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1.
Nanoscale zero‐valent iron particles supported on reduced graphene oxides (NZVI/rGOs) from spent graphene oxide (GO)‐bound iron ions were developed by using a hydrogen/argon plasma reduction method to improve the reactivity and stability of NZVI. The NZVI/rGOs exhibited excellent water treatment performance with excellent removal capacities of 187.16 and 396.37 mg g?1 for chromium and lead, respectively. Moreover, the NZVI/rGOs could be regenerated by plasma treatment and maintained high removal ability after four cycles. X‐ray photoelectron spectroscopy analysis results implied that the removal mechanisms could be attributed to adsorption/precipitation, reduction, or both. Such multiple removal mechanisms by the NZVI/rGOs were attributed to the reduction ability of the NZVI particles and the role of dispersing and stabilizing abilities of the rGOs. The results indicated that the NZVI/rGOs prepared by a hydrogen/argon plasma reduction method might be an effective composite for heavy‐metal‐ion removal.  相似文献   

2.
Graphene has attracted increasing attention in multidisciplinary studies because of its unique physical and chemical properties. Herein, the adsorption of polycyclic aromatic hydrocarbons (PAHs), such as naphthalene (NAP), anthracene (ANT), and pyrene (PYR), on reduced graphene oxides (rGOs) and graphene oxides (GOs) as a function of pH, humic acid (HA), and temperature were elucidated by means of a batch technique. For comparison, nonpolar and nonporous graphite were also employed in this study. The increasing of pH from 2 to 11 did not influence the adsorption of PAHs on rGOs, whereas the suppressed adsorption of NAP on rGOs was observed both in the presence of HA and under high‐temperature conditions. Adsorption isotherms of PAHs on rGOs were in accordance with the Polanyi–Dubinin–Ashtahhov (PDA) model, providing evidence that pore filling and flat surface adsorption were involved. The saturated adsorbed capacities (in mmol g?1) of rGOs for PAHs calculated from the PDA model significantly decreased in the order of NAP>PYR>ANT, which was comparable to the results of theoretical calculations. The pore‐filling mechanism dominates the adsorption of NAP on rGOs, but the adsorption mechanisms of ANT and PYR on rGOs are flat surface adsorption.  相似文献   

3.
The synthesis of nanoporous graphene by a convenient carbon nanofiber assisted self‐assembly approach is reported. Porous structures with large pore volumes, high surface areas, and well‐controlled pore sizes were achieved by employing spherical silica as hard templates with different diameters. Through a general wet‐immersion method, transition‐metal oxide (Fe3O4, Co3O4, NiO) nanocrystals can be easily loaded into nanoporous graphene papers to form three‐dimensional flexible nanoarchitectures. When directly applied as electrodes in lithium‐ion batteries and supercapacitors, the materials exhibited superior electrochemical performances, including an ultra‐high specific capacity, an extended long cycle life, and a high rate capability. In particular, nanoporous Fe3O4–graphene composites can deliver a reversible specific capacity of 1427.5 mAh g?1 at a high current density of 1000 mA g?1 as anode materials in lithium‐ion batteries. Furthermore, nanoporous Co3O4–graphene composites achieved a high supercapacitance of 424.2 F g?1. This work demonstrated that the as‐developed freestanding nanoporous graphene papers could have significant potential for energy storage and conversion applications.  相似文献   

4.
A new fluorescent hybrid porous polymer (HPP) is synthesized by an anhydrous FeCl3‐mediated oxidative coupling reaction of octa[4‐(9‐carbazolyl)phenyl]silsesquioxane (OCPS). The polymer possesses a surface area of 1741 m2 g?1 and hierarchical bimodal micropores (1.41 and 1.69 nm) and mesopores (2.65 nm). The material serves as an excellent adsorbent for CO2 and dyes with high adsorption capacity for CO2 (8.53 wt %,1.94 mmol g?1), congo red (1715 mg g?1) and rhodamine B (1501 mg g?1). In addition, the presence of peripheral cabozolyl groups with extended π‐conjugation in the crosslinked framework imparts luminescent character to the polymer and offers the detection of nitroaromatic compounds.  相似文献   

