonaqueous emulsion synthesis of colloidal halide perovskite quantum dots by controlled addition of a demulsifier into an emulsion of precursors. The size of resulting CH3NH3PbBr3 quantum dots can be tuned from 2 to 8 nm by varying the amount of demulsifier. Moreover, this emulsion synthesis also allows the purification of these quantum dots by precipitation from the colloidal solution and obtains solid-state powder which can be redissolved for thin film coating and device fabrication. The photoluminescence quantum yields of the quantum dots is generally in the range of 80–92%, and can be well-preserved after purification (∼80%). Green light-emitting diodes fabricated comprising a spin-cast layer of the colloidal CH3NH3PbBr3 quantum dots exhibited maximum current efficiency of 4.5 cd/A, power efficiency of 3.5 lm/W, and external quantum efficiency of 1.1%. This provides an alternative route toward high efficient solution-processed perovskite-based light-emitting diodes. In addition, the...

Journal ArticleDOI
TL;DR: A facile, effective, and scalable strategy by a deposition-precipitation method to fabricate metal-doped (Fe, Co, Ni) molybdenum sulfide with a few layers on carbon black as noble metal-free electrocatalysts for HER.
Abstract: Highly active and low-cost catalysts for hydrogen evolution reaction (HER) are crucial for the development of efficient water splitting. Molybdenum disulfide (MoS2) nanosheets possess unique physical and chemical properties, which make them promising candidates for HER. Herein, we reported a facile, effective, and scalable strategy by a deposition–precipitation method to fabricate metal-doped (Fe, Co, Ni) molybdenum sulfide with a few layers on carbon black as noble metal–free electrocatalysts for HER. The CoMoS phase after thermal annealing in Co-doped MoS2 plays a crucial role for the enhanced HER. The optimized Co-doped MoS2 catalyst shows superior HER performance with a high exchange current density of 0.03 mA·cm–2, low onset potential of 90 mV, and small Tafel slope of 50 mV·dec–1, which also exhibits excellent stability of 10000 cycles with negligible loss of the cathodic current. The superior HER activity originates from the synergistically structural and electronic modulations between MoS2 and Co ...

Journal ArticleDOI
TL;DR: The PU@Fe3O4@SiO2@FP sponges could be used as membranes for oil/water separation and for continuous separation of large amounts of oil pollutants from the water surface with the help of a pump.
Abstract: Magnetic, durable, and superhydrophobic polyurethane (PU) sponges were fabricated by chemical vapor deposition (CVD) of tetraethoxysilane (TEOS) to bind the Fe3O4 nanoparticles tightly on the sponge and then dip-coating in a fluoropolymer (FP) aqueous solution. The sponges were characterized using scanning electron microscopy and other analytical techniques. The effects of CVD time of TEOS and FP concentration on wettability, mechanical properties, oil absorbency, and oil/water selectivity of the sponges were also investigated. The sponges exhibit fast magnetic responsivity and excellent superhydrophobicity/superoleophilicity (CAwater = 157° and CAoil ≈ 0°). The sponges also show very high efficiency in oil/water separation and could, driven by a magnet, quickly absorb floating oils on the water surface and heavy oils under water. Moreover, the PU@Fe3O4@SiO2@FP sponges could be used as membranes for oil/water separation and for continuous separation of large amounts of oil pollutants from the water surfac...

Journal ArticleDOI
Heng Shen1, Jing Guo1, Hao Wang1, Ning Zhao1, Jian Xu1 
TL;DR: D dopamine chemistry has been used to achieve the facile surface modification of h-BN microplatelets by forming a polydopamine (PDA) shell on its surface.
Abstract: With the development of microelectronic technology, the demand of insulating electronic encapsulation materials with high thermal conductivity is ever growing and much attractive. Surface modification of chemical inert h-BN is yet a distressing issue which hinders its applications in thermal conductive composites. Here, dopamine chemistry has been used to achieve the facile surface modification of h-BN microplatelets by forming a polydopamine (PDA) shell on its surface. The successful and effective preparation of h-BN@PDA microplatelets has been confirmed by SEM, EDS, TEM, Raman spectroscopy, and TGA investigations. The PDA coating increases the dispersibility of the filler and enhances its interaction with PVA matrix as well. Based on the combination of surface modification and doctor blading, composite films with aligned h-BN@PDA are fabricated. The oriented fillers result in much higher in-plane thermal conductivities than the films with disordered structures produced by casting or using the pristine h...

