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1.
ACS Appl Mater Interfaces ; 16(21): 27714-27727, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38717953

RESUMO

Rapid and accurate quantification of metabolites in different bodily fluids is crucial for a precise health evaluation. However, conventional metabolite sensing methods, confined to centralized laboratory settings, suffer from time-consuming processes, complex procedures, and costly instrumentation. Introducing the MXene/nitrogen-doped electrochemically exfoliated graphene (MXene@N-EEG) nanocomposite as a novel biosensing platform in this work addresses the challenges associated with conventional methods, leveraging the concept of molecularly imprinted polymers (MIP) enables the highly sensitive, specific, and reliable detection of metabolites. To validate our biosensing technology, we utilize agmatine as a significant biologically active metabolite. The MIP biosensor incorporates electrodeposited Prussian blue nanoparticles as a redox probe, facilitating the direct electrical signaling of agmatine binding in the polymeric matrix. The MXene@N-EEG nanocomposite, with excellent metal conductivity and a large electroactive specific surface area, effectively stabilizes the electrodeposited Prussian blue nanoparticles. Furthermore, increasing the content of agmatine-imprinted cavities on the electrode enhances the sensitivity of the MIP biosensor. Evaluation of the designed MIP biosensor in buffer solution and plasma samples reveals a wide linear concentration range of 1.0 nM-100.0 µM (R2 = 0.9934) and a detection limit of 0.1 nM. Notably, the developed microfluidic biosensor offers low cost, rapid response time to the target molecule (10 min of sample incubation), good recovery results for detecting agmatine in plasma samples, and acceptable autonomous performance for on-chip detection. Moreover, its high reliability and sensitivity position this MIP-based biosensor as a promising candidate for miniaturized microfluidic devices with the potential for scalable production for point-of-care applications.


Assuntos
Técnicas Biossensoriais , Técnicas Eletroquímicas , Grafite , Polímeros Molecularmente Impressos , Nanocompostos , Nitrogênio , Grafite/química , Técnicas Biossensoriais/métodos , Nanocompostos/química , Nitrogênio/química , Polímeros Molecularmente Impressos/química , Técnicas Eletroquímicas/métodos , Humanos , Limite de Detecção , Impressão Molecular , Polímeros/química
2.
Langmuir ; 2024 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-38316141

RESUMO

Electrochemical regeneration of adsorbents presents a cost-effective and environmentally friendly approach. Yet, its application to 3D structured adsorbents such as cellulose/graphene-based aerogels remains largely unexplored. This study introduces a method for producing these aerogels, highlighting their significant adsorption capacity for dissolved organic pollutants and resilience during electrochemical regeneration. By adjusting the ratio of hydrophobized cellulose nanofibers to graphene, the aerogels demonstrate a tunable adsorption capacity, ranging from 56 to 228 mg/g. Hydrophobization using oleic acid is vital for maintaining the aerogels' structural stability in water. Notably, the aerogels maintain structural integrity and efficiency over at least 18 electrochemical regeneration cycles, underscoring their potential for long-term environmental applications. The increase in adsorption capacity observed after regeneration cycles, approximately 10-20% by the fifth cycle, is attributed to electrochemical surface roughening and the creation of new adsorption sites. The tunability and durability of these aerogels offer a sustainable solution for adsorption with electrochemical regeneration technology.

3.
ACS Appl Mater Interfaces ; 15(29): 34711-34725, 2023 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-37433014

RESUMO

Aqueous redox flow battery systems that use a zinc negative electrode have a relatively high energy density. However, high current densities can lead to zinc dendrite growth and electrode polarization, which limit the battery's high power density and cyclability. In this study, a perforated copper foil with a high electrical conductivity was used on the negative side, combined with an electrocatalyst on the positive electrode in a zinc iodide flow battery. A significant improvement in the energy efficiency (ca. 10% vs using graphite felt on both sides) and cycling stability at a high current density of 40 mA cm-2 was observed. A long cycling stability with a high areal capacity of 222 mA h cm-2 is obtained in this study, which is the highest reported areal capacity for zinc-iodide aqueous flow batteries operating at high current density, in comparison to previous studies. Additionally, the use of a perforated copper foil anode in combination with a novel flow mode was discovered to achieve consistent cycling at exceedingly high current densities of >100 mA cm-2. In situ and ex situ characterization techniques, including in situ atomic force microscopy coupled with in situ optical microscopy and X-ray diffraction, are applied to clarify the relationship between zinc deposition morphology on the perforated copper foil and battery performance in two different flow field conditions. With a portion of the flow going through the perforations, a significantly more uniform and compact zinc deposition was observed compared to the case where all of the flow passed over the surface of the electrode. Results from modeling and simulation support the conclusion that the flow of a fraction of electrolyte through the electrode enhances mass transport, enabling a more compact deposit.

