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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.
Afficher plus [+] Moins [-]Activation of sulfite autoxidation with CuFe2O4 prepared by MOF-templated method for abatement of organic contaminants
2020
Zhao, Xiaodan | Wu, Wenjing | Jing, Guohua | Zhou, Zuoming
Copper ferrite (denoted as CuFe₂O₄MOF), prepared via a complexation reaction to obtain bimetal–organic frameworks (Cu/Fe bi-MOFs), followed by a combustion process to remove the MOF template, is employed as a heterogeneous activator to promote sulfite autoxidation for the removal of organic contaminants. At pH 8.0, more than 80% of the recalcitrant organic contaminant iohexol (10 μM) can be removed within 2 min by the activation of sulfite (500 μM) with CuFe₂O₄MOF (0.1 g L⁻¹). CuFe₂O₄MOF exhibits more pronounced catalytic activity in accelerating sulfite autoxidation for iohexol abatement compared to that fabricated by hydrothermal and sol–gel combustion methods. Radical quenching studies suggest that the sulfate radical (SO₄•⁻) is the main reactive species responsible for iohexol abatement. The performance of CuFe₂O₄MOF/sulfite for iohexol abatement can be affected by several critical influencing factors, including the solution pH and the presence of humic acid, Cl⁻, and HCO₃⁻. The effect of the ionic strength and the results of the attenuated total reflectance–Fourier transform infrared (ATR–FTIR) analysis indicate that sulfite autoxidation in the presence of CuFe₂O₄MOF involves an inner-sphere interaction with the surface Cu(II) sites of CuFe₂O₄MOF. X-ray photoelectron spectroscopy (XPS) characterization suggests that the surface Cu(II)–Cu(I)–Cu(II) redox cycle is responsible for efficient SO₄•⁻ production from sulfite. Overall, CuFe₂O₄MOF can be considered an alternative activator for sulfite autoxidation for potential application in the treatment of organic-contaminated water.
Afficher plus [+] Moins [-]Water management impacts the soil microbial communities and total arsenic and methylated arsenicals in rice grains
2019
The bioavailability of the metalloid arsenic (As) in paddy soil is controlled by microbial cycling of As and other elements such as iron (Fe) and sulfur (S), which are strongly influenced by water management in paddy fields. In this study, we evaluated how water management affects As bioavailability by growing rice plants in a geogenic As-contaminated soil. We determined As speciation in soil porewater and the diversity of the associated microbial community. Continuous flooding enhanced the release of Fe and As and increased arsenite (As(III)) and methylated As species concentrations in the rice grain compared with aerobic treatment. Total inorganic and organic As in the grain was 84% and 81% lower, respectively, in the aerobic treatment compared with the continuous flooding treatment. The amounts of Fe(III)-reducing bacteria (FeRB) increased in the flooded rhizosphere soil. The abundance of FeRB in the soil correlated with the dissolution of Fe and As. Among the As-transformation genes quantified, the aioA gene for As(III) oxidation and arsM gene for As(III) methylation were most abundant. The arsM copy number correlated positively with the levels of dsrB (dissimilatory (bi) sulfite reductase β-subunit), suggesting that dissimilatory sulfate-reducing bacteria (SRB) may play an important role in dimethylarsenate (DMAs(V)) production in soil. Our results show that decreased populations of rhizosphere FeRB and SRB contributed to a lower bioavailability of As, and decreased production of methylated arsenicals under oxic conditions.
Afficher plus [+] Moins [-]Sulfur(IV) assisted oxidative removal of organic pollutants from source water
2022
Truzsi, Alexandra | Elek, János | Fábián, István
The removal of organic pollutants presents a major challenge for drinking water treatment plants. The chemical oxygen demand (COD) is essentially the measure of oxidizable organic matter in source waters. In this study, we report that COD can efficiently be decreased by adding Fe(II)/Fe(III) and sulfite ion to the source water while purging it with air. In this process, oxygen is activated to oxidize the main constituents of COD, i.e. organic substrates, via the generation of reactive inorganic oxysulfur radical ions. In the end, the total amount of sulfur(IV) is converted to the non-toxic sulfate ion. It has been explored how the COD removal efficiency depends on the concentration of S(IV), the total concentration of iron species, the concentration ratio of Fe(II) and Fe(III), the purging rate and the contact time by using source water from a specific location (Királyhegyes, Hungary). The process has been optimized by applying the Response Surface Methodology (RSM). Under optimum conditions, the predicted and experimentally found COD removal efficiencies are in excellent agreement: 85.4% and 87.5%, respectively. The robustness of the process was tested by varying the optimum values of the parameters by ± 20%. It was demonstrated that the method is universally applicable because a remarkable decrease was achieved in COD, 62.0–88.5%, with source waters of various compositions acquired from 9 wells at other locations using the same conditions as in the case of Királyhegyes.