5.
High‐quality reduced graphene, termed PG, has been synthesized by a simple, low‐cost, and green plasma approach, and applied as adsorbent to remove 4,4′‐dichloribiphenyl (4,4′‐DCB) from aqueous solutions. As a comparison, the adsorption of 4,4′‐DCB on graphene oxide (GO) and multiwalled carbon nanotubes (MWCNTs) was also studied under the same experimental conditions. PG performs significantly better with regard to 4,4′‐DCB adsorption than GO and MWCNTs, or any reported nanomaterials, with a maximum adsorption capacity (qmax) of 1552 mg g?1 at pH 7.0. The high affinity of 4,4′‐DCB to PG is mainly a result of strong π–π interactions, as also confirmed by DFT calculations. The results reveal that PG sheets hold promise for the removal of persistent organic pollutants. We expect possible applications of this fast and mild plasma technique in the fabrication of nanomaterials and envisage their use in a variety of advanced chemical processes.  相似文献   

6.
Metal–organic framework‐derived NiCo2.5S4 microrods wrapped in reduced graphene oxide (NCS@RGO) were synthesized for potassium‐ion storage. Upon coordination with organic potassium salts, NCS@RGO exhibits an ultrahigh initial reversible specific capacity (602 mAh g?1 at 50 mA g?1) and ultralong cycle life (a reversible specific capacity of 495 mAh g?1 at 200 mA g?1 after 1 900 cycles over 314 days). Furthermore, the battery demonstrates a high initial Coulombic efficiency of 78 %, outperforming most sulfides reported previously. Advanced ex situ characterization techniques, including atomic force microscopy, were used for evaluation and the results indicate that the organic potassium salt‐containing electrolyte helps to form thin and robust solid electrolyte interphase layers, which reduce the formation of byproducts during the potassiation–depotassiation process and enhance the mechanical stability of electrodes. The excellent conductivity of the RGO in the composites, and the robust interface between the electrodes and electrolytes, imbue the electrode with useful properties; including, ultrafast potassium‐ion storage with a reversible specific capacity of 402 mAh g?1 even at 2 A g?1.  相似文献   

7.
An imidazolium‐modified hexa‐peri‐hexabenzocoronene derivative (HBC‐C11‐MIM[Cl?]) was designed and synthesized as a stabilizer to fabricate reduced graphene oxide (RGO). The resulting RGO/HBC‐C11‐MIM[Cl?] hybrid shows excellent dispersivity (5.0 mg mL?1) and stability in water. RGO/HBC‐C11‐MIM[Cl?] was comprehensively characterized by using atomic force microscopy, X‐ray diffraction, X‐ray photoelectron spectroscopy, thermogravimetric analysis, and Raman spectroscopy, thus revealing that one HBC‐C11‐MIM[Cl?] group can stabilize about 178 carbon atoms on the graphene sheets. The obtained hybrid film exhibits a high conductivity of 286 S m?1. Furthermore, the HBC‐C11‐MIM[Cl?]‐modified RGO sheets can be readily dispersed in polar organic solvents upon exchange of the hydrophilic Cl? ions for hydrophobic bis(trifluoromethylsulfonyl) amide (NTf2?) ions.  相似文献   

8.
Three‐dimensional, vertically aligned MnO/nitrogen‐doped graphene (3D MnO/N‐Gr) walls were prepared through facile solution‐phase synthesis followed by thermal treatment. Polyvinylpyrrolidone (PVP) was strategically added to generate cross‐links to simultaneously form 3D wall structures and to incorporate nitrogen atoms into the graphene network. The unique wall features of the as‐prepared 3D MnO/N‐Gr hybirdes provide a large surface area (91.516 m2 g?1) and allow for rapid diffusion of the ion electrolyte, resulting in a high specific capacitance of 378 F g?1 at 0.25 A g?1 and an excellent charge/discharge stability (93.7 % capacity retention after 8000 cycles) in aqueous 1 m Na2SO4 solution as electrolyte. Moreover, the symmetric supercapacitors that were rationally designed by using 3D MnO/N‐Gr hybrids exhibit outstanding electrochemical performance in an organic electrolyte with an energy density of 90.6 Wh kg?1 and a power density of 437.5 W kg?1.  相似文献   

9.
Graphene is a 2D sp2‐hybridized carbon sheet and an ideal material for the adsorption‐based separation of organic pollutants. However, such potential applications of graphene are largely limited, owing to their poor solubility and extensive aggregation properties through graphene? graphene interactions. Herein, we report the synthesis of graphene‐based composites with γ‐Fe2O3 nanoparticle for the high‐performance removal of endocrine‐disrupting compounds (EDC) from water. The γ‐Fe2O3 nanoparticles partially inhibit these graphene? graphene interactions and offer water dispersibility of the composite without compromising much of the high surface area of graphene. In their dispersed form, the graphene component offers the efficient adsorption of EDC, whilst the magnetic iron‐oxide component offers easier magnetic separation of adsorbed EDC.  相似文献   

