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We report a remarkably rapid method for assembling pristine graphene platelets into a large area transparent film at a liquid surface. Some 2-3 layer pristine graphene platelets temporally solvated with N-methyl-2-pyrrolidone (NMP) are assembled at the surface of a dilute aqueous suspension using an evaporation-driven Rayleigh-Taylor instability and then are driven together by Marangoni forces. The platelets are fixed through physical binding of their edges. Typically, 8-cm-diameter circular graphene films are generated within two minutes. Once formed, the films can be transferred onto various substrates with flat or textured topologies. This interfacial assembly protocol is generally applicable to other nanomaterials, including 0D fullerene and 1D carbon nanotubes, which commonly suffer from limited solution compatibility.
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Counterfeiting is conducted in almost every industry, and the losses caused by it are growing as today's world trade continues to increase. In an attempt to provide an efficient method to fight such counterfeiting, we herein demonstrate anti-counterfeit nanoscale fingerprints generated by randomly distributed nanowires. Specifically, we prepare silver nanowires coated with fluorescent dyes and cast them onto the surface of transparent PET film. The resulting non-repeatable patterns characterized by the random location of the nanowires and their fluorescent colors provide unique barcodes suitable for anti-counterfeit purposes. Counterfeiting such a fingerprint pattern is impractical and expensive; the cost of replicating it would be higher than the value of the typical target item being protected. Fingerprint patterns can be visually authenticated in a simple and straightforward manner by using an optical microscope. The concept of generating unique patterns by randomness is not limited to the materials shown in this paper and should be readily applicable to other types of materials.
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Directed self-assembly of a block copolymer is successfully employed to fabricate device-oriented graphene nanostructures from CVD grown graphene. We implemented mussel-inspired polydopamine adhesive in conjunction with the graphoepitaxy principle to tailor graphene nanoribbon arrays and a graphene nanomesh located between metal electrodes. Polydopamine adhesive was utilized for facile and damage-free surface treatment to complement the low surface energy of pristine graphene. Our process minimizes the damage to the ideal graphitic structures and electrical properties of graphene during the nanopatterning process. Multi-channel graphene nanoribbon arrays and a graphene nanomesh were successfully fabricated between metal electrodes.
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Polymer grafting from graphitic carbon materials has been pursued for several decades. Unfortunately, currently available methods mostly rely on the harsh chemical treatment of graphitic carbons which causes severe degradation of chemical structure and material properties. A straightforward growth of polyaniline chain from the nitrogen (N)-doped sites of carbon nanotubes (CNTs) is presented. N-doping sites along the CNT wall nucleate the polymerization of aniline, which generates seamless hybrids consisting of polyaniline directly grafted onto the CNT walls. The resultant materials exhibit excellent synergistic electrochemical performance, and can be employed for charge collectors of supercapacitors. This approach introduces an efficient route to hybrid systems consisting of conducting polymers directly grafted from graphitic dopant sites.
Asunto(s)
Compuestos de Anilina/química , Nanotubos de Carbono/química , Nitrógeno/químicaRESUMEN
Surface modification of inorganic nanoparticles is critical for the quality and performance of pigments, cosmetics, and composite materials. We covered the titanium dioxide nanoparticles' surface with 2-(acetoacetoxy) ethyl methacrylate, a polymerizable chelating agent. Through the in situ polymerization procedure, this molecule's ß-ketoester moiety quickly coordinated with the metal atoms on titanium dioxide nanoparticles, and its methacrylate group formed homogeneous coating layers. This coating layer significantly reduced the photocatalytic activity of titanium dioxide nanoparticles and prevented their aggregation. This nanoparticle dispersion showed low viscosity up to the solid content of 60% (w/w) in the liquid dispersant. As a result, it increased the UV screening performance and dispersion stability. Additionally, this coating layer widened the absorption spectrum of titanium dioxide and could change the color of nanoparticles from pale yellow to brown. It can also be helpful for cosmetic applications.
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The synthesis of dual-function molybdenum (Mo)-complex carbonous sponges is reported for elucidating their utilization as positive and negative electrodes in electrochemical devices and their applicability to the active oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in electrocatalytic devices. Molybdenum (Mo)-coordinated polyvinyl alcohol gel is converted into a porous Mo-complex nitrogen-rich carbonous sponge (MNCS) via microwave and low-temperature-annealing processes as a positive electrode. This MNCS was further thermally treated at a higher temperature to prepare a more carbonized Mo-complex N-doped carbon sponge (cMNCS) as a negative electrode. Both sponges were lightweight and porous and exhibited excellent specific capacitances of 562 F g-1 as a positive MNCS electrode and 937 F g-1 as a negative cMNCS electrode. The asymmetric supercapacitor assembled using them reveals a power density of 887.5 W kg-1 at an energy density of 36 Wh kg-1, in addition to a retention rate of >95% after 5000 cycles. We furthermore demonstrate the electrocatalytic capabilities of these materials with overpotentials of -170 and -220 mV for the HER and 1.70 and 1.53 V for the OER at a current density of 10 mA cm-2 using a water-splitting electrocatalyzer.