4.
Environ Sci Technol ; 57(26): 9865-9873, 2023 07 04.
Artigo em Inglês | MEDLINE | ID: mdl-37343244

RESUMO

Operando visualization of interfacial pH is crucial, yet challenging in electrochemical processes. Herein, we report the fabrication and utilization of ratiometric, fluorescent pH-sensitive nanosensors for operando quantification of fast-dynamic, interfacial pH changes in electrochemical processes and environments where unprotected fluorescent dyes would be degraded. Spatio-temporal pH changes were detected using an electrochemically coupled laser scanning confocal microscope (EC-LSCM) during the electrocoagulation treatment of model and field samples of oil-sands-produced water. Operando visualization of interfacial pH provided new insights into the electrode processes, including ion speciation, electrode fouling, and Faradaic efficiency. We provide compelling evidence that formed metal complexes precipitate at the edge of the pH boundary layer and that there is a strong coupling between the thickness of the interfacial pH layer and the electrode fouling. Furthermore, these findings provide a powerful pathway for optimizing the operating conditions, minimizing electrode passivation, and enhancing the efficiency of electrochemical processes, e.g., electrocoagulation, flow batteries, capacitive deionization, and electrolyzes.


Assuntos
Corantes , Complexos de Coordenação , Fontes de Energia Elétrica , Eletrodos , Concentração de Íons de Hidrogênio
5.
Water Res ; 242: 120201, 2023 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-37336184

RESUMO

Anode fouling is one of the key limiting factors to the widespread application of electrocoagulation (EC) for treatment of different types of contaminated water. Promising mitigation strategy to fouling is to operate the process under polarity reversal (PR) instead of direct current (DC). However, the PR operation comes at the cost of process complexity due to the alternation of electrochemical and chemical reactions. In this study, we systematically investigated the link between evolving fouling layer during DC and PR close to iron and aluminum electrodes and morphological and rheological properties of the formed sludge. By operando visualization of EC process, we demonstrate that during PR operation, precipitation of the iron and aluminum species occurs close to the anode interface, resulting in flocs with higher porosity and lower density than those formed under DC conditions. However, rheological investigation revealed that the PR conditions resulted in a sludge with more pronounced solid-like signature, but this enhancement in its viscoelastic properties is closely related to a period of the current's polarity reversal. We attribute this unexpected result to higher shear rate and collision of particles during PR conditions.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Esgotos , Alumínio/química , Eletrocoagulação , Eletricidade , Eletrodos , Ferro
6.
Chemosphere ; 303(Pt 3): 135207, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35667507

RESUMO

Electrocoagulation (EC) in water treatment encounters several challenges, such as electrode fouling and passivation, especially when the effluent has a complex composition, such as produced water in the oil and gas industry. In this study, the effectiveness of applying an external magnetic field during EC with aluminum anodes (Al-EC) or mild steel anodes (Fe-EC) was investigated for the first time for the removal of inorganic contaminants (including silica, calcium, magnesium, and sulfide) from synthetic and field samples of produced waters. For Al-EC, the presence of a magnetic field perpendicular to the electric field was found to enhance the treatment performance and mitigate the fouling formation on the electrode surface. Chronoamperometric investigations indicated that the application of MF in Al-EC enhances the current density and reduces the time to form a fouling layer on the electrode. In contrast, with Fe-EC, the presence of the magnetic field increased the rate of fouling on the electrodes. Potentiodynamic and kinetic investigations indicate that the magnetic field improves mass transfer via Kelvin force and magnetohydrodynamic (MHD) effects with no impact on the type of kinetic model, while the change in the spin states of the accumulated species has a negligible impact on reducing the fouling. The resistivity of the accumulated fouling layer (δRF) was found to reduce by around 23% due to a magnetic field of 0.158 T. Although increasing the strength of the applied MF increases the mass transfer, the effect is not linear. The results indicate that applying a magnetic field in Al-EC can be an effective method to mitigate fouling during water treatment.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Eletrocoagulação/métodos , Eletrodos , Campos Magnéticos , Eliminação de Resíduos Líquidos/métodos , Poluentes Químicos da Água/análise , Purificação da Água/métodos
7.
Water Sci Technol ; 85(3): 925-942, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-35166711