10.
Ferric nitrate–graphene (FG) nanocomposites synthesized via the equivalent‐volume impregnation method were used for the removal of As(V) species from simulated arsenic‐containing wastewater. Effects of various factors were assessed, such as the reaction temperature, solution pH, adsorbent dosage, and reaction time. The results indicated that the As(V) removal efficiency was as high as 99%, and the concentration of arsenic‐containing wastewater after FG treatment was as low as 9.4 μg L–1 as a result of the optimal absorption capacity and maximum specific surface area (171.766 m2/g) of this material. The equilibrium adsorption capacity of FG for As(V) was achieved in approximately 20 min, and the maximum adsorption capacity was calculated to be 112.4 mg g–1 by Langmuir adsorption isotherm, which was higher than that of other adsorbents such as manganese‐incorporated iron(III) oxide–graphene (14.42 mg g–1). Moreover, the removal efficiency of As(V) can be maintained above 95% under acidic and alkaline conditions. Brunauer–Emmett–Teller analysis showed that the modified FG pore structure was regular. Based on the characterizations by X‐ray diffraction, X‐ray photoelectron spectroscopy, and Fourier transform infrared, the products on the surface of the used FG were Fe(OH)3, FeAsO4, and other compounds, and As(V) was mainly removed by the formation of insoluble compounds and coprecipitation.  相似文献   

11.
Metal oxides have a large storage capacity when employed as anode materials for lithium‐ion batteries (LIBs). However, they often suffer from poor capacity retention due to their low electrical conductivity and huge volume variation during the charge–discharge process. To overcome these limitations, fabrication of metal oxides/carbon hybrids with hollow structures can be expected to further improve their electrochemical properties. Herein, ZnO‐Co3O4 nanocomposites embedded in N‐doped carbon (ZnO‐Co3O4@N‐C) nanocages with hollow dodecahedral shapes have been prepared successfully by the simple carbonizing and oxidizing of metal–organic frameworks (MOFs). Benefiting from the advantages of the structural features, i.e. the conductive N‐doped carbon coating, the porous structure of the nanocages and the synergistic effects of different components, the as‐prepared ZnO‐Co3O4@N‐C not only avoids particle aggregation and nanostructure cracking but also facilitates the transport of ions and electrons. As a result, the resultant ZnO‐Co3O4@N‐C shows a discharge capacity of 2373 mAh g?1 at the first cycle and exhibits a retention capacity of 1305 mAh g?1 even after 300 cycles at 0.1 A g?1. In addition, a reversible capacity of 948 mAh g?1 is obtained at a current density of 2 A g?1, which delivers an excellent high‐rate cycle ability.  相似文献   

12.
A new, ultralight, superhigh surface area, multifunctional aerogel, which is macroassembled from sandwich‐like, hierarchical, porous carbon/graphene nanosheets, is described. The multifunctional aerogel was characterized by means of XRD, SEM, TEM, Raman spectroscopy, and UV/Vis absorption spectroscopy. The multifunctional aerogel had an ultralow density of 8 mg cm?3 and a superhigh surface area of 2650 m2 g?1. The multifunctional aerogel was thermal stability and compressible. Meanwhile, the multifunctional aerogel exhibited high capacity for the adsorption of oils and organic solvents, unexpectedly high hydrogen adsorption and good electrochemical performance.  相似文献   

13.
Mesoporous silica synthesized from the cocondensation of tetraethoxysilane and silylated carbon dots containing an amide group has been adopted as the carrier for the in situ growth of TiO2 through an impregnation–hydrothermal crystallization process. Benefitting from initial complexation between the titania precursor and carbon dot, highly dispersed anatase TiO2 nanoparticles can be formed inside the mesoporous channel. The hybrid material possesses an ordered hexagonal mesostructure with p6mm symmetry, a high specific surface area (446.27 m2 g?1), large pore volume (0.57 cm3 g?1), uniform pore size (5.11 nm), and a wide absorption band between λ=300 and 550 nm. TiO2 nanocrystals are anchored to the carbon dot through Ti?O?N and Ti?O?C bonds, as revealed by X‐ray photoelectron spectroscopy. Moreover, the nitrogen doping of TiO2 is also verified by the formation of the Ti?N bond. This composite shows excellent adsorption capabilities for 2,4‐dichlorophenol and acid orange 7, with an electron‐deficient aromatic ring, through electron donor–acceptor interactions between the carbon dot and organic compounds instead of the hydrophobic effect, as analyzed by the contact angle analysis. The composite can be photocatalytically recycled through visible‐light irradiation after adsorption. The narrowed band gap, as a result of nitrogen doping, and the photosensitization effect of carbon dots are revealed to be coresponsible for the visible‐light activity of TiO2. The adsorption capacity does not suffer any clear losses after being recycled three times.  相似文献   