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Layered double hydroxides (LDHs) have drawn significant interest as emerging active materials for advanced energy storage devices; however, their low electric and ionic conductivity limit their applications. In this study, we report sulfur (S) and phosphorus (P) co-doped NiCo LDH nanoarrays prepared via a facile phosphor-sulfurization process to impart diverse co-doping effects. Combining the benefits of their unique hierarchical structure and reduced charge transfer resistance, the S and P co-doped NiCo LDH (NiCo LDH-SP) nanoarrays realize faster and more efficient redox reactions and achieve enhanced surface reactivity, thereby resulting in a performance superior to that of pristine NiCo LDH. Therefore, a NiCo LDH-SP shows an ultra-high specific capacitance of 3844.8 F g-1 at a current density of 3 A g-1 and maintains a specific capacitance of 2538.8 F g-1 at a high current density of 20 A g-1. Additionally, an asymmetric supercapacitor, assembled with the NiCo LDH-SP as the cathode and activated carbon (AC) as the anode (NiCo LDH-SP//AC), shows a high energy density of 74.5 W h kg-1 at a power density of 0.8 kW kg-1 and outstanding cycling stability, thereby retaining â¼81.3% of its initial specific capacitance after 5000 cycles. This study presents a facile and promising strategy for developing LDH-based electrode materials with excellent electrochemical performance for advanced energy storage applications.
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A electrode for energy storage cells is possible directly on Ni foam, using a simple reduction process to form NiF2 nanorod arrays (NA). We demonstrate NiF2@Ni NA for a symmetric electrochemical supercapattery electrode. With an areal specific capacitance of 51 F cm-2 at 0.25 mA cm-2 current density and 94% cycling stability, a NiF2@Ni electrode can exhibit supercapattery behavior, a combination of supercapacitor and battery-like redox. The symmetric electrochemical supercapattery delivers 31 W h m-2 energy density and 797 W m-2 power density with 83% retention in a 1 M KOH electrolyte, constituting a step toward manufacturing a laboratory-scale energy storage device based on metal halides. Producing self-grown hierarchically porous nanostructured electrodes on three-dimensional metal foams by displacement reactions may be useful for other metal halides as electrodes for supercapacitors, supercapatteries, and lithium-ion batteries.
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The surface characteristics of electrodes vary depending on the solvent used. Furthermore, electrochemical performance varies depending on the surface morphology of the electrode. In this study, we grew 3D binary NiCu-based composites on Ni foam, via a binder-free hydrothermal method, for use as a cathode in high-performance supercapacitors. We employed different solvents to prepare the electrodes by adjusting the ratio of deionized water (DI water) to methanol. The electrode prepared using DI water as the solvent had the largest surface area with a nanowire structure. This morphology allowed for good electrical performance by greatly improving the electrode and electrolyte contact area and shortening the ion diffusion path. The optimized deposition of NiCu(CO3)(OH)2 nanowires (50 mL of DI water as solvent) showed an excellent maximum specific capacity of 758.9 mA h g-1 at a current density of 3 A g-1, as well as outstanding cycling performance with 87.2% retention after 5000 cycles. In this work, we focused on the large specific surface area and suitable electrochemical properties of NiCu(CO3)(OH)2 electrodes with various solvents. As a result, the asymmetric supercapacitor (ASC) using the NiCu(CO3)(OH)2 electrode prepared with 50 ml of DI water as the solvent as the positive electrode and graphene as the negative electrode, exhibited an energy density of 26.7 W h kg-1 at a power density of 2534 W kg-1, and excellent cycling stability with 91.3% retention after 5000 cycles. The NiCu(CO3)(OH)2//graphene ASC could turn on an LED light and demonstrated better electrical performance than most previously reported nickel- and copper-based carbonate hydroxide ASCs. In addition, in the present scenario where many nanoscale studies are conducted, a method of controlling the nanostructure of a material through facile solvent control will be of great help to many researchers.
