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Synergistic effects of ozone/peroxymonosulfate for isothiazolinone biocides degradation: Kinetics, synergistic performance and influencing factors النص الكامل
2022
Yang, Zheng-Wei | Wang, Wen-Long | Lee, Min-Yong | Wu, Qian-Yuan | Guan, Yun-Tao
Synergistic effects of ozone (O₃) and peroxymonosulfate (PMS, HSO₅⁻) for isothiazolinone biocides degradation was studied. The synergistic ozonation process (O₃/PMS) increased the efficiency of methyl-isothiazolinone (MIT) and chloro-methyl-isothiazolinone (CMIT) degradation to 91.0% and 81.8%, respectively, within 90 s at pH 7.0. This is 30.6% and 62.5% higher than the corresponding ozonation efficiency, respectively. Total radical formation value (Rcₜ,R) for the O₃/PMS process was 24.6 times that of ozonation alone. Calculated second-order rate constants for the reactions between isothiazolinone biocides and ▪ (kSO₄₋,MIT and kSO₄₋,CMIT) were 8.15 × 10⁹ and 4.49 × 10⁹ M⁻¹ s⁻¹, respectively. Relative contributions of O₃, hydroxyl radical (OH) and ▪ oxidation to MIT and CMIT removal were estimated, which were 15%, 45%, and 40% for O₃, OH and ▪ oxidation to MIT, and 1%, 67%, and 32% for O₃, OH and ▪ oxidation to CMIT at pH 7.0, respectively. Factors influencing the O₃/PMS process, namely the solution pH, chloride ions (Cl⁻), and bicarbonate (HCO₃⁻), were evaluated. Increasing the solution pH markedly accelerated O₃ decay and OH and ▪ formation, thus weakening the relative contribution of O₃ oxidation while enhancing that of OH and ▪. Cl⁻ had a negligible effect on MIT and CMIT degradation. Under the dual effect of bicarbonate (HCO₃⁻) as inhibitor and promoter, low concentrations (1–2 mM) of bicarbonate weakly promoted MIT and CMIT degradation, while high concentrations (10–20 mM) induced strong inhibition. Lastly, oxidation performance of O₃ and O₃/PMS processes for MIT and CMIT degradation in different water matrices was compared.
اظهر المزيد [+] اقل [-]Identification of hydrochemical genesis and screening of typical groundwater pollutants impacting human health: A case study in Northeast China النص الكامل
2019
Zhai, Yuanzheng | Zheng, Fuxin | Zhao, Xiaobing | Xia, Xuelian | Teng, Yanguo
Concentrations of common pollutants in groundwater continue to increase, and emerging pollutants are also increasingly found worldwide, thereby increasingly impacting human activities. In this new situation, it is necessary, albeit more difficult, to once again recognize the hydrochemical genesis of groundwater and to subsequently screen the typical pollutants. Taking the groundwater of the Songnen Plain of Northeast China as an example, the hydrochemical genesis was identified using space interpolation, characteristic element ratio and factor analysis methods based on 368 groundwater samples. Subsequently, the typical pollutants with potential impacts on the health of the local residents were screened by the index system method newly established. All the measured hydrochemical compositions show an obvious spatial variation, with a uniform hydrochemical type of HCO3–Ca in the whole area. Both the major compositions (K, Na, Ca, Mg, HCO3, Cl and SO4) and trace compositions (Fe, Mn, Cu, Zn, Pb, As, F, I and Se) are mainly protogenetic in an environment impacted by the lixiviation of groundwater in the migration process in the strata, although these compositions have been impacted by human activities to varying degrees. The mass concentration of NO3–N has exceeded most of the major compositions except for HCO3 and Ca, which means the nitrogen pollution problem is already very serious; and this problem is mainly caused by the utilization of fertilizers and the discharge of industrial wastewater and domestic sewage. Human activities have obviously disrupted the natural dynamic balance of these chemicals between the environment and the groundwater, thereby intensifying the release of F, Fe and Mn from the environment. TDS, total hardness, tri-nitrogen, F, Fe, Mn, Pb and As in some parts are found to exceed the standards of groundwater quality to varying degrees. As, Pb, Fe, NO3–N, NO2–N, Mn, F and NH4–N are finally screened as the typical pollutants.