RESUMO

One of the main challenges for the implementation of electrocoagulation (EC) in water treatment are fouling and passivation of the electrodes, especially for applications with high contaminant concentrations. For the first time, we investigated in this study the process of fouling mitigation by polarity reversal during the EC treatment of boiler blowdown water from oil-sands produced water, characterized by high silica concentrations (0.5-4 g L-1). This effluent is typically obtained from an evaporative desalination process in oil production industries. Potentiodynamic characterisation was used to study the impact of passivation on the anode dissolution. Although a charge loading of 4,800 C L-1 was found to remove about 98% of silica from a 1 L batch of 4 g L-1 Si solution, fouling reduced the performance significantly to about 40% in consecutive cycles of direct current EC (DC-EC) treatment. Periodic polarity reversal (PR) was found to reduce the amount of electrode fouling. Decreasing the polarity period from 60 to 10 s led to the formation of a soft powdery fouling layer that was easily removed from the electrodes. In contrast, with DC operation, a hard scale deposit was observed. The presence of organics in the field samples did not significantly affect the Si removal, and organics with high levels of oxygen and sulfate groups were preferentially removed. Detailed electrochemical and economic investigations suggest that the process operating at 85 °C achieves 95% silica removal (from an initial concentration of 481 mg L-1) with an electrical energy requirement of 0.52 kWh m-3, based on a charge loading of 1,200 C L-1, an inter-electrode gap of 1.8 cm and a current density of 16 mA cm-2.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Alumínio , Eletrocoagulação , Eletrodos , Dióxido de Silício
8.
Water Res ; 203: 117497, 2021 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-34371234

RESUMO

Electrocoagulation (EC) is a promising electrochemical water treatment technology. However, a major challenge to sustaining effective long-term EC operation is controlling the precipitation of materials on the electrodes, commonly referred to as fouling. Periodically reversing electrode polarity has been suggested as an in-situ fouling mitigation strategy and is often implemented in EC field applications. However, the utility of this approach has not been investigated in detail. In this study, the effect of polarity reversal (PR) on the performance of EC using iron electrodes was examined under different water chemistry conditions and at a range of reversal frequencies. It was observed that the faradaic efficiency in PR-EC was always lower than that in the EC systems operated with a direct current (i.e., DC-EC). It was also observed that the faradaic efficiency progressively decreased as the current reversal frequency increased, with the faradaic efficiency dropping as low as 10% when the PR interval was 0.5 min. Results from fouling layer, chronopotentiometric, and cyclic voltammetric investigations indicated that the decrease in the faradaic efficiency was caused by (i) increased electrode fouling by iron precipitates and (ii) electrochemical side reactions at the electrode-electrolyte interface. The extent of these effects was dependent on the solution chemistry; oxyanions and sulfide were found to be particularly detrimental to the performance of PR-EC, causing severe electrode fouling while decreasing the faradaic efficiency. Fouling could be mitigated by increasing the solution convection rate, resulting in a shear on the electrode surface that removed iron and other electrochemically reactive species from the electrodes.