14.
A new preconcentration method is presented for lead on TAN‐loaded polyurethane foam (PUF) and its measurement by differential pulse anodic stripping voltammetry (DPASV). The optimum sorption conditions of 1.29 × 10?5 M solution of Pb(II) ions on TAN‐loaded PUF were investigated. The maximum sorption was observed at pH 7 with 20 minutes equilibrated time on 7.25 mg mL?1 of TAN‐loaded foam. The kinetic study indicates that the overall sorption process was controlled by the intra‐particle diffusion process. The validity of Freundlich, Langmuir and Dubinin ‐ Radushkevich adsorption isotherms were tested. The Freundlich constants 1/n and KF are evaluated to be 0.45 ±0.04 and (1.03 +0.61) × 10?3 mol g?1, respectively. The monolayer sorption capacity and adsorption constant related to the Langmuir isotherm are (1.38 ± 0.08) × 10?5 mol g?1 and (1.46 ± 0.27) × 105 L mol?1, respectively. The mean free energy of Pb(II) ions sorption on‐TAN loaded PUF is 11.04 ± 0.28 kJ mol?1 indicating chemisorption phenomena. The effect of temperature on the sorption yields thermodynamics parameters of ΔH, ΔS and ΔG at 298 K that are 15.0 ± 1.4 kJ mol?1, 74 ±5 J mol?1 K?1 and ‐7.37 ± 0.28 kJ mol?1, respectively. The positive values of enthalpy (ΔH) and entropy (ΔS) indicate the endothermic sorption and stability of the sorbed complexes are entropy driven. However, the negative value of Gibb's free energy (ΔG) indicates the spontaneous nature of sorption. On the basis of these data, the sorption mechanism has been postulated. The effect of different foreign ions on the sorption and desorption studies were also carried out. The method was successfully applied for the determination of lead from different water samples at ng levels.  相似文献   

15.
Zn2GeO4/N‐doped graphene nanocomposites have been synthesized through a fast microwave‐assisted route on a large scale. The resulting nanohybrids are comprised of Zn2GeO4 nanorods that are well‐embedded in N‐doped graphene sheets by in situ reducing and doping. Importantly, the N‐doped graphene sheets serve as elastic networks to disperse and electrically wire together the Zn2GeO4 nanorods, thereby effectively relieving the volume‐expansion/contraction and aggregation of the nanoparticles during charge and discharge processes. We demonstrate that an electrode that is made of the as‐formed Zn2GeO4/N‐doped graphene nanocomposite exhibits high capacity (1463 mAh g?1 at a current density of 100 mA g?1), good cyclability, and excellent rate capability (531 mAh g?1 at a current density of 3200 mA g?1). Its superior lithium‐storage performance could be related to a synergistic effect of the unique nanostructured hybrid, in which the Zn2GeO4 nanorods are well‐stabilized by the high electronic conduction and flexibility of N‐doped graphene sheets. This work offers an effective strategy for the fabrication of functionalized ternary‐oxide‐based composites as high‐performance electrode materials that involve structural conversion and transformation.  相似文献   

16.
Ion diffusion efficiency at the solid–liquid interface is an important factor for energy storage and adsorption from aqueous solution. Although K2Mn4O8 (KMO) exhibits efficient ion diffusion and ion‐exchange capacities, due to its high interlayer space of 0.70 nm, how to enhance its mass transfer performance is still an issue. Herein, novel layered KMO/reduced graphene oxide (RGO) nanocomposites are fabricated through the anchoring of KMO nanoplates on RGO with a mild solution process. The face‐to‐face structure facilitates fast transfer of lithium and lead ions; thus leading to excellent lithium storage and lead ion adsorption. The anchoring of KMO on RGO not only increases electrical conductivity of the layered nanocomposites, but also effectively prevents aggregation of KMO nanoplates. The KMO/RGO nanocomposite with an optimal RGO content exhibits a first cycle charge capacity of 739 mA h g?1, which is much higher than that of KMO (326 mA h g?1). After 100 charge–discharge cycles, it still retains a charge capacity of 664 mA h g?1. For the adsorption of lead ions, the KMO/RGO nanocomposite exhibits a capacity of 341 mg g?1, which is higher than those of KMO (305 mg g?1) and RGO (63 mg g?1) alone.  相似文献   