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A dual phase bismuth oxyiodide (BiOI/Bi9I2) nanostructure battery type supercapacitor electrode is synthesized using chemical bath deposition (CBD) and the capacitance and energy/power density (ED/PD) reported. The supercapacitor electrode BiOI/Bi9I2 exhibited a specific capacitance of 515.5 F g-1 (capacity value 143 mA h g-1) at a current density of 2 A g-1, with 80% of the original capacitance retained, even at a high current density of 4 A g-1 over 5000 cycles. A pouch-type symmetric supercapacitor (PSS) device was created, based on BiOI/Bi9I2//BiOI/Bi9I2 electrodes (acting as anode and cathode electrodes) with 6 M KOH as the aqueous electrolyte and with an extended voltage up to 1.5 V. The ED value was 38.2 W h kg-1 at a current density of 2 A g-1, and the PD was 2280.4 W·kg-1. Three PSS type BiOI/Bi9I2//BiOI/Bi9I2 devices were connected in series and used to illuminate a red LED for 20 min with full brightness, confirming potential use as an energy storage device. The above summarized results indicate that BiOI/Bi9I2//BiOI/Bi9I2 could be a potential electrode for battery type supercapacitor applications.
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A simple, room-temperature operable, glycerol-supported single beaker-inspired, and binder-free soft-chemical protocol has been developed to synthesize 3-D dandelion flower-type nickel chloride (NiCl2) supercapattery (supercapacitor + battery) nanostructured electrode material from solid 3-D nickel-foam (NiF). The dandelion flower-type NiCl2@NiF labeled as B electrode, demonstrates a battery-type electrochemical performance as obtained 1551 F·g-1 specific capacitance (SC) and 95% cyclability over 50,000 cycles is higher than that of a setaria viridis-type NiCl2@NiF electrode, prepared without glycerol labeled as A electrode. As a commercial market product, assembled NiCl2@NiF@ (cathode)// BiMoO3 (anode) pouch-type asymmetric supercapacitor energy storage device demonstrates moderate energy density and power density (28 Wh·kg-1 and 845 W·kg-1). By utilizing three devices in series, three different colored LEDs can be operated at full brightness. The as-proposed low temperature protocol impeccably effective and efficient on account of the low-cost, easy synthesis methodology for scalability, and high crytallinity as well as solvent-free and non-toxic as pyrolated gases were used while synthesis processing.
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Room-temperature (27 °C) synthesis and carbon dioxide (CO2)-gas-sensor applications of bismuth oxide (Bi2O3) nanosensors obtained via a direct and superfast chemical-bath-deposition method (CBD) with different surface areas and structures, i.e., crystallinities and morphologies including a woollen globe, nanosheet, rose-type, and spongy square plate on a glass substrate, are reported. Moprhologies of the Bi2O3 nanosensors are tuned through polyethylene glycol, ethylene glycol, and ammonium fluoride surfactants. The crystal structure, type of crystallinity, and surface appearance are determined from the X-ray diffraction patterns, X-ray photoelectron spectroscopy spectra, and high-resolution transmission electron microscopy images. The room-temperature gas-sensor applications of these Bi2O3 nanosensors for H2, H2S, NO2, SO2, and CO2 gases are monitored from 10 to 100 ppm concentrations, wherein Bi2O3 nanosensors of different physical properties demonstrate better performance and response/recovery time measurement for CO2 gas than those for the other target gases employed. Among various sensor morphologies, the nanosheet-type Bi2O3 sensor has exhibited at 100 ppm concentration of CO2 gas, a 179% response, 132 s response time, and 82 s recovery time at room-temperature, which is credited to its unique surface morphology, high surface area, and least charge transfer resistance. This suggests that the importance of the surface morphology, surface area, and crystallinity of the Bi2O3 nanosensors used for designing room-temperature operable CO2 gas sensors for commercial benefits.