Assuntos
Ferro , Purificação da Água , Eletricidade , Eletrocoagulação , Eletrodos
9.
ACS Appl Mater Interfaces ; 13(35): 41563-41572, 2021 Sep 08.
Artigo em Inglês | MEDLINE | ID: mdl-34428017

RESUMO

Among the aqueous redox flow battery systems, redox chemistries using a zinc negative electrode have a relatively high energy density, but the potential of achieving high power density and long cycle life is hindered by dendrite growth at the anode. In this study, a new cell design with a narrow gap between electrode and membrane was applied in a zinc-iodide flow battery. In this design, some of the electrolyte flows over the electrode surface and a fraction of the flow passes through the porous felt electrode in the direction of current flow. The flow battery was tested under constant current density over 40 cycles, and the efficiency, discharge energy density, and power density of the battery were significantly improved compared to conventional flow field designs. The power density obtained in this study is one of the highest power densities reported for the zinc-iodide battery. The morphology of the zinc deposition was studied using scanning electron microscopy and optical profilometry. It was found that the flow through the electrode led to a thinner zinc deposit with lower roughness on the surface of the electrode, in comparison to the case where there was no flow through the electrode. In addition, inhibition of dendrite formation enabled operation at a higher range of current density. Ex situ tomographic measurements were used to image the zinc deposited on the surface and inside the porous felt. Volume rendering of graphite felt from X-ray computed tomography images showed that in the presence of flow through the electrode, more zinc deposition occurred inside the porous felt, resulting in a compact and thinner surface deposit, which may enable higher battery capacity and improved performance.

10.
ChemSusChem ; 14(9): 2100-2111, 2021 May 06.
Artigo em Inglês | MEDLINE | ID: mdl-33739619

RESUMO

The charge-discharge operation of the vanadium redox flow battery degrades the electrodes over time and results in a performance and efficiency decay. The impact of extended charge-discharge cycling operation on carbon electrodes is investigated using carbon paper as a model electrode. Electrode degradation along with 70 % degradation of charge-discharge capacity was observed after 100 charge-discharge cycles of a single cell vanadium redox flow battery operating at a current density of 80 mA cm-2 at room temperature (23 °C). Raman mapping of the electrodes shows a decrease in structural defects in the negative electrode, and an increase in defects in the positive electrode, indicating differences in the degradation mechanism at each electrode. Electrochemical investigation reveals an increase in the activation overpotential at both the positive and negative electrodes. However, the negative electrode showed a higher activation overpotential indicating a higher impact of electrode degradation on the negative side. X-ray photoelectron spectroscopy shows around an eightfold increase in surface oxygen functional groups after degradation in both positive and negative electrodes. The composition of oxygen functional groups was also observed to change significantly after degradation from dominantly carbonyl-based to a combination of carbonyl- and carboxyl-based groups. This study provides insight into the electrode degradation mechanism and highlights the differences in the mechanism for the positive and negative electrodes.

11.
Water Res ; 187: 116433, 2020 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-33002774

RESUMO

Treating water and wastewater is energy-intensive, and traditional methods that require large amounts of chemicals are often still used. Electrocoagulation (EC), an electrochemical treatment technology, has been proposed as a more economically and environmentally sustainable alternative. In EC, sacrificial metal electrodes are used to produce coagulant in-situ, which offers many benefits over conventional chemical coagulation. However, material precipitation on the electrodes during long term operation induces a passivating effect that decreases treatment performance and increases power requirements. Overcoming this problem is considered to be the greatest challenge facing the development of EC. In this critical review, the studies that have examined the nature of electrode passivation, and its effect on treatment performance are considered. A fundamental approach is used to examine the association between passivation and faradaic efficiency, a surrogate for EC performance. In addition, the strategies that have been proposed to remove or avoid passivation are reviewed, including aggressive ion addition, AC current operation, polarity reversal, ultrasonication, and mechanical cleaning of the electrodes. It is concluded that the success of implementing each method is dependent on critical operating parameters, and careful consideration should be taken when designing an EC system based on the phenomena discussed in this article. In conclusion, this review provides insight into passivation mechanisms, delivers guidelines for sustaining high treatment performance, and offers an outlook for the future development of EC.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Eletrocoagulação , Eletrodos , Eliminação de Resíduos Líquidos , Águas Residuárias
12.
Molecules ; 25(15)2020 Jul 26.
Artigo em Inglês | MEDLINE | ID: mdl-32722653