Afficher plus [+] Moins [-]Impact of wildfires on SO2 detoxification mechanisms in leaves of oak and beech trees
2021
Weber, Jan-Niklas | Kaufholdt, David | Minner-Meinen, Rieke | Bloem, Elke | Shahid, Afsheen | Rennenberg, H. (Heinz) | Hänsch, Robert
Frequency and intensity of wildfire occurrences are dramatically increasing worldwide due to global climate change, having a devastating effect on the entire ecosystem including plants. Moreover, distribution of fire-smoke can influence the natural environment over very long distances, i.e. hundreds of kilometres. Dry plant matter contains 0.1–0.9% (w/w) sulphur, which is mainly released during combustion into the atmosphere as sulphur dioxide (SO₂) resulting in local concentrations of up to 3000 nL L⁻¹. SO₂ is a highly hazardous gas, which enters plants mostly via the stomata. Toxic sulphite is formed inside the leaves due to conversion of SO₂. Plants as sessile organisms cannot escape from threats, why they evolved an impressive diversity of molecular defence mechanisms. In the present study, two recent wildfires in Germany were evaluated to analyse the effect of SO₂ released into the atmosphere on deciduous trees: the Meppen peat fire in 2018 and the forest fire close to Luebtheen in 2019. Collected leaf material from beech (Fagus sylvatica) and oak (Quercus robur) was examined with respect to detoxification of sulphur surplus due to the exposure to elevated SO₂. An induced stress reaction in both species was indicated by a 1.5-fold increase in oxidized glutathione. In beech leaves, the enzymatic activities of the sulphite detoxification enzymes sulphite oxidase and apoplastic peroxidases were increased 5-fold and a trend of sulphate accumulation was observed. In contrast, oaks did not regulate these enzymes during smoke exposure, however, the constitutive activity is 10-fold and 3-fold higher than in beech. These results show for the first time sulphite detoxification strategies of trees in situ after natural smoke exposure. Beech and oak trees survived short-term SO₂ fumigation due to exclusion of toxic gases and different oxidative detoxification strategies. Beeches use efficient upregulation of oxidative sulphite detoxification enzymes, while oaks hold a constitutively high enzyme-pool available.
Afficher plus [+] Moins [-]Bacterial shifts during in-situ mineralization bio-treatment to non-ferrous metal(loid) tailings
2019
Liu, Jian-li | Yao, Jun | Duran, Robert | Mihucz, Victor G. | Hudson-Edwards, K. A. (Karen A.)
Nonferrous mine tailings have caused serious problems of co-contamination with metal(loid)s. It is still a global challenge to cost-effectively manage and mitigate the effect of the mining wastes. We conducted an in-situ bio-treatment of non-ferrous metal(loid) tailings using a microbial consortium of sulfate reducing bacteria (SRB). During the bio-treatment, the transformation of metal(loid)s (such as Cu, Fe, Mn, Pb, Sb, and Zn) into oxidizable and residual fractions in the subsurface tended to be higher than that observed in the surface. As well the mineral compositions changed becoming more complex, indicating that the sulfur reducing process of bio-treatment shaped the bio-transformation of metal(loid)s. The added SRB genera, especially Desulfotomaculum genus, colonized the tailings suggesting the coalescence of SRB consortia with indigenous communities of tailings. Such observation provides new insights for understanding the functional microbial community coalescence applied to bio-treatment. PICRUSt analysis revealed presence of genes involved in sulfate reduction, both assimilatory and dissimilatory. The potential for the utilization of both inorganic and organic sulfur compounds as S source, as well as the presence of sulfite oxidation genes indicated that SRB play an important role in the transformation of metal(loid)s. We advocate that the management of microorganisms involved in S-cycle is of paramount importance for the in situ bio-treatment of tailings, which provide new insights for the implementation of bio-treatments for mitigating the effect of tailings.
Afficher plus [+] Moins [-]A model for performance of sulfite oxidation of ammonia-based flue gas desulfurization system
2015
Jia, Yong | Yin, Liguo | Xu, Yalin | Ding, Xilou | Sheng, Guanghong
A mathematical model was developed to simulate the oxidation of total sulfite in the holding tank of ammonia-based flue gas desulfurization (FGD) system. The model could provide predictions of the oxidation ratio of total sulfite at different operating condition such as pH, concentration of total sulfur, air flow and residence time. The calculation results of an ammonia-based FGD system for 2 × 150 MW boilers by this model were compared to that of corresponding measured values. The comparison results show that the simulated oxidation ratio of total sulfite agrees well with the measured data. The difference between calculated values and measured data is below 4.2%. This model appears to be beneficial for optimizing design and operation of total sulfite oxidation of an ammonia-based FGD system.
