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1.
Chemosphere ; 307(Pt 3): 135812, 2022 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-35963386

RESUMO

The presence of antibiotics in wastes and drinking water has led to serious environmental and health concerns, further necessitating the development of an advanced sustainable strategy to eliminate antibiotics from aquatic media. In this context, the present research reports the successful fabrication of a spinning disc photoreactor (SDPR) supported ZnO/Ag/WO3 S-scheme visible-light-driven thin-film photocatalyst to study the degradation of cephalexin (CPX) as a target pollutant under blue light irradiation. The optical, electrochemical and physicochemical characterization of the as-prepared thin-film samples were carried out by XRD, top-view FE-SEM, EDS-mapping, UV-Vis-DRS, contact angle, EIS, transient photocurrent, mott Schottky and AFM techniques. The rod shape morphology of the samples with moderate surface roughness, desirable hydrophobicity, low bandgap and remarkable band structure alignment confirmed the applicability of as-prepared thin-film with an average photon flux of 1.94 × 10-4-8.61 × 10-5 E's m-2 s-1. The use of a rotating catalytic disc impressively declined the photon propagation distance, decremented the probability of light absorption by the solution, and intensified the mass transfer rate. The maximum throughputs of 98.8% efficiencies for CPX degradation were achieved at a rotational speed of 180 rpm, the solution flow rate of 1.0 L min-1, the light intensity of 11 mW cm-2, and initial CPX concentration of 40 mg L-1, illumination time of 80 min, and pH of 6. Damkohler number (Da) value was found to be 1.23 × 10-2 at the optimum conditions, indicating the negligibility of the external mass transfer resistance in the SDPR. The photocatalytic mechanism was elucidated for finding the most operative radical species, suggesting the crucial role of ·O2- in photodegradation of CPX and a drastic improvement of the charge separation by S-scheme heterostructure and facilitation by Ag mediator. Findings indicated that the developed reusable and robust SDPR benefited from an s-scheme photocatalyst can be a promising technology for degradation of the organic compounds.


Assuntos
Água Potável , Poluentes Ambientais , Óxido de Zinco , Antibacterianos/química , Cefalexina , Fotólise , Óxido de Zinco/química
2.
J Hazard Mater ; 416: 126196, 2021 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-34492960

RESUMO

A Schottky junction based on Ti3C2Tx MXene sheet integrated with marigold flower-like V2O5/CuWO4 heterojunction was designed and fabricated for robust ammonia sensing by monitoring the electrical resistance changes in air and ammonia. The electron transport behavior of the sensor was investigated by electrochemical analysis, ultraviolet photoelectron spectroscopy and reflection electron energy loss spectroscopy. Besides, negative zeta potential obtained for sensor components was in consistent with surface functional groups (e.g. OH and F) observed by XPS analysis helping better understanding of the ammonia sensing mechanism. The results desirably confirmed high sensitivity, selectivity, linear range (1-160 ppm), the limit of quantification, repeatability, long-term stability, very short response time (few seconds) and low working temperature (25 °C) of the sensor. The measurements on the resistance changes of the MXene/V2O5/CuWO4-based sensor under the exposure to various types of analytes (Ammonia, Acetone, Benzene, Chloroform, DMF, Ethanol, humidity (80%), Methanol and Toluene as well as NO, NO2, H2S, SO2, CO and CH4) at different concentrations revealed that the fabricated sensor is excellently selective to ammonia with ultra-high sensitivity. Intra-day stability (7 runs a day) and long-term stability (every 10 days over 70 days) as important sensor characteristics were investigated at 51 ppm and ambient temperature, which showed very good repeatability and recoverability in both short and long periods for sensing the ammonia. Overall, MXene/V2O5/CuWO4 was shown to be cost-effective, easy to handle and suitably applicable for simple, ultrafast and extremely efficient trace ammonia detection, which could be of high interest for future exhaled breath analysis and the development of a novel noninvasive diagnostic strategy to monitor chronic kidney disease to stop a large measure of unnecessary invasive testing.