RESUMO

Catalyst layer (CL) ionomers control several transport and interfacial phenomena including long-range transport of protons, local transport of oxygen to Pt catalyst, effective utilization of Pt catalyst, electrochemical reaction kinetics and double-layer capacitance. In this work, the variation of these properties, as a function of humidity, for CLs made with two ionomers differing in side-chain length and equivalent weight, Nafion-1100 and Aquivion-825, was investigated. This is the first study to examine humidity-dependent oxygen reduction reaction (ORR) kinetics in-situ for CLs with different ionomers. A significant finding is the observation of higher ORR kinetic activity (A/cm2Pt) for the Aquivion-825 CL than for the Nafion-1100 CL. This is attributed to differences in the interfacial protonic concentrations at Pt/ionomer interface in the two CLs. The differences in Pt/ionomer interface is also noted in a higher local oxygen transport resistance for Aquivion-825 CLs compared to Nafion-1100 CLs, consistent with stronger interaction between ionomer and Pt for ionomer with more acid groups. Similar dependency on Pt utilization (ratio of electrochemically active area at any relative humidity (RH) to that at 100% RH) as a function of RH is observed for the two CLs. As expected, strong influence of humidity on proton conduction is observed. Amongst the two, the CL with high equivalent weight ionomer (Nafion-1100) exhibits higher conduction.


Assuntos
Técnicas Eletroquímicas , Polímeros de Fluorcarboneto/química , Íons/química , Platina/química , Catálise , Fontes de Energia Elétrica , Membranas Artificiais , Oxigênio/química , Prótons
13.
RSC Adv ; 10(50): 29975-29982, 2020 Aug 10.
Artigo em Inglês | MEDLINE | ID: mdl-35518211

RESUMO

A rapid microwave hydrothermal process is adopted for the synthesis of titanium dioxide and reduced graphene oxide nanocomposites as high-performance anode materials for Li-ion batteries. With the assistance of hydrazine hydrate as a reducing agent, graphene oxide was reduced while TiO2 nanoparticles were grown in situ on the nanosheets to obtain the nanocomposite material. The morphology of the nanocomposite obtained consisted of TiO2 particles with a size of ∼100 nm, uniformly distributed on the reduced graphene oxide nanosheets. The as-prepared TiO2-graphene nanocomposite was able to deliver a capacity of 250 mA h g-1 ± 5% at 0.2C for more than 200 cycles with remarkably stable cycle life during the Li+ insertion/extraction process. In terms of high rate capability performance, the nanocomposite delivered discharge capacity of ca. 100 mA h g-1 with >99% coulombic efficiency at C-rates of up to 20C. The enhanced electrochemical performance of the material in terms of high rate capability and cycling stability indicates that the as-developed TiO2-rGO nanocomposites are promising electrode materials for future Li-ion batteries.

14.
Chemosphere ; 241: 125020, 2020 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-31614314

RESUMO

A nanocomposite of graphene and titanium dioxide (G/TiO2) was prepared using the sol-gel method for use in an electrochemical adsorption/regeneration process. The effect of annealing temperature on electrochemical characteristics of the nanocomposites was investigated by cyclic voltammetry and constant current electrochemical regeneration, using methylene blue (MB) as the adsorbate. The G/TiO2 could be regenerated more rapidly and with less corrosion than the bare graphene. The G/TiO2 annealed at 400 °C had a higher proportion of anatase phase TiO2 (ca. 7% rutile TiO2) compared to that annealed at 500 °C (ca. 40% rutile TiO2). Cyclic voltammetry indicated that the G/TiO2 annealed at 400 °C had a higher activity for MB oxidation than the nanocomposite annealed at 500 °C. Similarly, the regeneration of MB loaded G/TiO2 annealed at 400 °C was much faster than for the nanocomposite annealed at 500 °C. Complete regeneration of the G/TiO2 annealed at 400 °C was obtained after an electrochemical charge of 21 C per mg of adsorbate. The G/TiO2 annealed at 400 °C was regenerated in half the time required for the bare graphene. TEM studies showed that the bare graphene was rapidly corroded, while corrosion was not observed for the G/TiO2 nanocomposites.