اظهر المزيد [+] اقل [-]Contamination of groundwater with per- and polyfluoroalkyl substances (PFAS) from legacy landfills in an urban re-development precinct النص الكامل
2019
Hepburn, Emily | Madden, Casey | Szabo, Drew | Coggan, Timothy L. | Clarke, Bradley | Currell, Matthew
The extent of per- and polyfluoroalkyl substances (PFAS) in groundwater surrounding legacy landfills is currently poorly constrained. Seventeen PFAS were analysed in groundwater surrounding legacy landfills in a major Australian urban re-development precinct. Sampling locations (n = 13) included sites installed directly in waste material and down-gradient from landfills, some of which exhibited evidence of leachate contamination including elevated concentrations of ammonia-N (≤106 mg/L), bicarbonate (≤1,740 mg/L) and dissolved methane (≤10.4 mg/L). Between one and fourteen PFAS were detected at all sites and PFOS, PFHxS, PFOA and PFBS were detected in all samples. The sum of detected PFAS (∑₁₄PFAS) varied from 26 ng/L at an ambient background site to 5,200 ng/L near a potential industrial point-source. PFHxS had the highest median concentration (34 ng/L; range: 2.6–280 ng/L) followed by PFOS (26 ng/L; range: 1.3–4,800 ng/L), PFHxA (19 ng/L; range: <LOQ – 46 ng/L) and PFOA (12 ng/L; range: 1.7–74 ng/L). Positive correlations between ∑₁₄PFAS, PFOA and other perfluoroalkyl carboxylic acids (PFCAs) (e.g. PFHxA) with typical leachate indicators including ammonia-N and bicarbonate were observed. In contrast, no such correlations were found with perfluoroalkyl sulfonic acids (PFSAs) (e.g., PFOS and PFHxS). In addition, a strong positive linear correlation (R² = 0.69) was found between the proportion of PFOA in the sum of detected perfluorinated alkylated acids (PFOA/∑PFAA) and ammonia-N concentrations in groundwater. This is consistent with previous research showing relatively high PFOA/∑PFAA in municipal landfill leachates, and more conservative behaviour (e.g. less sorption and reactivity) of PFCAs during subsurface transport compared to PFSAs. PFOA/∑PFAA in groundwater may therefore be a useful indicator of municipal landfill-derived PFAA. One site with significantly elevated PFOS and PFHxS concentrations (4,800 and 280 ng/L, respectively) appears to be affected by point-source industrial contamination, as landfill leachate indicators were absent.
اظهر المزيد [+] اقل [-]Mechanism of matrix-bound phosphine production in response to atmospheric elevated CO2 in paddy soils النص الكامل
2018
An, Shaorong | Niu, Xiaojun | Chen, Weiyi | Sheng, Hong | Lai, Senchao | Yang, Zhiquan | Gu, Xiaohong | Zhou, Shaoqi
To explore the effect of elevated CO₂ concentrations ([CO₂]) on phosphine formation in paddy fields, the matrix-bound phosphine (MBP) content, different phosphorus fractions and various carbon forms in soil samples from rice cultivation under varying CO₂ concentrations of 400 ppm, 550 ppm and 700 ppm by indoor simulation experiment were determined. This study showed that MBP concentration did not increase significantly with elevated [CO₂] over four-week cultivation periods of rice seedlings, regardless of soil layers. MBP had a significant positive correlation with total phosphorus (TP) and inorganic phosphorus (IP), and multiple stepwise linear regression analysis further indicated that MBP preservation in neutral paddy soils with depths of 0–20 cm may have been due to conversion from FeP and CaP. Based on redundancy analysis and forward selection analysis, speculated that the formation of MBP in the neutral paddy soils as the response to atmospheric elevated [CO₂] was due to two processes: (i) FeP transformation affected by the changes of soil respiration (SCO₂) and TOC was the main precursor for the production of MBP; and (ii) CaP transformation resulting from variation in HCO₃⁻ was the secondary MBP source. The complex combination of these two processes is simultaneously controlled by SCO₂. In a word, the soil environment in the condition of elevated [CO₂] was in favor of MBP storage in neutral paddy soils. The results of our study imply that atmospheric CO₂ participates in and has a certain impact on the global biogeochemical cycle of phosphorus.