Assuntos
Amônia , Testes Respiratórios , Técnicas Eletroquímicas , Umidade , Temperatura
3.
Chemosphere ; 267: 129206, 2021 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-33321280

RESUMO

In this study, a facile four-step hydrothermal method was utilized to deposit a core-shell structure on UiO-66(Zr/Ti) nanoflake (NFs) as a visible-light-driven photocatalyst. The core was magnetic Fe3O4 which served as a charge carrier coated with WO3 shell. The as-prepared photocatalyst was characterized by XRD, VSM, BET, FTIR, FE-SEM, UV-Vis-DRS, and PL techniques which proved successful deposition of Fe3O4@WO3 core/shell particle on UiO-66(Zr/Ti)-NFs. The obtained photocatalyst was subsequently applied for urea photo-oxidation. This magnetically recoverable photocatalyst exhibited superior activity due to its desirable band alignment, high stability, and generation of the photo-induced charge carriers, as well as providing a high surface area with low mass transfer resistance. Fe3O4 core acted as charge-carrier to transport the photogenerated charges of UiO-66(Zr/Ti)-NFs (electron-donor) to WO3 charge-collectors for effective photoconversion. The central composite design was applied to design the experiments matrix in which flow rate, pH, irradiation time, catalyst mass, and initial urea concentration were considered as operational factors. The optimized condition was found by defining the desirability function. 90% degradation percentage was achieved at 550 mL/min solution flowrate, pH = 7, 120 min irradiation time, 0.22 g UiO-66(Zr)-NFs-Fe3O4@WO3, and 40 mg/L of the initial concentration of urea with the desirability value of 0.89. Such a superior photocatalytic activity of UiO-66-Fe3O4@WO3 can be ascribed to the reclamation of Fe3O4 as a low bandgap carrier, which accelerated the conveyance of electrons and followed surpassing charge separation. Our present findings open a new strategy to produce a wide range of core-shell heterogeneous catalysts to be applied in photoreactors scale-up.


Assuntos
Titânio , Ureia , Catálise , Luz , Oxirredução
4.
J Hazard Mater ; 393: 122360, 2020 07 05.
Artigo em Inglês | MEDLINE | ID: mdl-32114134

RESUMO

This work presents the characterization of novel synthesized UiO-66(Ti)-Fe3O4-WO3 magnetic photocatalyst and investigates their photocatalytic activity for the photodegradation of ammonia in a designed continuous flow-loop thin-film slurry flat-plate photoreactor (TFSR). Excellent ammonia degradation efficiency was achieved in the presence of the synthesized catalyst at ambient conditions using no more reactive oxidant species. Several independent variables involving catalyst mass, flowrate, pH, irradiation time and initial ammonia concentration as well as corresponding experiments were analyzed and design using the central composite design (CCD). The influence and significance of each parameter and their binary interactions were then evaluated by applying the analysis of variance. The ammonia degradation efficiency of 91.80 % with the desirability of 0.903 were obtained at optimum values of operational parameters including 550 mL/min,10, 0.125 g/L, 60 min and 30 mg/L for solution flowrate, pH, catalyst mass, irradiation time and initial ammonia concentration, respectively. Furthermore, the liquid phase products of ammonia degradation such as nitrate and nitrite ions were completely removed, and purified water was produced using the combination of reverse osmosis process and mixed resins beds. The photocatalyst mechanism study revealed that [Formula: see text] was the predominant reactive oxygen species in the ammonia photodegradation.

5.
Sci Rep ; 9(1): 3798, 2019 03 07.
Artigo em Inglês | MEDLINE | ID: mdl-30846771

RESUMO

Natural carbon powder has been used as a precursor to prepare two main types of sensitising agents of nitrogen-doped carbon nanoparticles (N-CNPs) and nitrogen-doped graphene quantum dots coupled to nanosheets (N-GQDs-NSs) by using simple treatments of chemical oxidation and centrifugation separation. Characterization based on FTIR, XPS, XRD, Raman spectroscopy, FE-SEM, HR-TEM, AFM, UV-Vis and FL, revealed successful doping carbon nanoparticle with nitrogen with an average plane dimension of 50 nm and relatively smooth surface. The versatility of the prepared samples as sensitising agents was developed and established by exploiting its ability for detection of volatile organic compounds via simple optical fibre based sensing configuration. The comparative experimental studies on the proposed sensor performance indicate fast response achieved at a few tens of seconds and excellent repeatability in exposure to the methanol vapour. The low limit of detection of 4.3, 4.9 and 10.5 ppm was obtained in exposure to the methanol, ethanol and propanol vapours, respectively, in the atmosphere condition. This study gives insights into the chemical/physical mechanism of an enhanced economic optical fibre based gas sensor and illustrates it for diverse sensing applications, especially for chemical vapour remote detection and future air quality monitoring.

