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Sustainable ferrate oxidation: Reaction chemistry, mechanisms and removal of pollutants in wastewater
2021
Dar, Afzal Ahmed | Pan, Bao | Qin, Jiani | Zhu, Qiuhui | Lichtfouse, Eric | ʻUs̲mān, Muḥammad | Wang, Chuanyi
This review is intended to evaluate the use of ferrate (Fe(VI)), being a green coagulant, sustainable and reactive oxidant, to remove micro pollutants especially pharmaceutical pollutants in contaminated water. After a brief description of advanced oxidation processes, fundamental dimensions regarding the nature, reactivity, and chemistry of this oxidant are summarized. The degradation of contaminants by Fe(VI) involves several mechanisms and reactive agents which are critically evaluated. The efficiency and chemistry of Fe(VI) oxidation differs according to the reaction conditions and activation agent, such as soluble Fe(VI) processes, which involve Fe(VI), UV light, and electro-Fe(VI) oxidation. Fe(VI) application methods (including single dose, multiple doses, chitosan coating etc), and Fe(VI) with activating agents (including sulfite, thiosulfate, and UV) are also described to degrade the micro pollutants. Besides, application of Fe(VI) to remove pharmaceuticals in wastewater are intensely studied. Electrochemical prepared Fe(VI) has more wide application than wet oxidation method. Meanwhile, we elaborated Fe(VI) performance, limitations, and proposed innovative aspects to improve its stability, such as the generation of Fe(III), synergetic effects, nanopores entrapment, and nanopores capsules. This study provides conclusive direction for synergetic oxidative technique to degrade the micro pollutants.
Show more [+] Less [-]Ferrate (VI)-mediated transformation of diethyl phthalate (DEP) in soil: Kinetics, degradation mechanisms and theoretical calculation
2021
Yu, Yao | Qi, Yumeng | Li, Chenguang | Cao, Wanming | Chen, Jing | Qu, Ruijuan | Zhou, Dongmei | Wang, Zunyao
Diethyl phthalate (DEP), as a kind of universally used plasticizer, has aroused considerable public concern owing to its wide detection, environmental stability, and potential health risks. In this work, the highly efficient removal of DEP by ferrate (VI) (Fe(VI)) was systematically explored in soil environment. The effects of the oxidant dosages, soil types, as well as the presence of coexisting cations and anions in tested soil on DEP removal were evaluated. When the dosage of Fe(VI) was 20 mM, complete removal of DEP (50 μg/g) was achieved in the tested soil after 2 min of reaction. Furthermore, the removal rate of DEP was closely related to the soil types, and the degradation rates were decreased obviously in red soil (RS), black soil (BS) and paddy soil (PS), probably due to the acidic condition and high content of organic matters. Moreover, the presence of Ca²⁺, Mg²⁺ and Al³⁺ in soil can inhibit the removal of DEP by Fe(VI), while SO₄²⁻ has an slightly promotion effect. Six oxidation intermediates were detected in the reaction process of DEP, product analysis revealed that the transformation of DEP was mainly through two pathways, including hydrolysis and hydroxylation reactions, which were probably mediated by oxygen atom transfer process of Fe(VI). Based on the frontier electron density theory calculation, two ester groups of DEP were prone to be attacked by Fe(VI), and the hydroxyl addition tended to occur at the para-position of one of the ester groups on the benzene ring. This study provides a novel approach for phthalate esters removal from soil using Fe(VI) oxidation and shows new insights into the oxidation mechanisms.
