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1.
J Environ Manage ; 365: 121441, 2024 Jun 18.
Artigo em Inglês | MEDLINE | ID: mdl-38897076

RESUMO

In response to environmental concerns at the global level, there is considerable momentum in the exploration of materials derived from waste that are both sustainable and eco-friendly. In this study, CS-Fe (carbon, silica, and iron) composite was synthesized from coal gasification slag (CGS) and innovatively applied as a catalyst to activate PS (persulfate) for the degradation of trichloroethylene (TCE) in water. Scanning electron microscope (SEM), fourier transmission infrared spectroscopy (FTIR), energy dispersive x-ray spectroscopy (EDS), brunauer, emmet, and teller (BET) technique, and x-ray diffractometer (XRD) spectra were employed to investigate the surface morphology and physicochemical composition of the CS-Fe composite. CS-Fe catalyst showed a dual nature by adsorption and degradation of TCE simultaneously, displaying 86.1% TCE removal in 3 h. The synthesized CS-Fe had better adsorption (62.1%) than base material CGS (36.4%) due to a larger BET surface area (770.8 m2 g-1), while 24.0% TCE degradation was recorded upon the activation of PS by CS-Fe. FTIR spectra confirmed the adsorption and degradation of TCE by investigating the used and fresh samples of CS-Fe catalyst. Scavengers and Electron paramagnetic resonance (EPR) analysis confirmed the availability of surface radicals and free radicals facilitated the degradation process. The acidic nature of the solution favored the degradation while the presence of bicarbonate ion (HCO3-) hindered this process. In conclusion, these results for real groundwater, surfactant-added solution, and degradation of other TCE-like pollutants propose that the CS-Fe composite offers an economically viable and favorable catalyst in the remediation of organic contaminants within aqueous solutions. Further investigation into the catalytic potential of coal gasification slag-based carbon materials and their application in Fenton reactions is warranted to effectively address a range of environmental challenges.

2.
Environ Pollut ; 333: 122062, 2023 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-37330185

RESUMO

Rapid growth and industrialization have become a major threat to water contamination with carcinogenic chlorinated hydrocarbons such as trichloroethylene (TCE). Therefore, this study aims to assess the TCE degradation performance through advanced oxidation process (AOP) using catalyst FeS2 in combination with oxidants persulfate (PS), peroxymonosulfate (PMS), and hydrogen peroxide (H2O2) in PS/FeS2, PMS/FeS2, and H2O2/FeS2 systems, respectively. TCE concentration was analyzed using gas chromatography (GC). The results found the trend for TCE degradation by the systems was PMS/FeS2>PS/FeS2>H2O2/FeS2 (99.84, 99.63, and 98.47%, respectively). Degradation of TCE was analyzed at different pH ranges (3-11) and maximum degradation at a wide pH range was observed for PMS/FeS2. The analysis using electron paramagnetic resonance (EPR) and scavenging tests explored responsible reactive oxygen species (ROS) for TCE degradation and found that HO• and SO4-• played the most effective role. The results of catalyst stability showed PMS/FeS2 system the most promising with the stability of 99, 96 and 50% for the first, second and third runs, respectively. The system was also found efficient in the presence of surfactants (TW-80, TX-100, and Brij-35) in ultra-pure water (89.41, 34.11, 96.61%, respectively), and actual groundwater (94.37, 33.72, and 73.48%, respectively), but at higher reagents dosages (5X for ultra-pure water and 10X actual ground water). Furthermore, it is demonstrated that the oxic systems have degradation capability for other TCE-like pollutants. In conclusion, due to its high stability, reactivity, and cost-effectiveness, PMS/FeS2 system could be a better choice for the treatment of TCE contaminated water and can be beneficial for field application.