6.
Ultrason Sonochem ; 35(Pt A): 51-60, 2017 Mar.
Artigo em Inglês | MEDLINE | ID: mdl-27765487

RESUMO

Funthenalized chitosan (CS) was composited with mesoprous SBA-15 and characterized via. different techniques such as FT-IR and FE-SEM. Subsequently, this new material was applied for simulations ultrasound-assisted adsorption of Pb2+ ion and alizarin red S (ARS) dye after their complexation. Efficient conventional variables in adsorption process such as initial ARS and Pb2+ concentration, adsorbent mass and sonication time were studied by small central composite design (CCD) and optimized with desirability function approach. Lack of fit testes and model summary statistics for linear, 2FI, quadratic and cubic models were investigated and according to the insignificant lack of fit and maximizing the R-squared (R2), adjusted R-squared and the predicted R-squared quadratic model was selected for other step analysis for removal of ARS dye, while, for Pb2+ ions 2FI model was selected as best model. Quadratic model ANOVA for ARS dye removal shows the F-value parameter (683.91), very low p-value model (<0.0001) and p-value lack of fit (0.0568) that implied this model was highly significant. Also, 2FI model ANOVA for Pb2+ ions removal shows the F-value parameter (282.51), very low p-value model (<0.0001) and p-value lack of fit (2.05). According to desirability function approach maximum removal percentage of ARS (87.61%) and Pb2+ ions (83.54%) was shown at optimum of condition that were set as at: 25 and 25mgL-1, 0.028g and 11.8min for initial ARS and Pb2+ ions concentration, adsorbent mass and sonication time, respectively. Finally, it was found that the equilibrium and kinetic of adsorption process follow the Langmuir isotherm and pseudo-second-order kinetic model, respectively. From the Langmuir isotherm, maximum monolayer capacity (qmax) was obtained 50.25 and 57.14mgg-1 for ARS and Pb2+ ions removal, respectively.

7.
Spectrochim Acta A Mol Biomol Spectrosc ; 167: 157-164, 2016 10 05.
Artigo em Inglês | MEDLINE | ID: mdl-27318150

RESUMO

Maximum malachite green (MG) adsorption onto ZnO Nanorod-loaded activated carbon (ZnO-NR-AC) was achieved following the optimization of conditions, while the mass transfer was accelerated by ultrasonic. The central composite design (CCD) and genetic algorithm (GA) were used to estimate the effect of individual variables and their mutual interactions on the MG adsorption as response and to optimize the adsorption process. The ZnO-NR-AC surface morphology and its properties were identified via FESEM, XRD and FTIR. The adsorption equilibrium isotherm and kinetic models investigation revealed the well fit of the experimental data to Langmuir isotherm and pseudo-second-order kinetic model, respectively. It was shown that a small amount of ZnO-NR-AC (with adsorption capacity of 20mgg(-1)) is sufficient for the rapid removal of high amount of MG dye in short time (3.99min).

8.
Ultrason Sonochem ; 32: 119-131, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27150752

RESUMO

Chromium doped zinc oxide nanoparticles (ZnO: Cr-NPs) was synthesized by ultrasonically assisted hydrothermal method and characterized by FE-SEM, XRD and TEM analysis. Subsequently, this composite ultrasonically assisted was deposited on activated carbon (ZnO: Cr-NPs-AC) and used for simultaneous ultrasound-assisted removal of three toxic organic dye namely of malachite green (MG), eosin yellow (EY) and Auramine O (AO). Dyes spectra overlap in mixture (major problem for simultaneous investigation) of this systems was extensively resolved by derivative spectrophotometric method. The magnitude of variables like initial dyes concentration, adsorbent mass and sonication time influence on dyes removal was optimized using small central composite design (CCD) combined with desirability function (DF) approach, while pH was studied by one-a-time approach. The maximized removal percentages at desirability of 0.9740 was set as follow: pH 6.0, 0.019g ZnO: Cr-NPs-AC, 3.9min sonication at 4.5, 4.8 and 4.7mgL(-1) of MG, EY and AO, respectively. Above optimized points lead to achievement of removal percentage of 98.36%, 97.24%, and 99.26% correspond to MG, EY and AO, respectively. ANOVA for each dyes based p-value less than (<0.0001) suggest highly efficiency of CCD model for prediction of data concern to simultaneous removal of these dyes within 95% confidence interval, while their F-value for MG, EY and AO is 935, 800.2, and 551.3, respectively, that confirm low participation of this them in signal. The value of multiple correlation coefficient R(2), adjusted and predicted R(2) for simultaneous removal of MG is 0.9982, 0.9972 and 0.9940, EY is 0.9979, 0.9967 and 0.9930 and for AO is 0.9970, 0.9952 and 0.9939. The adsorption rate well fitted by pseudo second-order and Langmuir model via high, economic and profitable adsorption capacity of 214.0, 189.7 and 211.6mgg(-1) for MG, EY and AO, respectively.