اظهر المزيد [+] اقل [-]Effect of pH, temperature, humic acid and coexisting anions on reduction of Cr(Ⅵ) in the soil leachate by nZVI/Ni bimetal material النص الكامل
2017
Zhu, Fang | Li, Luwei | Ren, Wentao | Deng, Xiaoqiang | Liu, Tao
Nano zero valent iron/Ni bimetal materials (nZVI/Ni) were prepared by borohydride reduction method to remediate toxic Cr(Ⅵ) contaminated in soil leachate. nZVI/Ni was characterized using scanning electron microscopy (SEM), X-ray diffraction (XRD) and X-ray Photoelectron Spectroscopy (XPS). Different factors including pH value of soil leachate, reaction time, temperature, humic acid and coexisting anions (SO42-, NO3−, HCO3−, CO32-) were studied to analyze the reduction rate. Results showed that the reduction rate of Cr(Ⅵ) could reach 99.84% under the condition of pH of 5 and temperature of 303 K. pH values and temperature of soil leachate had a significant effect on the reduction efficiency, while humic acid had inhibition effect for the reduction reaction. SO42-, HCO3− and CO32- had inhibition effect for reduction rate, while NO3− barely influenced the reduction process of nZVI/Ni. Moreover, Langumir-Hinshelwood first order kinetic model was studied and could describe the reduction process well. The thermodynamic studies indicated that the reaction process was endothermic and spontaneous. Activation energy was 143.80 kJ mol−1, showing that the reaction occurred easily. Therefore, the study provides an idea for nZVI/Ni further research and practical application of nZVI/Ni in soil remediation.
اظهر المزيد [+] اقل [-]A field-based method to derive macroinvertebrate benchmark for specific conductivity adapted for small data sets and demonstrated in the Hun-Tai River Basin, Northeast China النص الكامل
2016
Zhao, Qian | Jia, Xiaobo | Xia, Rui | Lin, Jianing | Zhang, Yuan
Ionic mixtures, measured as specific conductivity, have been increasingly concerned because of their toxicities to aquatic organisms. However, identifying protective values of specific conductivity for aquatic organisms is challenging given that laboratory test systems cannot examine more salt-intolerant species nor effects occurring in streams. Large data sets used for deriving field-based benchmarks are rarely available. In this study, a field-based method for small data sets was used to derive specific conductivity benchmark, which is expected to prevent the extirpation of 95% of local taxa from circum-neutral to alkaline waters dominated by a mixture of SO42− and HCO3− anions and other dissolved ions. To compensate for the smaller sample size, species level analyses were combined with genus level analyses. The benchmark is based on extirpation concentration (XC95) values of specific conductivity for 60 macroinvertebrate genera estimated from 296 sampling sites in the Hun-Tai River Basin. We derived the specific conductivity benchmark by using a 2-point interpolation method, which yielded the benchmark of 249 μS/cm. Our study tailored the method that was developed by USEPA to derive aquatic life benchmark for specific conductivity for basin scale application, and may provide useful information for water pollution control and management.
اظهر المزيد [+] اقل [-]Activation of sulfite autoxidation with CuFe2O4 prepared by MOF-templated method for abatement of organic contaminants النص الكامل
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.
اظهر المزيد [+] اقل [-]Human health risk assessment of some bottled waters from Romania النص الكامل
2020
Dippong, Thomas | Hoaghia, Maria-Alexandra | Mihali, Cristina | Cical, Elena | Calugaru, Mihai
The paper presents the quality status of 14 brands of bottled water, with sources of groundwaters from different mountain areas alongside the Carpathian Mountains from Romania. A number of 12 physico-chemical parameters (ammonium, bicarbonate, electrical conductivity, carbonate, chemical oxygen demand, chloride, nitrate, nitrite, pH, sulphate, total hardness, turbidity), 9 metals and metalloids (Li, B, Na, Mg, Al, K, Ca, Sr, Ba) and 17 heavy metals (V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Mo, Ag, Cd, In, Tl, Pb, Bi) were determined and studied. The quality status, the potential contamination and the health risk assessment of bottled waters were assessed, by using the drinking water quality index, the heavy metal pollution index, the heavy metal evaluation index, the degree of contamination and the human health risk indices. Hierarchical cluster analysis was applied, indicating similarities among the studied bottled waters based on their metal content. The Piper diagram reveals that the majority of bottled water samples fall into the Ca, Mg, Na, K, Cl⁻, SO₄²⁻, CO₃²⁻, HCO₃⁻ categories. The quality of bottled waters based on the indices results indicated marginal, poor and very-poor quality status of the studied water samples, while the health risk assessment indices presented potential risks at aluminium, chloride and nitrate for the inhabitants who used those water samples with the purpose of drinking. The pollution indices with respect to metals generally reflected a low pollution status. This study represents the first attempt in assessing the overall quality of some bottled water collected from the mountain area, Romania, likewise assessing the comprehensive human health risk due to several chemical elements determined in water in amounts around and exceeding the maximum allowable concentrations. This research can be useful for development of potential strategies for risk control and management in the field of drinking water.