Afficher plus [+] Moins [-]Diversity and biogenesis contribution of sulfate-reducing bacteria in arsenic-contaminated soils from realgar deposits
2022
Zhu, Xianbin | Chen, Liyuan | Pan, Hongzhong | Wang, Lei | Zhang, Xun | Wang, Dan
Microbial sulfate reduction, a vital mechanism for microorganisms living in anaerobic, sulfate-rich environments, is an essential aspect of the sulfur biogeochemical cycle. However, there has been no detailed investigation of the diversity and biogenesis contribution of sulfate-reducing bacteria in arsenic-contaminated soils from realgar deposits. To elucidate this issue, soil samples from representative abandoned realgar deposits were collected. Microcosm assays illustrated that all three samples (2–1, 2–2, and 2–3) displayed efficient sulfate and As(V)-respiring activities. Furthermore, a total of 28 novel sequence variants of dissimilatory sulfite reductase genes and 2 new families of dsrAB genes were successfully identified. A novel dissimilatory sulfate-reducing bacterium, Desulfotomaculum sp. JL1, was also isolated from soils, and can efficiently respiratory reduce As(V) and sulfate in 4 and 5 days, respectively. JL1 can promote the generation of yellow precipitates in the presence of multiple electron acceptors (both contain sulfate and As(V) in the cultures), which indicated the biogenesis contribution of sulfate-reducing bacteria to the realgar mine. Moreover, this area had unique microbial communities; the most abundant populations belonged to the phyla Proteobacteria, Chloroflexi, and Acidobacteriota, which were attributed to the unique geochemistry characteristics, such as total organic carbon, total As, NO₃⁻, and SO₄²⁻. The results of this study provide new insight into the diversity and biogenesis contributions of sulfate-reducing bacteria in arsenic-contaminated soils from realgar deposits.
Afficher plus [+] Moins [-]Buffer effect of MgO on Na2SO3 to stabilize S(IV) for the enhancement in simultaneous absorption of NOx and SO2 from non-ferrous smelting gas
2022
Huang, Wenjun | Li, Sichao | Wang, Hongbin | Cui, Peng | Xu, Haomiao | Cheng, Can | Qu, Zan | Yan, Naiqiang
Oxidation–reduction-absorption based on sulfite is a promising process for simultaneous removal of NOₓ and SO₂. However, excessive oxidation of sulfite and competitive absorption between NOₓ and SO₂ limit its application. A matching strategy between antioxidants and alkaline agents has been proposed to solve these problems and enhance the absorption process. The comparison results of inhibitors showed that hydroquinone exhibited long-term high-efficiency inhibition of S(IV) (SO₃²⁻/HSO₃⁻) oxidation. The comparison of alkaline agents showed that the Na₂SO₃ solution with heterogeneous mixture of MgO and hydroquinone exhibited better absorption performance than that with other combinations. The absorption amounts of NOₓ in 0.15 mol/L Na₂SO₃ 50 mL solution added 0.1% hydroquinone (HQ) with 0.09 mol/L MgO were 2.24 mmol, which improved 5 times than that without additives. In addition, studies on the influence of pH showed that the pH of MgO mixture could be stabilized at 9–10 for a long time, while the pH of Na₂CO₃ mixture decreased faster. Further studies suggested that the hydration of MgO resulted in the solution with MgO keeping high pH. This is also the main reason why the combination of MgO and hydroquinone is superior to the combination of Na₂CO₃ and hydroquinone in desulfurization and denitration performance.
Afficher plus [+] Moins [-]Comparative study of energy consumption, kinetic, and performance between conventional and baffled photocatalytic reactor (BPCR) to ofloxacin photo-degradation
2022
Karimi, Pouria | Sadani, Mohsen | Azarpira, Hossein | Rasolevandi, Tayebeh | Sarafraz, Mansour
Regarding the cost-effective photo-degradation of ofloxacin (OFL), present study investigates UV/sulfite /ZnO (USZ) in reactor conventional (without baffles) and baffled photocatalytic reactor (BPCR). The optimal condition was 0.77:2:50 sulfite/ZnO/OFL molar ratio, pH 7, and 30 min reaction time for 100% degradation of 200 mg L⁻¹ concentration of OFL. As information obtained, the UZI process reduces the BOD and COD level about 66% to 86.29% within 80 min reaction, respectively. Also, BOD/COD ratio initial from 0.26 reaches 0.6 after 30 min of reaction time. Kinetic investigation increasing OFL concentration, kₒbₛ and rₒbₛ increase, and, secondly, in the conventional and BPCR reactor, kₒbₛ increase is about 17% and 50% with increasing OFL concentration from 50 to 200 mgL⁻¹. Also, figure-of-merit EEₒ varies from 12.66 to 17.41 and 7.26 to 10.15 kWhm³ for conventional reactor and 8.66–13.61 to 5.24–8.12 kWhm³, respectively. Also, kinetic model EEₒ declines from 15.23 to 8.61 and from 13.31 to 5.37 kWh m⁻³ in conventional and BPCR, respectively. Total cost of the system (TCS) decreases from 7.31 to 2.16 $ in conventional reactor and 4.57 to 0.55 $ in PCBR reactor. Total cost of the system (TCS) was investigated at different concentrations.
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