9.
Ultrason Sonochem ; 32: 387-397, 2016 09.
Artigo em Inglês | MEDLINE | ID: mdl-27150785

RESUMO

An efficient simultaneous sonophotocatalytic degradation of trypan blue (TB) and vesuvine (VS) using Ag3PO4/Bi2S3-HKUST-1-MOF as a novel visible light active photocatalyst was carried out successfully in a continuous flow-loop reactor equipped to blue LED light. Ag3PO4/Bi2S3-HKUST-1-MOF with activation ability under blue light illumination was synthesized and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy dispersive X-ray (EDX), photoluminescence (PL) and diffuse reflectance spectra (DRS). The effect of operational parameters such as the initial TB and VS concentration (5-45mg/L), flow rate (30-110mL/min), irradiation and sonication time (10-30min), pH (3-11) and photocatalyst dosage (0.15-0.35g/L) has been investigated and optimized using central composite design (CCD) combined with desirability function (DF). Maximum sonophotodegradation percentage (98.44% and 99.36% for TB and VS, respectively) was found at optimum condition set as: 25mg/L of each dye, 70mL/min of solution flow rate, 25min of irradiation and sonication time, pH 6 and 0.25g/L of photocatalyst dosage. At optimum conditions, synergistic index value was obtained 2.53 that indicated the hybrid systems including ultrasound irradiation and photocatalysis have higher efficiency compared with sum of the individual processes.

10.
Phys Chem Chem Phys ; 18(16): 11278-87, 2016 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-27053427

RESUMO

A novel nanorose-like metal organic system (MOS) based on Cu(II) and biphenyl-4,4-dicarboxylic acid (Cu-BPDCA) was hydrothermally synthesized and characterized via EDS, FE-SEM, XRD, DRS and FT-IR analysis. This novel nanomaterial was found to be of narrow energy band gap (1.24 eV) and thus it was applied as a photocatalyst driven by visible light for the degradation of the rose bengal (RB) and eosin Y (EY) dyes. For further improvement in the photocatalytic performance of Cu-BPDCA, it was doped with a trace amount of Ce(III) in a simple way followed by characterization. The achieved improvement is due to the formation of a large number of O2⁻˙ and ˙OH radicals compared to the case of undoped Cu-BPDCA. The influence of important variables such as initial dye concentration, photocatalyst dosage and time of irradiation on the photocatalytic degradation efficiency was studied and optimized using central composite design. The optimum condition for the photodegradation of RB was found to be 40 min, 4.0 mg L(-1) and 0.015 g, corresponding to the irradiation time, RB concentration and photocatalyst mass, respectively. The photodegradation of EY was optimized at 4.0, 76 min, 5.9 mg L(-1) and 0.015 g corresponding to the pH, irradiation time, EY concentration and photocatalyst mass, respectively. At these optimum conditions, the photocatalytic degradation percentages of RB and EY with a desirability of 0.95 and 1.0 were found to be 78.90% and 67.63%, respectively. Kinetics study showed that the Langmuir-Hinshelwood kinetics model suitably fits the experimental data. From the Langmuir-Hinshelwood kinetics model, a significantly high photodegradation to surface adsorption ratio was obtained which is the great advantage of this work in addition to applying visible light.