Show more [+] Less [-]In-depth investigation of Sodium percarbonate as oxidant of PAHs from soil contaminated with diesel oil
2021
Cavalcanti, Jorge Vinicius Fernandes Lima | Fraga, Tiago José Marques | Loureiro Leite, Mirella de Andrade | dos Santos e Silva, Daniella Fartes | de Lima, Valmir Félix | Schuler, Alexandre Ricardo Pereira | do Nascimento, Clístenes Williams Araújo | da Motta Sobrinho, Maurício Alves
Sodium percarbonate (SPC, 2Na₂CO₃∙3H₂O₂), is a compound that can be used under multiple environmental applications. In this work, SPC was employed as oxidant in the treatment of soil contaminated with diesel oil. The soil samples were collected during the earthmoving stage of RNEST Oil Refinery (Petrobras), Brazil. Then, the samples were air-dried, mixed and characterized. Subsequently, raw soil was contaminated with diesel and treated by photo-Fenton reaction (H₂O₂/Fe²⁺/UV). SPC played a significant role in the generation of hydroxyl radicals under the catalytic effect of ferrous ions (Fe²⁺), hydrogen peroxide (H₂O₂) and radiation. These radicals provoked the photodegradation of polycyclic aromatic hydrocarbons (PAHs), in the soil remediation. A factorial design 3³ was carried out to assess the variables which most influenced the decrease in total organic carbon (TOC). The study was performed with the following variables: initial concentration of [H₂O₂] and [Fe²⁺], between 190.0 and 950.0 mmol L⁻¹ and 0.0–14.4 mmol L⁻¹, respectively. UV radiation was supplied from sunlight, blacklight lamps, and system without radiation. All experiments were performed with 5.0 g of contaminated soil in 50.0 mL of solution. The initial concentration of Fe²⁺ showed the statistically most significant effect. The oxidation efficiency evaluated in the best condition showed a decrease from 34,765 mg kg⁻¹ to 15,801 mg kg⁻¹ in TOC and from 85.750 mg kg⁻¹ to 20.770 mg kg⁻¹ in PAHs content. Moreover, the sums of low and high molecular weight polycyclic aromatic hydrocarbons (LMW-PAHs and HMW-PAHs) were 19.537 mg kg⁻¹ and 1.233 mg kg⁻¹, respectively. Both values are within the limits recommended by the United Sates Environmental Protection Agency (USEPA) and evidenced the satisfactory removal of PAHs from contaminated soil, being an alternative to classic oxidation protocols.
Show more [+] Less [-]Understanding the true effects of the COVID-19 lockdown on air pollution by means of machine learning
2021
Lovrić, Mario | Pavlović, Kristina | Vuković, Matej | Grange, Stuart K. | Haberl, Michael | Kern, Roman
During March 2020, most European countries implemented lockdowns to restrict the transmission of SARS-CoV-2, the virus which causes COVID-19 through their populations. These restrictions had positive impacts for air quality due to a dramatic reduction of economic activity and atmospheric emissions. In this work, a machine learning approach was designed and implemented to analyze local air quality improvements during the COVID-19 lockdown in Graz, Austria. The machine learning approach was used as a robust alternative to simple, historical measurement comparisons for various individual pollutants. Concentrations of NO₂ (nitrogen dioxide), PM₁₀ (particulate matter), O₃ (ozone) and Oₓ (total oxidant) were selected from five measurement sites in Graz and were set as target variables for random forest regression models to predict their expected values during the city’s lockdown period. The true vs. expected difference is presented here as an indicator of true pollution during the lockdown. The machine learning models showed a high level of generalization for predicting the concentrations. Therefore, the approach was suitable for analyzing reductions in pollution concentrations. The analysis indicated that the city’s average concentration reductions for the lockdown period were: -36.9 to −41.6%, and −6.6 to −14.2% for NO₂ and PM₁₀, respectively. However, an increase of 11.6–33.8% for O₃ was estimated. The reduction in pollutant concentration, especially NO₂ can be explained by significant drops in traffic-flows during the lockdown period (−51.6 to −43.9%). The results presented give a real-world example of what pollutant concentration reductions can be achieved by reducing traffic-flows and other economic activities.
Show more [+] Less [-]Phenylurea herbicide degradation and N-nitrosodimethylamine formation under various oxidation conditions: Relationships and transformation pathways
2021
Wang, Wanfeng | Yang, Panqing | Guo, Yanling | Ji, Haoran | Liang, Fang
Four phenylurea herbicides (PUHs) were assessed for degradation and transformation into N-nitrosodimethylamine (NDMA) under three oxidation conditions (chlorine (Cl₂), chlorine dioxide (ClO₂), and ozone (O₃)) from an aqueous solution. Removal ratios correlated with the numbers of halogen elements contained in PUHs (isoproturon ₍₀₎ > chlorotoluron ₍₁ Cₗ₎ > diuron ₍₂ Cₗ₎ > fluometuron ₍₃ F₎), and the degradation efficiencies of oxidants from fastest to slowest were: O₃, ClO₂, and Cl₂. NDMA can be generated directly from the ozonation of PUHs. Further, compared with chloramination alone, ozonation prominently promoted NDMA formation potential (NDMA-FP) during post-chloramination, and NDMA-FPs increased approximately 23–68 times than those during ozonation only at 2.5 mg/L O₃ over 10 min; molar yields of NDMA from highest to lowest were 11.1% (isoproturon), 1.17% (chlorotoluron), 1.0% (diuron), and 0.73% (fluometuron). The PUH degradation kinetics data during ozonation agreed with the pseudo-first-order model. The rate constant kₒbₛ were 0.31 × 10⁻³–19.8 × 10⁻³ s⁻¹. The kₒbₛ and removal ratios of PUHs during ozonation partially scaled with the mass, LogKₒw, and Henry’s constants of PUHs. Comparisons of measured NDMA-FPs with calculated NDMA-FPs from residual PUH after oxidation showed that the intermediates produced during ozonation facilitated NDMA-FPs; this contribution was also observed for chlorotoluron and isoproturon during ClO₂ oxidation. Examination of reaction mechanisms revealed that tertiary amine ozonation, N-dealkylation, hydroxylation, the cleavage of N–C bonds, ammonification, and nitrification occurred during the ozonation of PUHs, and the dimethylamine (DMA) functional groups could be decomposed directly and transformed into NDMA via the formation of the intermediate unsymmetrical dimethylhydrazine. NDMA is also formed from the reaction between DMA and phenylamino-compounds. Clarifying primary degradation products of PUHs and transformation pathways of NDMA during oxidation processes is useful to optimize treatment processes for water supplies.