Assuntos
Água Subterrânea , Tricloroetileno , Poluentes Químicos da Água , Peróxido de Hidrogênio/análise , Ferro/química , Tricloroetileno/análise , Água/análise , Oxirredução , Poluentes Químicos da Água/análise , Água Subterrânea/química
3.
Water Environ Res ; 94(4): e10710, 2022 Mar 23.
Artigo em Inglês | MEDLINE | ID: mdl-35373447

RESUMO

Few researches have focused on the role of nanoscale zero-valent iron (nZVI) in Fenton-like process for polycyclic aromatic hydrocarbons (PAHs) removal. In this study, the naphthalene (NAP) degradation tests in ultrapure water showed that nZVI addition could enhance NAP degradation from 79.7% to 99.0% in hydrogen peroxide (H2 O2 )/Fe (II)/nZVI/NAP system at the molar ratio of 10/5/3/1, showing the excellent role of nZVI in promoting NAP removal. Multiple linear regression analysis found that the correlation coefficient between H2 O2 consumption and NAP degradation was converted from -9.17 to 0.48 with nZVI and 1-mM H2 O2 , indicating that nZVI could decompose H2 O2 more beneficially for NAP degradation. Multiple Fe (II)-dosing and iron leaching tests revealed that nZVI could gently liberate Fe (II) and promote Fe (II)/Fe (III) redox cycle to enhance the NAP degradation. When the H2 O2 /Fe (II)/nZVI/NAP molar ratios of 10/5/3/1 and 50/25/15/1 were applied in the simulated NAP contaminated actual groundwater and soil slurry, respectively, 75.0% and 82.9% of NAP removals were achieved. Based on the major degradation intermediates detected by GC/MS, such as 1,4-naphthalenedione, cinnamaldehyde, and o-phthalaldehyde, three possible NAP degradation pathways were proposed. This study provided the applicable potential of nZVI in Fenton process for PAHs contaminated groundwater and soil remediation. PRACTITIONER POINTS: nZVI enhanced the NAP degradation in Fenton-like process. Three schemes of NAP degradation pathway were proposed. nZVI performed well in the remediation of the simulated NAP contamination.

4.
J Hazard Mater ; 416: 125935, 2021 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-34492864

RESUMO

Carbonaceous materials (CMs) have been applied extensively for enhancing the catalytic performance of environmental catalysts, however, the self-catalytic mechanism of CMs for groundwater remediation is rarely investigated. Herein, we unveiled the catalytic ability of various CMs via Fe(III) reduction through polyvinyl alcohol-coated calcium peroxide nanoparticles (PVA@nCP) for trichloroethylene (TCE) removal. Among selected CMs (graphite (G), biochar (BC) and activated carbon (AC)), BC and AC showed enhancement of TCE removal of 89% and 98% via both adsorption and catalytic degradation. BET and SEM analyses showed a higher adsorption capacity of AC (27.8%) than others. The generation of solution-Fe(II) and surface-Fe(II) revealed the reduction of Fe(III) on CMs-surface. The role of O-containing groups was investigated by the FTIR technique and XPS quantified the 52% and 57% surface-Fe(II) in BC and AC systems, respectively. EPR and quenching tests confirmed that both solution and surface-bound species (HO•, O2-• and 1O2) contributed to TCE degradation. Acidic pH condition encouraged TCE removal and the presence of HCO3- negatively affected TCE removal than other inorganic ions. Both schemes (PVA@nCP/Fe(III)/BC and PVA@nCP/Fe(III)/AC) exhibited promising results in the actual groundwater, surfactant-amended solution, and removal of other chlorinated-pollutants, opening a new direction towards green environmental remediation for prolonged benefits.


Assuntos
Água Subterrânea , Nanopartículas , Tricloroetileno , Poluentes Químicos da Água , Preparações de Ação Retardada , Compostos Férricos , Oxirredução , Poluentes Químicos da Água/análise
5.
J Hazard Mater ; 420: 126589, 2021 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-34329106

RESUMO

In this study, amorphous boron was employed as a reductant in traditional Fenton system for the first time to accelerate the regeneration of Fe(II). The degradation of 1,2-dichloroethane (DCA) was only 40.0% in Fenton system, while in the presence of amorphous boron, it could reach to 93.0% in 60 min. HO• was demonstrated to be the major reactive oxygen species (ROSs) and responsible for DCA degradation. Further, the mechanism of amorphous boron-enhanced Fenton system was described as follows. With the addition of amorphous boron, the reduction process occurred on its surface and Fe(III) was regenerated to Fe(II) to further utilize H2O2 and produce more HO• for DCA removal. Meanwhile, amorphous boron was oxidized to B2O3 and a portion of H3BO3 leaching into the solution occurred. Both B2O3 and H3BO3 had no reactivity for Fe(III) reduction. Moreover, DCA could be entirely dechlorinated and mineralized to CO2, Cl- and H2O. Vinyl chloride (VC) and dichloromethane (DCM) were the mainly intermediates in DCA degradation and two possible pathways were inferred. Eventually, the performance of DCA degradation in complex solution matrixes and for other contaminants removal were tested, demonstrating the broad-spectrum reactivity and superiority of amorphous boron-enhanced Fenton system in the remediation of contaminated groundwater.