17.
A nanostructured organic–inorganic framework, hexagonal NH2‐MIL‐88B, has been prepared through a facile one‐pot reflux reaction and then it was characterized using various techniques. The as‐prepared sample with high specific surface area (414 m2 g?1) showed excellent adsorption for 2,4,6‐trinitrophenol (TNP) in the liquid phase. Detailed studies of the adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were conducted. The adsorption mechanism of NH2‐MIL‐88B for TNP may be ascribed to hydrogen bond interaction, and the complexation between ─OH in TNP and unsaturated Fe(III) on the surface of NH2‐MIL‐88B. The maximum adsorption capacity of NH2‐MIL‐88B for TNP based on the Langmuir isotherm was 163.66 mg g?1. The as‐prepared NH2‐MIL‐88B adsorbent seems to be a promising material in practice for TNP removal from aqueous solution.  相似文献   

18.
The aim of this study was to evaluate the surface adsorption capacity of CrFeO3 nanoparticle‐loaded activated carbon (CrFeO3‐NPs–AC) for the removal of a cationic dye (methyl violet, MV). CrFeO3‐NPs were hydrothermally synthesized and loaded on AC followed by characterization using X‐ray diffraction, field‐emission scanning electron microscopy and energy‐dispersive and Fourier transform infrared spectroscopies. The CrFeO3‐NPs were tested for in vitro antibacterial activities against Gram‐positive (Staphylococcus aureus) and Gram‐negative (Pseudomonas aeruginosa) bacteria. Minimum inhibitory and minimum bactericidal concentrations of CrFeO3‐NPs–AC were obtained to be 50 and 100 μg ml?1, respectively, against S. aureus and 25 and 50 μg ml?1 against P. aeruginosa. These results indicated the antibacterial properties of CrFeO3‐NPs–AC. To investigate the adsorption process, several systematic experiments were designed by varying parameters such as adsorbent mass, pH, initial MV concentration and sonication time. The adsorption process was modelled and the optimal conditions were determined to be 0.013 g, 7.4, 15 mg l?1 and 8 min for adsorbent mass, pH, MV concentration and sonication time, respectively. The real experimental data were found to be efficiently explained by response surface methodology and genetic algorithm model. Kinetic studies for MV adsorption showed rapid sorption dynamics described by a second‐order kinetic model, suggesting a chemisorption mechanism. Then, the experimental equilibrium data obtained at various concentrations of MV and adsorbent masses were fitted to conventional Langmuir, Freundlich, Temkin and Dubinin–Radushkevich isotherm models. Dye adsorption equilibrium data were fitted well to the Langmuir isotherm. From the Langmuir model, the maximum monolayer capacity was calculated to be 65.67 mg g?1 at optimum adsorbent mass.  相似文献   

19.
We designed, synthesized, and characterized a new Zr‐based metal–organic framework material, NU‐1100 , with a pore volume of 1.53 ccg?1 and Brunauer–Emmett–Teller (BET) surface area of 4020 m2g?1; to our knowledge, currently the highest published for Zr‐based MOFs. CH4/CO2/H2 adsorption isotherms were obtained over a broad range of pressures and temperatures and are in excellent agreement with the computational predictions. The total hydrogen adsorption at 65 bar and 77 K is 0.092 g g?1, which corresponds to 43 g L?1. The volumetric and gravimetric methane‐storage capacities at 65 bar and 298 K are approximately 180 vSTP/v and 0.27 g g?1, respectively.  相似文献   

20.
Tin oxide nanoparticles (SnO2 NPs) have been encapsulated in situ in a three‐dimensional ordered space structure. Within this composite, ordered mesoporous carbon (OMC) acts as a carbon framework showing a desirable ordered mesoporous structure with an average pore size (≈6 nm) and a high surface area (470.3 m2 g?1), and the SnO2 NPs (≈10 nm) are highly loaded (up to 80 wt %) and homogeneously distributed within the OMC matrix. As an anode material for lithium‐ion batteries, a SnO2@OMC composite material can deliver an initial charge capacity of 943 mAh g?1 and retain 68.9 % of the initial capacity after 50 cycles at a current density of 50 mA g?1, even exhibit a capacity of 503 mA h g?1 after 100 cycles at 160 mA g?1. In situ encapsulation of the SnO2 NPs within an OMC framework contributes to a higher capacity and a better cycling stability and rate capability in comparison with bare OMC and OMC ex situ loaded with SnO2 particles (SnO2/OMC). The significantly improved electrochemical performance of the SnO2@OMC composite can be attributed to the multifunctional OMC matrix, which can facilitate electrolyte infiltration, accelerate charge transfer, and lithium‐ion diffusion, and act as a favorable buffer to release reaction strains for lithiation/delithiation of the SnO2 NPs.  相似文献   

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