اظهر المزيد [+] اقل [-]Hydrogeochemical controls on arsenic mobility in an arid inland basin, Southeast of Iran: The role of alkaline conditions and salt water intrusion النص الكامل
2019
Dehbandi, Reza | Abbasnejad, Ahmad | Karimi, Zohreh | Herath, Indika | Bundschuh, Jochen
Elevated inorganic arsenic concentrations in groundwater has become a major public and environmental health concern in different parts of the world. Currently, As-contaminated groundwater issue in many countries and regions is a major topic for publications at global level. However, there are many regions worldwide where the problem has still not been resolved or fully understood due to inadequate hydrogeochemical investigations. Hence, this study evaluates for the first time the hydrogeochemical behavior of the arid and previously unexplored inland basin of Sirjan Plain, south east (SE) Iran, in order to assess the controlling factors which influence arsenic (As) mobility and its distribution through groundwater resources. Total inorganic arsenic concentration was measured using inductive-coupled plasma optical emission spectrometry (ICP-OES). Arsenic content in groundwater of this region ranged between 2.4 and 545.8 μg/L (mean value: 86.6 μg/L) and 50% of the samples exceeded the World Health Organization (WHO) guideline value of 10 μg/L in drinking water. Groundwater was mainly of Na-Cl type and alkaline due to silicate weathering, ion exchange and evaporation in arid conditions. Elevated As concentrations were generally observed under weakly alkaline to alkaline conditions (pH > 7.4). Multivariate statistical analysis including cluster analysis and bi-plot grouped As with pH and HCO3 and demonstrated that the secondary minerals including oxyhydroxides of Fe are the main source of As in groundwater in this region. The desorption of As from these mineral phases occurs under alkaline conditions in oxidizing arid environments thereby leading to high levels of As in groundwater. Moreover, evaporation, ion exchange and saltwater intrusion were the secondary processes accelerating As release and its mobility in groundwater. Based on the results of this study, desorption of As from metal oxy-hydroxides surfaces under alkaline conditions, evaporation and intrusion of As-rich saline water are considered to be the major factors causing As enrichment in arid inland basins such as those in southeast Iran. This study proposes the regular monitoring and proper groundwater management practices to mitigate high levels of arsenic in groundwater and related drinking water wells of Sirjan Plain.
اظهر المزيد [+] اقل [-]Micromorphology and environmental behavior of oxide deposit layers in sulfide-rich tailings in Tongling, Anhui Province, China النص الكامل
2019
Zheng, Liugen | Qiu, Zheng | Tang, Quan | Li, Yang
Sulfide-rich tailings produced by mineral processing are prone to oxidation and cause many pollution problems in the surrounding environment; therefore, this issue has become a focus of attention. The Tongling Shuimuchong tailings reservoir contains a large amount of sulfide minerals, especially pyrrhotite and pyrite. This reservoir features obvious oxidation in the surface layer, and the slab is very hard. Mineralogical and environmental geochemical analyses were performed on tailings with different degrees of oxidation in the Shuimuchong tailings reservoir to investigate the influence of the formation of the hard oxidized layer on environmental pollution in the tailings pond. The samples were first subjected to particle-size analysis. The shallow tailings were mainly composed of medium particle; the proportions of coarse particle and fine tailings particles were equal; and the proportions of clay and silt were less than those of the other size fractions. Mineralogical analysis showed that pyrrhotite and pyrite were replaced by residual structures in the oxide layer. The secondary minerals goethite, hematite and jarosite were attached to the edges and fractures of sulfide minerals. The samples were geochemically analyzed to determine the total concentrations of 5 elements, the pH and the major anions. The maximum SO₄²⁻ concentrations of 33,970 and 32,749 mg/kg were observed at a depth of 40 cm in profiles 1 and 2, respectively. Metal sulfide mineral oxidation in the tailings lowered the pH of the materials to values less than 4. The concentration of HCO₃⁻ (122–635 mg/kg) in the tailings samples was very low, and the concentration of CO₃²⁻ was zero. As (53.2–133.7 mg/kg), Pb (24.2–307.5 mg/kg) and Hg (0.03–0.06 mg/kg) were concentrated in the highly oxidized layer at the surface; the Cd content (0.23–10.5 mg/kg) increased with decreasing oxidation degree of the tailings; and the Cr content (38.0–54.9 mg/kg) fluctuated around a certain value.
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