Show more [+] Less [-]Column tests for evaluation of the enzymatic biodegradation capacity of hydrocarbons (C10–C50) contaminated soil
2021
Kadri, Tayssir | Robert, Thomas | Rouissi, Tarek | Sebastian, Joseph | Magdouli, Sara | Brar, Satinder Kaur | Martel, Richard | Lauzon, Jean-Marc
Though many studies pertaining to soil bioremediation have been performed to study the microbial kinetics in shake flasks, the process efficiency in column tests is seldom. In the present study, soil columns tests were carried out to study the biodegradation of soil contaminated with a high concentration of diesel (≈19.5 g/kg) petroleum hydrocarbons expressed as C₁₀–C₅₀. Experiments were done with crude enzymatic cocktail produced by the hydrocarbonoclastic bacterium, Alcanivorax borkumensis. A. borkumensis was grown on a media with 3% (v/v) motor oil as the sole carbon and energy source. The effects of the enzyme concentration, treatment time and oxidant on the bioremediation efficiency of C₁₀–C₅₀ were investigated. A batch test was also carried out in parallel to investigate the stability of the enzymes and the effect of the biosurfactants on the desorption and the bioconversion of C₁₀–C₅₀. Batch tests indicated that the biosurfactants significantly affected the desorption and alkane hydroxylase and lipase enzymes, maintained their catalytic activity during the 20-day test, with a half-life of 7.44 days and 8.84 days, respectively. The crude enzyme cocktail, with 40 U/mL of lipase and 10 U/mL of alkane hydroxylase, showed the highest conversion of 57.36% after 12 weeks of treatment with a degradation rate of 0.0218 day⁻¹. The results show that the soil column tests can be used to optimize operating conditions for hydrocarbon degradation and to assess the performance of the overall bioremediation process.
Show more [+] Less [-]Solar photocatalytic degradation of ibuprofen with a magnetic catalyst: Effects of parameters, efficiency in effluent, mechanism and toxicity evolution
2021
Gong, Han | Zhu, Wei | Huang, Yumei | Xu, Lijie | Chen, Meijuan | Yan, Muting
The environmental-friendly photocatalytic process with a magnetic catalyst CoFe₂O₄/TiO₂ mediated by solar light for ibuprofen (IBP) degradation in pure water, wastewater effluent and artificial seawater was investigated systematically. The study aims to reveal the efficiency, the mechanism and toxicity evolution during IBP degradation. Hydroxyl radicals and photo-hole (h⁺) were found to contribute to the IBP decay. The presence of SO₄²⁻ showed no significant effect, while NO₃⁻ accelerated the photodegradation, and other anions including HCO₃⁻, Cl⁻, F⁻, and Br⁻ showed significant inhibition. The removal efficiency was significantly elevated with the addition of peroxymonosulfate (PMS) or persulfate (PS) ([Oxidant]₀:[IBP]₀ = 0.4–4), with reaction rate of 5.3–13.1 and 1.3–2.9 times as high as the control group, respectively. However, the reaction was slowed down with the introduction of H₂O₂. A mathematic model was employed to describe the effect of ferrate, high concentration or stepwise addition of ferrate was suggested to play a positive role in IBP photodegradation. Thirteen transformation products were identified and five of them were newly reported. The degradation pathways including hydroxylation, the benzene ring opening and the oxidation of carbon were proposed. IBP can be efficiently removed when spiked in wastewater and seawater despite the decreased degradation rate by 41% and 56%, respectively. Compared to the IBP removal, mineralization was relatively lower. The adverse effect of the parent compound IBP to the green algae Chlorella vulgaris was gradually eliminated with the decomposition of IBP. The transformation product C178a which possibly posed toxicity to rotifers Brachionus calyciflorus can also be efficiently removed, indicating that the photocatalysis process is effective in IBP removal, mineralization and toxicity elimination.