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The specific capacitance and energy density of antimony trisulfide (Sb2S3)@carbon supercapacitors (SCs) have been limited and are in need of significant improvement. In this work, Sb2S3 nanoparticles were selectively encapsulated or anchored in a sulfur-doped carbon (S-carbon) sheet depending on the use of microwave-assisted synthesis. The microwave-triggered Sb2S3 nanoparticle growth resulted in core-shell hierarchical spherical particles of uniform diameter assembled with Sb2S3 as the core and an encapsulated S-carbon layer as the shell (Sb2S3-M@S-C). Without the microwave mediation, the other nanostructure was found to comprise fine Sb2S3 nanoparticles widely anchored in the S-carbon sheet (Sb2S3-P@S-C). Structural and morphological analyses confirmed the presence of encapsulated and anchored Sb2S3 nanoparticles in the carbon. These two materials exhibited higher specific capacitance values of 1179 (0 to +1.0 V) and 1380 F·g-1 (-0.8 to 0 V) at a current density of 1 A·g-1, respectively, than those previously reported for Sb2S3 nanomaterials in considerable SCs. Furthermore, both materials exhibited outstanding reversible capacitance and cycle stability when used as SC electrodes while retaining over 98% of the capacitance after 10 000 cycles, which indicates their long-term stability. Furthermore, a hybrid Sb2S3-M@S-C/Sb2S3-P@S-C device was designed, which delivers a remarkable energy density of 49 W·h·kg-1 at a power density of 2.5 kW·kg-1 with long-term cycle stability (94% over 10 000 cycles) and is comparable to SCs in the recent literature. Finally, a light-emitting diode (LED) panel comprising 32 LEDs was powered using three pencil-type hybrid SCs in series.
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We report water-splitting application of chemically stable self-grown nickel sulfide (Ni x S y ) electrocatalysts of different nanostructures including rods, flakes, buds, petals, etc., synthesized by a hydrothermal method on a three-dimensional Ni foam (NiF) in the presence of different sulfur-ion precursors, e.g., thioacetamide, sodium thiosulfate, thiourea, and sodium sulfide. The S2- ions are produced after decomposition from respective sulfur precursors, which, in general, react with oxidized Ni2+ ions from the NiF at optimized temperatures and pressures, forming the Ni x S y superstructures. These Ni x S y electrocatalysts are initially screened for their structure, morphology, phase purity, porosity, and binding energy by means of various sophisticated instrumentation technologies. The as-obtained Ni x S y electrocatalyst from sodium thiosulfate endows an overpotential of 200 mV. The oxygen evolution overpotential results of Ni x S y electrocatalysts are comparable or superior to those reported previously for other self-grown Ni x S y superstructure morphologies.
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Soft chemical synthesis is used to obtain a hydrangea-type bismuth molybdate (Bi2MoO6) supercapattery electrode that demonstrates considerable energy/power density and cycling life. Structure and morphology studies, initially, reveal a phase-pure polycrystalline and hydrangea-type surface appearance for Bi2MoO6, which upon testing in an electrochemical energy storage system displays supercapattery behavior, a combination of a supercapacitor and a battery. From the power law, an applied-potential-dependent charge storage mechanism is established for the Bi2MoO6 electrode material. A Trasatti plot evidences the presence of inner and outer surface charges. The hydrangea-type Bi2MoO6 electrode demonstrates a specific capacitance of 485 F g-1 at 5 A g-1 and a stability of 82% over 5000 cycles. An assembled symmetric supercapattery with a Bi2MoO6//Bi2MoO6 configuration demonstrates energy and power densities of 45.6 W h kg-1 and 989 W kg-1, respectively. A demonstration elucidating the lighting up of three light-emitting diodes, connected in series, by the symmetric supercapattery signifies the practical potentiality of the as-synthesized hydrangea-type Bi2MoO6 electrode in energy storage devices.
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Sulphur source-inspired self-grown polycrystalline and mesoporous nickel sulfide (Ni xS y) superstructures with vertically aligned nanomorphologies viz. rods, flakes, buds, and petals, synthesized at elevated temperatures and moderate pressures by a facile one-pot hydrothermal method on a three-dimensional Ni foam demonstrate remarkable areal specific capacitances of 7152, 4835, and 2160 F cm-2 at current densities of 1, 2, and 5 mA cm-2, respectively, with a cycling stability of 94% for a battery-type electrochemical supercapacitor when used as an electrode material in a supercapacitor. The Ni xS y//Bi2O3 asymmetric supercapacitor assembly exhibits an energy density of 41 W h·kg-1 at a power density of 1399 W kg-1 for 1 A g-1 and was used in a three-cell series combination to operate a "GFHIM" display panel (our research institute name, Global Frontier R & D Center for Hybrid Interface Materials) composed of nearly 50 differently colored light-emitting diodes with high intensity in 1 M KOH water-alkali electrolyte. The electrochemical supercapacitor results obtained for the Ni xS y superstructures because of a combination of catalytically active amorphous and high mobility polycrystalline are highly comparable to those reported previously for salt-mediated and self-grown Ni xS y structures and morphologies.