Journal ArticleDOI
Zhenwei Tong, Dong Yang1, Jiafu Shi1, Yanhu Nan1, Yuanyuan Sun1, Zhongyi Jiang1 
TL;DR: The photocatalyst exploited in this study may become an attractive material in many environmental and energy related applications.
Abstract: It is curial to develop a high-efficient, low-cost visible-light responsive photocatalyst for the application in solar energy conversion and environment remediation. Here, a three-dimensional (3D) porous g-C3N4/graphene oxide aerogel (CNGA) has been prepared by the hydrothermal coassembly of two-dimensional g-C3N4 and graphene oxide (GO) nanosheets, in which g-C3N4 acts as an efficient photocatalyst, and GO supports the 3D framework and promotes the electron transfer simultaneously. In CNGA, the highly interconnected porous network renders numerous pathways for rapid mass transport, strong adsorption and multireflection of incident light; meanwhile, the large planar interface between g-C3N4 and GO nanosheets increases the active site and electron transfer rate. Consequently, the methyl orange removal ratio over the CNGA photocatalyst reaches up to 92% within 4 h, which is much higher than that of pure g-C3N4 (12%), 2D hybrid counterpart (30%) and most of representative g-C3N4-based photocatalysts. In addi...

Journal ArticleDOI
TL;DR: The performance of solution exfoliated MoS2 thin flexible membranes as supercapacitor electrodes in a symmetrical coin cell arrangement using an aqueous electrolyte (Na2SO4) demonstrates a simple and scalable application of layered 2D materials toward electrochemical energy storage.
Abstract: Two-dimensional materials, such as graphene and molybdenum disulfide (MoS2), can greatly increase the performance of electrochemical energy storage devices because of the combination of high surface area and electrical conductivity. Here, we have investigated the performance of solution exfoliated MoS2 thin flexible membranes as supercapacitor electrodes in a symmetrical coin cell arrangement using an aqueous electrolyte (Na2SO4). By adding highly conductive graphene to form nanocomposite membranes, it was possible to increase the specific capacitance by reducing the resistivity of the electrode and altering the morphology of the membrane. With continued charge/discharge cycles the performance of the membranes was found to increase significantly (up to 800%), because of partial re-exfoliation of the layered material with continued ion intercalation, as well as increasing the specific capacitance through intercalation pseudocapacitance. These results demonstrate a simple and scalable application of layered...

Journal ArticleDOI
Xiao-Yu Xu1, Bing Yan1
TL;DR: Remarkably, it is the first Eu-doped MOF to exhibit an excellent ability for the detection of Fe(3+) and Fe(2+) in an aqueous environment without any structural disintegration of the framework.
Abstract: A layerlike MOF (MIL-124, orGa2(OH)4(C9O6H4)) has been prepared and chosen as a parent compound to encapsulate Eu3+ cations by one uncoordinated carbonyl group in its pores. The Eu3+-incorporated sample (Eu3+@MIL-124) is fully characterized, which shows excellent luminescence and good fluorescence stability in water or other organic solvents. Subsequently, we choose Eu3+@MIL-124 as sensitive probe for sensing metal ions, anions, and organic small molecules because of its robust framework. Studying of the luminescence properties reveals that the complex Eu3+@MIL-124 was developed as a highly selective and sensitive probe for detection of Fe3+ (detection limit, 0.28 μM) and Fe2+ ions through fluorescence quenching of Eu3+ and MOF over other metal ions. In connection to this, a probable sensing mechanism was also discussed in this paper. In addition, when Eu3+@MIL-124 was immersed in the different anions solutions and organic solvents, it also shows highly selective for Cr2O72–(detection limit, 0.15 μM)and a...