Show more [+] Less [-]Triphenyl methyl phosphonium tosylate as an efficient phase transfer catalyst for ultrasound-assisted oxidative desulfurization of liquid fuel
2021
Desai, Komal | Dharaskar, Swapnil | Khalid, Mohammad | Gupta, Thummalapalli Chandra Sekhara Manikyam
The novel phosphonium-based ionic liquid (IL), triphenyl methyl phosphonium tosylate ([TPMP][Tos]), has been synthesized and applied as a phase transfer catalyst (PTC) in the ultrasound-assisted oxidative desulfurization (UAODS). Oxidation of model fuel (MF) containing dibenzothiophene (DBT) was carried out using an equimolar mixture of H₂O₂-CH₃COOH as an oxidant at 40–70 °C in the presence of IL. The sulfur compound is converted into polar sulfone, and the maximum desulfurization efficiency was examined. The effect of process parameters such as reaction temperature, reaction time, molar ratio of oxidant to sulfur (n(O/S)), and the mass ratio of ionic liquid to model fuel (m(IL/MF)) was studied, and the conditions for maximizing the DBT conversion rate were found. Maximum conversion (> 99%) was obtained at a temperature of 70 °C with m(IL/MF) of 0.8. The oxidation reactivity of various sulfur compounds was studied at different time intervals. To verify the effect of ionic liquid and ultrasound irradiation, extractive desulfurization (EDS), oxidative desulfurization (ODS), and UAODS in the presence of IL were carried out. The experimental results show that the UAODS process gives the highest desulfurization efficiency. A kinetic study was performed to estimate the rate constant and the order of oxidation reaction.
Show more [+] Less [-]Potential therapeutic effect of Chrysopogon zizanioides (Vetiver) as an anti-inflammatory agent
2021
Grover, Madhuri | Behl, Tapan | Bungau, Simona | Aleya, Lotfi
Vetiver has a broad history of traditional medicinal uses, but only a handful of research article has reported its utility in treating diseases. But unfortunately, no work has been reported on the anti-inflammatory activity of its plant extract and inflammatory-linked diseases. Hence, the present review focuses on investigating the several presumptions which can be put forward to explain its anti-inflammatory property. Thus, for ensuring the same, all the databases like science direct, PubMed, book chapters, and other authenticated papers were thoroughly studied to present a connection between inflammation and the plant potential. After gaining enough knowledge on pathogenesis of inflammation, it has been observed that the release of mediators from the arachidonic acid metabolism pathway and generation of oxidative and nitrogen species are presented as the main reason for the occurrence of inflammation condition. The stimulation of antioxidant enzyme system network by the plant extract reduces the level of oxidative stress, creating a balance between oxidant and antioxidant system. Moreover, its antimicrobial activity will prevent the biological source of stimulation towards injury and the CNS depressant effect will subside the pain of inflammation. Amalgamating all the factors together, the plant can be utilized as anti-inflammatory can be and also can be proved as a beneficial perspective in the treatment of inflammation-linked disorders.
Show more [+] Less [-]Oxidation of benzophenone-3 in aqueous solution by potassium permanganate: kinetics, degradation products, reaction pathways, and toxicity assessment
2021
Cao, Wanming | Wu, Nannan | Qu, Ruijuan | Sun, Cheng | Huo, Zongli | Ajarem, Jamaan S. | Allam, Ahmed A. | Wang, Zunyao | Zhu, Feng
Benzophenone-3 (BP-3) is used in a wide range of personal care products and plastics to resist ultraviolet light, which has aroused considerable public concern due to its endocrine-disrupting effects. In this work, we systematically investigated the chemical oxidation process of BP-3 by KMnO₄. The influences of several factors, such as pH, oxidant dose, temperature, coexisting water constituents, and water matrices, on BP-3 degradation efficiency were evaluated. The removal rate of 10 μM BP-3 could reach 91.3% in 2 h under the conditions of pH = 8.0, [BP-3]₀:[KMnO₄]₀ = 1:20, and T = 25 °C, with the observed rate constant (kₒbₛ) value of 0.0202 min⁻¹. The presence of typical anions (Cl⁻, NO₃⁻, SO₄²⁻) and HA could slightly increase BP-3 removal, while HCO₃⁻ caused a relatively significant promotion of BP-3 degradation. On the basis of mass spectrometry and theoretical calculations, hydroxylation, direct oxidation, and carbon–carbon bridge bond cleavage were mainly involved in the oxidation process. Toxicity assessment revealed that the acute and chronic toxicities were reduced significantly, which suggested KMnO₄ is a promising technique for BP-3 removal.
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