11.
Phys Chem Chem Phys ; 18(19): 13310-21, 2016 05 11.
Artigo em Inglês | MEDLINE | ID: mdl-27119755

RESUMO

The aim of this work is the study of the predictive ability of a hybrid model of support vector regression with genetic algorithm optimization (GA-SVR) for the adsorption of malachite green (MG) onto multi-walled carbon nanotubes (MWCNTs). Various factors were investigated by central composite design and optimum conditions was set as: pH 8, 0.018 g MWCNTs, 8 mg L(-1) dye mixed with 50 mL solution thoroughly for 10 min. The Langmuir, Freundlich, Temkin and D-R isothermal models are applied to fitting the experimental data, and the data was well explained by the Langmuir model with a maximum adsorption capacity of 62.11-80.64 mg g(-1) in a short time at 25 °C. Kinetic studies at various adsorbent dosages and the initial MG concentration show that maximum MG removal was achieved within 10 min of the start of every experiment under most conditions. The adsorption obeys the pseudo-second-order rate equation in addition to the intraparticle diffusion model. The optimal parameters (C of 0.2509, σ(2) of 0.1288 and ε of 0.2018) for the SVR model were obtained based on the GA. For the testing data set, MSE values of 0.0034 and the coefficient of determination (R(2)) values of 0.9195 were achieved.

12.
Ultrason Sonochem ; 31: 383-93, 2016 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-26964963

RESUMO

Activated carbon (AC) composite with HKUST-1 metal organic framework (AC-HKUST-1 MOF) was prepared by ultrasonically assisted hydrothermal method and characterized by FTIR, SEM and XRD analysis and laterally was applied for the simultaneous ultrasound-assisted removal of crystal violet (CV), disulfine blue (DSB) and quinoline yellow (QY) dyes in their ternary solution. In addition, this material, was screened in vitro for their antibacterial actively against Methicillin-resistant Staphylococcus aureus (MRSA) and Pseudomonas aeruginosa (PAO1) bacteria. In dyes removal process, the effects of important variables such as initial concentration of dyes, adsorbent mass, pH and sonication time on adsorption process optimized by Taguchi approach. Optimum values of 4, 0.02 g, 4 min, 10 mg L(-1) were obtained for pH, AC-HKUST-1 MOF mass, sonication time and the concentration of each dye, respectively. At the optimized condition, the removal percentages of CV, DSB and QY were found to be 99.76%, 91.10%, and 90.75%, respectively, with desirability of 0.989. Kinetics of adsorption processes follow pseudo-second-order model. The Langmuir model as best method with high applicability for representation of experimental data, while maximum mono layer adsorption capacity for CV, DSB and QY on AC-HKUST-1 estimated to be 133.33, 129.87 and 65.37 mg g(-1) which significantly were higher than HKUST-1 as sole material with Qm to equate 59.45, 57.14 and 38.80 mg g(-1), respectively.


Assuntos
Antibacterianos/farmacologia , Corantes/isolamento & purificação , Ultrassom , Adsorção , Corantes/farmacologia , Cinética , Testes de Sensibilidade Microbiana , Microscopia Eletrônica de Transmissão , Espectroscopia de Infravermelho com Transformada de Fourier
13.
Spectrochim Acta A Mol Biomol Spectrosc ; 153: 257-67, 2016 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-26318700

RESUMO

In this work, central composite design (CCD) combined with response surface methodology (RSM) and desirability function approach (DFA) gives useful information about operational condition and also to obtain useful information about interaction and main effect of variables concerned to simultaneous ultrasound-assisted removal of brilliant green (BG) and eosin B (EB) by zinc sulfide nanoparticles loaded on activated carbon (ZnS-NPs-AC). Spectra overlap between BG and EB dyes was extensively reduced and/or omitted by derivative spectrophotometric method, while multi-layer artificial neural network (ML-ANN) model learned with Levenberg-Marquardt (LM) algorithm was used for building up a predictive model and prediction of the BG and EB removal. The ANN efficiently was able to forecast the simultaneous BG and EB removal that was confirmed by reasonable numerical value i.e. MSE of 0.0021 and R(2) of 0.9589 and MSE of 0.0022 and R(2) of 0.9455 for testing data set, respectively. The results reveal acceptable agreement among experimental data and ANN predicted results. Langmuir as the best model for fitting experimental data relevant to BG and EB removal indicates high, economic and profitable adsorption capacity (258.7 and 222.2 mg g(-1)) that supports and confirms its applicability for wastewater treatment.

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