6.
Sci Total Environ ; 794: 148674, 2021 Nov 10.
Artigo em Inglês | MEDLINE | ID: mdl-34214820

RESUMO

A novel catalyst of sulfidated iron-nickel supported on biochar (S-FeNi@BC) was synthesized to activate persulfate (PS) for the removal of trichloroethylene (TCE). A number of techniques including XRD, SEM, TEM, FTIR, BET and EDS were employed to characterize S-FeNi@BC. The influence of sulfur to iron ratio (S/F) on TCE removal was investigated by batch experiments and a higher TCE removal (98.4%) was achieved at 0.22/1 ratio of S/F in the PS/S-FeNi@BC oxidation system. A dominant role in iron species conversion was noticed by the addition of sulfur in FeNi@BC system. Significant enhancement in recycling of the dissolved and surface Fe(II) was confirmed which contributed to the generation of free and surface-bound active radical species (OH, O2-, 1O2, SO4-). Further, the presence and contribution of these radicals were validated by the electron paramagnetic resonance (EPR) and quenching study. In addition, XPS results demonstrated the dominant role of S(-II) with the increase of Fe(II) from 36.3% to 58.6% and decrease of Fe(III) from 52.1% to 39.8% in the PS/S-FeNi@BC system. In crux, the influence of initial pH, catalyst dosage, oxidant dosage, and inorganic ions (HCO3-, Cl-, NO3- and SO42-) on TCE removal was also investigated. The findings obtained from this study suggest that S-FeNi@BC is an appropriate catalyst to activate PS for TCE contaminated groundwater remediation.


Assuntos
Água Subterrânea , Tricloroetileno , Poluentes Químicos da Água , Compostos Férricos , Oxirredução , Espécies Reativas de Oxigênio , Tricloroetileno/análise , Poluentes Químicos da Água/análise
7.
Chemosphere ; 281: 130798, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34000655

RESUMO

In this study, the common chlorinated solvent trichloroethene (TCE) was selected as the target contaminant. The aqueous solution after solubilization treatment (containing TCE and sodium dodecyl sulfate (SDS)) was used as the research object to carry out the remediation technology research of citric acid (CA) enhanced Fe(II) activation in sodium percarbonate (SPC) system. In 0.15 mM TCE and 1 critical micelle concentration (CMC) SDS solution, CA chelating Fe(II) activated SPC could effectively promote 93.2% degradation of TCE when the dosages of SPC, Fe(II) and CA were 3.0, 6.0 and 3.0 mM, respectively. SDS had a significant inhibitory effect on the degradation of TCE, and the surface tension changed after the reaction. The addition of CA greatly increased the generation of hydroxyl radicals (HO) in the system, while the removal of TCE was mainly attributed to HO, and the removed TCE was almost completely dechlorinated. The pH range from 3 to 7 could keep the TCE degradation above 80.0%. In the actual groundwater remediation, this technique could also efficiently degrade TCE (including SDS), showing a great application potential and development prospective in practice.


Assuntos
Água Subterrânea , Tricloroetileno , Poluentes Químicos da Água , Carbonatos , Ácido Cítrico , Compostos Ferrosos , Oxirredução , Estudos Prospectivos , Dodecilsulfato de Sódio , Poluentes Químicos da Água/análise
8.
J Hazard Mater ; 407: 124814, 2021 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-33338809