Assuntos
Corantes/química , Técnicas Eletroquímicas/métodos , Grafite , Nanocompostos/química , Reciclagem/métodos , Titânio , Adsorção , Corrosão , Eletrodos , Azul de Metileno/química
15.
Angew Chem Int Ed Engl ; 58(47): 16815-16819, 2019 Nov 18.
Artigo em Inglês | MEDLINE | ID: mdl-31538391

RESUMO

In aqueous electrochemical processes, the pH evolves spatially and temporally, and often dictates the process performance. Herein, a new method for the in-operando monitoring of pH distribution in an electrochemical cell is demonstrated. A combination of pH-sensitive fluorescent dyes, encompassing a wide pH range from ≈1.5 to 8.5, and rapid electrochemically coupled laser scanning confocal microscopy is used to observe pH changes in the cell. Using electrocoagulation as an example process, we show that the method provides new insights into the reaction mechanisms. The pH close to the aluminium electrode surface is influenced by the applied current density, hydrolysis of aluminium cations, and gas evolution. Through quantification of the pH at the anode, along with gas analysis, we find that hydrogen is evolved at the anode due to a non-Faradaic chemical reaction. This leads to increased production of coagulant, which may open new routes to enhance the process performance. This method for in-operando dynamic visualization of pH paves the way for studies of electrochemical processes, including other water treatment, electrosynthesis, and batteries.

16.
Chemosphere ; 230: 596-605, 2019 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-31125888

RESUMO

In this study a process of adsorption and electrochemical regeneration was evaluated for its efficiency in removing low concentrations of emulsified oil from produced water, which is generated as a by-product from the thermal in-situ production of heavy oil. Adsorption behavior was investigated using synthetic model emulsions and samples of produced water; theoretical models were applied to the adsorption equilibrium and kinetics. It was demonstrated that the rate of the adsorption process was controlled by external mass transport, with no contribution from intra-particle diffusion. The non-porous structure of the Graphite Intercalation Compound (GIC) adsorbent led to effective and fast adsorption of oil in less than 30 min. Based on the cryo-SEM imaging and EDX phase mapping, the underlying adsorption mechanism was envisioned in the frame of adhesion and spreading of the emulsified oil droplets on the surface of the predominately hydrophobic GIC surface. The adsorptive capacity of the GIC was 100% recoverable by electrochemical regeneration. Energy consumption for the adsorbent regeneration process was found to be 22 kWh per kg of COD removed for treatment of the synthetic emulsion and 36 kWh per kg of COD for produced water.


Assuntos
Técnicas Eletroquímicas/métodos , Grafite/química , Hidrocarbonetos/análise , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Adsorção , Emulsões , Interações Hidrofóbicas e Hidrofílicas , Cinética , Modelos Teóricos , Propriedades de Superfície , Águas Residuárias/química
17.
Chemosphere ; 201: 807-815, 2018 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-29550575

RESUMO

This work compares the ability of physical and chemical treatments, namely adsorption and electrochemical advanced oxidation processes, to remove tyrosol from aqueous medium. Adsorption on graphene nanoplatelets (GNPs) performed much better than that with a graphite intercalation compound. Adsorption isotherms were found to follow the Freundlich model (R2 = 0.96), which is characteristic of a chemisorption process. Successful electrochemical regeneration enables 5 successive adsorption/regeneration cycles before corrosion of GNPs occurs. Other typical aromatic contaminants that may coexist with tyrosol can be also adsorbed on GNPs. Percentage of regeneration efficiency of GNPs showed a higher affinity towards Lewis acids group compounds and a lower one towards Lewis base. The treatment of 100 mL of 0.723 mM tyrosol solutions in non-chlorinated and chlorinated matrices at pH 3.0 was carried out by electrochemical oxidation with electrogenerated H2O2 (EO-H2O2), electro-Fenton (EF) and UVA photoelectro-Fenton (PEF). Trials were made with a BDD anode and an air-diffusion cathode at 10-30 mA cm-2. Hydroxyl radicals formed at the anode from water oxidation and/or in the bulk from Fenton's reaction between added Fe2+ and generated H2O2, along with active chlorine produced in chlorinated medium, were the main oxidants. Tyrosol concentration always decayed following a pseudo-first-order kinetics and its mineralization rose as EO-H2O2 < EF < PEF, more rapidly in the chlorinated matrix. The potent photolysis of intermediates under UVA radiation explained the almost total mineralization achieved by PEF in the latter medium. The effect of current density and tyrosol content on the performance of all processes was examined.