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In the current study, we have explored the coupling of Bi2O3 negative electrode and MnO2 positive electrode materials as an asymmetric faradaic assembly for a high-performance hybrid electrochemical energy storage device (HEESD). Aiming at a low-cost device, both the electrodes have been synthesized by a simple, scalable, and cost-effective chemical synthesis method. After their requisite structure-morphological confirmation and correlation, these electrodes were separately examined for their electrochemical performance in a three-electrode configuration. The results obtained confirm that Bi2O3 and MnO2 exhibit 910 C g-1 and 424 C g-1 specific capacity, respectively, at 2 A g-1 current density. Notably, the performance of both electrodes has been analyzed using Dunn's method to highlight the distinct nature of their faradaic properties. Afterwards, the asymmetric faradaic assembly of both electrodes, when assembled as a HEESD (MnO2//Bi2O3), delivered 411 C g-1 specific capacity at 1 A g-1 current density due to the inclusive contribution from the capacitive as well as the non-capacitive faradaic quotient. Consequently, the assembly offers an excellent energy density of 79 W h kg-1 at a power density of 702 W kg-1, with a magnificent retention of energy density up to 21.1 W h kg-1 at 14 339 W kg-1 power density. Moreover, it demonstrates long-term cycling stability at 10 A g-1, retaining 85.2% of its initial energy density after 5000 cycles, which is significant in comparison with the previously reported literature. Additionally, to check the performance of the device in real time, two HEESDs were connected in series to power a light-emitting diode. The results obtained provide significant insight into hybrid coupling, where two different faradaic electrodes can be combined in a synergistic combination for a high-performance HEESD.
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Superfast (≤10 min) room-temperature (300 K) chemical synthesis of three-dimensional (3-D) polycrystalline and mesoporous bismuth(III) oxide (Bi2O3) nanostructured negatrode (as an abbreviation of negative electrode) materials, viz., coconut shell, marigold, honey nest cross section and rose with different surface areas, charge transfer resistances, and electrochemical performances essential for energy storage, harvesting, and even catalysis devices, are directly grown onto Ni foam without and with poly(ethylene glycol), ethylene glycol, and ammonium fluoride surfactants, respectively. Smaller diffusion lengths, caused by the involvement of irregular crevices, allow electrolyte ions to infiltrate deeply, increasing the utility of inner active sites for the following electrochemical performance. A marigold 3-D Bi2O3 electrode of 58 m2·g-1 surface area has demonstrated a specific capacitance of 447 F·g-1 at 2 A·g-1 and chemical stability of 85% even after 5000 redox cycles at 10 A·g-1 in a 6 M KOH electrolyte solution, which were higher than those of other morphology negatrode materials. An asymmetric supercapacitor (AS) device assembled with marigold Bi2O3 negatrode and manganese(II) carbonate quantum dots/nickel hydrogen-manganese(II)-carbonate (MnCO3QDs/NiH-Mn-CO3) positrode corroborates as high as 51 Wh·kg-1 energy at 1500 W·kg-1 power and nearly 81% cycling stability even after 5000 cycles. The obtained results were comparable or superior to the values reported previously for other Bi2O3 morphologies. This AS assembly glowed a red-light-emitting diode for 20 min, demonstrating the scientific and industrial credentials of the developed superfast Bi2O3 nanostructured negatrodes in assembling various energy storage devices.
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We report the preparation of graphene oxide nanoparticles (GONPs), a metal-free, heterogeneous, non-toxic, reusable and mesoporous green-(acid)-catalyst obtained by sugar carbonization through a micro-wave chemical synthesis method for the synthesis of bio-active benzylpyrazolyl coumarin derivatives (BCDs) under thermal conditions (50 °C) in ethanol solvent. The obtained products were purified by re-crystallization from ethanol, assuring usability of GONPs in multicomponent reactions (MCRs) that could find wide application in the synthesis of a variety of biologically potent molecules of therapeutic significance.
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The structure and morphology of titanium carbide (Ti3C2Tx) MXene, a new class of two dimensional (2D) materials, are investigated and reported. Ti3AlC2 MAX, treated with a hydrofluoric acid etching process, is used as a promising electrode material for electrochemical supercapacitor studies. The electrochemical supercapacitor performance of Ti3C2Tx as a negatrode in a natural seawater electrolyte solution, tested in a three-electrode system, demonstrated a specific capacitance of 67.7 F g-1 at a current density of 1 A g-1 which is in accordance with the volumetric specific capacitance of 121.8 F cm-3. A symmetric supercapacitor assembled with a Ti3C2Tx//Ti3C2Tx electrode configuration revealed a volumetric specific capacitance of 27.4 F cm-3 at 0.25 A g-1, and 96.6% capacitance retention even after 5000 cycles, which is superior to those reported previously in similar systems, suggesting the importance of abundant and cost-effective seawater as a natural electrolyte in developing energy storage devices.