RESUMO

The mechanism of surfactants in surfactant-in situ chemical oxidation (S-ISCO) coupled process for trichloroethene (TCE) degradation was firstly reported. The performance of TCE solubilization and inhibition of TCE degradation in three nonionic surfactants (TW-80, Brij-35, TX-100) in PS/Fe(II)/citric acid (CA) system was compared and TW-80 was evaluated to be the optimal surfactant in S-ISCO coupled process due to the best TCE solubilizing ability and minimal inhibition for TCE degradation (only 31.8% TCE inhibition in the presence of 1 g L-1 TW-80 surfactant). The inhibition mechanism in TCE degradation was also demonstrated by comparing the strength of ROSs and PS utilization. In the presence of TW-80 (1 g L-1), over 97.5% TCE was removed at the PS/Fe(II)/CA/TCE molar ratio of 30/4/4/1, in which more than 86.7% TCE was dechlorinated. The result of scavenger experiments revealed that the dominant radicals were HO• and SO4-• in PS/Fe(II)/CA system in TW-80 containing aqueous solution, among which SO4-• performed a greater role in TCE removal. Moreover, over 85.3% TCE degradation in actual groundwater revealed the potential of PS/Fe(II)/CA process for actual groundwater remediation in containing TW-80 of TCE contaminant. This research provided a novel alternative technology for groundwater remediation with TCE contaminant when containing surfactants.

9.
Environ Sci Pollut Res Int ; 28(3): 3121-3135, 2021 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-32902746

RESUMO

In this study, the enhanced trichloroethylene (TCE) degradation performance was investigated by polyvinyl alcohol coated calcium peroxide nanoparticles (PVA@nCP) as an oxidant in Fe(II)-based catalytic systems. The nanoscale iron sulfide (nFeS), having an average particle size of 115.4 nm, was synthesized in the laboratory and characterized by SEM, TEM, HR-TEM along with EDS elemental mapping, XRD, FTIR, ICP-OES, and XPS techniques. In only ferrous iron catalyzed system (PVA@nCP/Fe(II)), TCE degradation was recorded at 58.9% in 6 h. In comparison, this value was increased to 97.5% or 99.7% with the addition of citric acid (CA) or nFeS in PVA@nCP/Fe(II) system, respectively. A comparative study was performed with optimum usages of chemical reagents in both PVA@nCP/Fe(II)/CA and PVA@nCP/Fe(II)/nFeS systems. Further, the probe compounds tests and electron paramagnetic resonance (EPR) analysis confirmed the generation of reactive oxygen species. The scavenging experiments elucidated the dominant role of HO• to TCE degradation, particularly in PVA@nCP/Fe(II)/nFeS system. Both CA and nFeS strengthened PVA@nCP/Fe(II) system, but displayed completely different mechanisms in the enhancement of active radicals generation; hence, their different contribution to TCE degradation. The acidic environment was favorable for TCE degradation, and a high concentration of HCO3- inhibited TCE removal in both systems. Conclusively, compared to PVA@nCP/Fe(II)/nFeS system, PVA@nCP/Fe(II)/CA system resulted in encouraging TCE degradation outcomes in actual groundwater, showing great potential for prolonged benefits in the remediation of TCE polluted groundwater. Graphical abstract.


Assuntos
Água Subterrânea , Nanopartículas , Tricloroetileno , Poluentes Químicos da Água , Catálise , Ácido Cítrico , Compostos Ferrosos , Oxirredução , Peróxidos , Álcool de Polivinil , Poluentes Químicos da Água/análise
10.
Water Sci Technol ; 82(5): 998-1008, 2020 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-33031076

RESUMO

The feasibility of an advanced oxidation process based upon sodium persulfate (SPS) activated simultaneously by heat (50 °C) and nanoscale zero-valent iron (nZVI) on benzene removal was investigated. The experimental results strongly showed the synergistic effect of thermal and nZVI activation to SPS and benzene removal was enhanced with the increase of SPS/nZVI/benzene molar ratio. Specifically, 94% of benzene could be removed in 1 hr at 50 °C at the SPS/nZVI/benzene molar ratio of 10/5/1. The radical scavenger tests and electron paramagnetic resonance (EPR) analysis confirmed that SO4•- was the predominant species contributing to benzene degradation. Further, the effects of the solution matrix on benzene elimination were investigated. The results indicated that benzene destruction in the thermally activated SPS/nZVI system performed better under acidic conditions, and the high concentration of both Cl- and HCO3 - had adverse effects on benzene elimination. The test for the performance of benzene degradation in the actual groundwater demonstrated that benzene could be degraded entirely at SPS/nZVI/benzene molar ratio of 40/40/1 at 50 °C, indicating that the synergistic catalysis of thermal and nZVI activation to SPS is exploitable and the thermally activated SPS/nZVI system can be applicable to the remediation of benzene contaminated groundwater.


Assuntos
Água Subterrânea , Poluentes Químicos da Água , Benzeno , Ferro , Oxirredução , Poluentes Químicos da Água/análise
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