Assuntos
Técnicas Eletroquímicas/métodos , Grafite/química , Álcool Feniletílico/análogos & derivados , Raios Ultravioleta , Poluentes Químicos da Água/análise , Purificação da Água/métodos , Adsorção , Eletrodos , Peróxido de Hidrogênio/química , Oxirredução , Álcool Feniletílico/análise , Álcool Feniletílico/química , Fotólise , Águas Residuárias/química , Poluentes Químicos da Água/química
18.
ACS Appl Mater Interfaces ; 9(16): 14171-14179, 2017 Apr 26.
Artigo em Inglês | MEDLINE | ID: mdl-28374986

RESUMO

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 segregated conductive structure and magnetic properties of the magnetite nanoparticles.

19.
Water Res ; 114: 237-245, 2017 05 01.
Artigo em Inglês | MEDLINE | ID: mdl-28249215

RESUMO

In this work, two different reduced graphene oxide/iron oxide (rGO-IO) nanocomposites with different iron oxide loadings were fabricated using a one-step solvothermal method. The structure, properties and applications of the synthesized nanocomposites were evaluated with Raman spectroscopy, attenuated total reflectance Fourier transform infrared spectroscopy, thermogravimetric analysis, X-ray diffraction, electron microscopy, and energy-dispersive X-ray spectroscopy. The iron oxide is in the form of magnetite (Fe3O4), so that the resultant adsorbent can readily be separated from the treated water using a magnetic field. The ability of the nanocomposites to remove methylene blue (MB) from water by adsorption was investigated. The highest adsorptive capacity observed was 39 mg g-1, for the composite containing 60 wt% iron oxide. The adsorptive capacity of the rGO-IO decreased to 26 mg g-1 when the mass fraction of iron oxide was increased to 75 wt%. Electrochemical regeneration of MB loaded rGO-IO was also investigated. The electrochemical regeneration was found to be rapid and with low electrical energy consumption relative to conventional adsorbents, due to the high electrical conductivity and nonporous surface of the rGO. A regeneration efficiency of 100% was obtained after 30 min of electrochemical treatment using a 2 mm thick bed of rGO-IO loaded with 39 mg g-1 MB, using a current density of 10 mA cm-2. Multiple adsorption-electrochemical regeneration cycles demonstrated that the surface of the rGO was modified leading to increase in the adsorptive capacity to around 80 mg g-1 after the second regeneration cycle. The morphology of the rGO was observed to change significantly after electrochemical regeneration, suggesting that the rGO based adsorbent materials could only be used for a few cycles.


Assuntos
Grafite/química , Azul de Metileno , Óxido Ferroso-Férrico , Óxidos/química , Regeneração
20.
Environ Sci Technol ; 40(19): 6098-103, 2006 Oct 01.
Artigo em Inglês | MEDLINE | ID: mdl-17051806

RESUMO

The application of electrokinetic treatment to phenol contaminated soil combined with the addition of a chemical oxidant (permanganate) to the catholyte has been evaluated. It was found that the counter-current flow of the phenol (by electrosmosis) and permanganate (by electromigration) leads to a rapid oxidation of the phenol in the soil. After 5 days of treatment over 90% of the phenol (initial concentration 1 g kg(-1) dry soil) in a 15 cm long container of kaolin was removed by electrokinetic treatment with a voltage gradient of 1 V cm(-1) and an initial concentration of KMnO4 of 9 g L(-1) in the catholyte. This level of treatment was achieved with an electrical energy consumption of less than 15 kWh per m3 of soil treated.


Assuntos
Oxidantes/química , Fenol/isolamento & purificação , Permanganato de Potássio/química , Poluentes do Solo/isolamento & purificação , Gerenciamento de Resíduos/métodos , Eletroquímica , Caulim , Cinética , Manganês/análise , Oxirredução , Fenol/química , Poluentes do Solo/química
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