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Geochemical factors controlling the occurrence of high-fluoride groundwater in the western region of the Ordos basin, northwestern China
2019
Su, He | Wang, Jiading | Liu, Jingtao
Hydrogeochemistry and isotope hydrology were carried out to investigate the spatial distribution of fluoride (F−) and the mechanisms responsible for its enrichment in the western region of the Ordos basin, northwestern China. Sixty-two groundwater samples from the unconfined aquifer and fifty-six from confined aquifer were collected during the pre-monsoon (June 2016). Over 77% of groundwater samples from the unconfined aquifer (F− concentration up to 13.30 mg/L) and approximately 66% from confined aquifer (with a maximum F− concentration of 3.90 mg/L) exhibit F− concentrations higher than the Chinese safe drinking limit (1.0 mg/L). High-F− groundwater presents a distinctive hydrochemical characteristic: a high pH value and HCO3− concentration with Ca-poor and Na-rich. Mineral dissolution (e.g., feldspar, calcite, dolomite, fluorite), cation exchange and evaporation in the aquifers predominate the formation of groundwater chemistry, which are also important for F− enrichment in groundwater. Mixing with unconfined groundwater is a significant mechanism resulting in the occurrence of high-F− groundwater in confined aquifer. These findings indicate that physicochemical processes play crucial roles in driving F− enrichment and that may be useful for studying F− occurrence in groundwater in arid and semi-arid areas.
Show more [+] Less [-]Direct Z-Scheme charge transfer in heterostructured MoO3/g-C3N4 photocatalysts and the generation of active radicals in photocatalytic dye degradations
2019
Xue, Shengyang | Wu, Chunzheng | Pu, Shengyan | Hou, Yaqi | Tong, Tian | Yang, Guang | Qin, Zhaojun | Wang, Zhiming | Bao, Jiming
Photocatalytic degradation is an attractive strategy to purify waste water contaminated by macromolecular organics. Compared with the single-component photocatalysts, heterostructures of different semiconductors have been widely used to improve the photocatalytic performance. In this work, we fabricate a hetero-structured photocatalyst consisting of two-dimensional graphitic carbon nitride (g-C3N4) nanosheets and commercial MoO3 microparticles through a simple mixing and annealing process. The photocatalytic performance was evaluated in various dye degradation reactions, especially Rhodamine (RhB) degradation. The MoO3/g-C3N4 composite shown a significant improvement compared with individual MoO3 or g-C3N4 as well as their physical mixture. By applying electron spin resonance (ESR) spin-trap spectra, radical scavenge experiments and electrochemical analysis, we find that a direct Z-scheme charge transfer between MoO3 and g-C3N4 not only causes an accumulation of electrons in g-C3N4 and holes in MoO3, but also boosts the formation of superoxide radical and hydroxyl radical. The superoxide radical and hole dominate the photocatalytic degradation, while the hydroxyl radical plays a negligible role and its production can be suppressed by lowering the pH value.
Show more [+] Less [-]Are there pharmaceutical compounds in sediments or in water? Determination of the distribution coefficient of benzodiazepine drugs in aquatic environment
2019
Nunes, Chalder Nogueira | dos Anjos, Vanessa Egéa | Quináia, Sueli Pércio
Alprazolam, clonazepam and diazepam are drugs belonging to the benzodiazepine class. These drugs might be important environmental contaminants in aquatic media. A total understanding of behavior and fate of drugs in aquatic environment is not available for these and other drugs. Thus, in this work, a complete optimization of sample treatment and extraction of analytes from sediments and water was described, as well a study of sediment/water distribution comparing it with sample characteristics. Ultrasound for 10 min and 3 steps using 3 mL of extraction solvent were chosen as the stirring form for extraction. A methanol/water (1:1) solution pH 12 was the best extraction solvent. Aiming to eliminate interferences, an addition of 10 μL of NaCl 3.06 mol L⁻¹ was necessary after each step of extraction. Sediment and water samples were characterized, presenting different values on physical-chemical parameters. Six distinct sample sets of water and sediments were spiked with each benzodiazepine and analyzed. Kd values varied from 1.4 to 9.2 L kg⁻¹ for clonazepam, 1.8–11.5 L kg⁻¹ for alprazolam and 2.31–12 L kg⁻¹ for diazepam. A principal component analysis showed high dependence on Kd with sample characteristics mainly related to sediments. In the systems, whose sediments presented high levels of clay, silt and organic matter, the drugs presented a great interaction with the solid part of the system, increasing the Kd value. Koc values varied from 149.25 to 634.13 L kg⁻¹ for clonazepam, 186.57–852.48 L kg⁻¹ for alprazolam, and 194.68–1189.81 L kg⁻¹ for diazepam.
Show more [+] Less [-]Perchlorate behavior in the context of black carbon and metal cogeneration following fireworks emission at Oak Lake, Lincoln, Nebraska, USA
2019
Manish Kumar, | Snow, Daniel D. | Li, Yusong | Shea, Patrick J.
The imprints of fireworks displays on the adjacent water body were investigated from the perspective of cogeneration of black carbon, metals and perchlorate (ClO₄⁻). In particular, the mixing and dissipation of ClO₄⁻ were studied at Oak Lake, Lincoln, Nebraska, following fireworks displays in 2015 and 2016. Following the display, ClO₄⁻ concentration in the water increased up to 4.3 μg/L and 4.0 μg/L in 2015 and 2016, respectively. A first-order model generally provided a good fit to the measured perchlorate concentrations from which the rate of dissipation was estimated as 0.07 d⁻¹ in 2015 and 0.43 d⁻¹ in 2016. SEM images show imprints of soot and metal particles in aerosol samples. EDS analysis of the lake sediment confirmed the presence of Si, K, Ca, Zn and Ba, most of which are components of fireworks. The δ¹³C range of −7.55‰ to −9.19‰ in the lake water system closely resembles fire-generated carbon. Cogeneration of black carbon and metal with perchlorate was established, indicating that ClO₄⁻ is an excellent marker of fireworks or a burning event over all other analyzed parameters. Future microcosmic, aggregation and column-based transport studies on black carbon in the presence of perchlorate and metals under different environmental conditions will help in developing transport and fate models for perchlorate and black carbon particles.
Show more [+] Less [-]Large eddy simulation of reactive pollutants in a deep urban street canyon: Coupling dynamics with O3-NOx-VOC chemistry
2017
Zhong, Jian | Cai, Xiao-Ming | Bloss, William James
A large eddy simulation (LES) model coupled with O3-NOx-VOC chemistry is implemented to simulate the coupled effects of emissions, mixing and chemical pre-processing within an idealised deep (aspect ratio = 2) urban street canyon under a weak wind condition. Reactive pollutants exhibit significant spatial variations in the presence of two vertically aligned unsteady vortices formed in the canyon. Comparison of the LES results from two chemical schemes (simple NOx-O3 chemistry and a more comprehensive Reduced Chemical Scheme (RCS) chemical mechanism) shows that the concentrations of NO2 and Ox inside the street canyon are enhanced by approximately 30–40% via OH/HO2 chemistry. NO, NOx, O3, OH and HO2 are chemically consumed, while NO2 and Ox (total oxidant) are chemically produced within the canyon environment. Within-canyon pre-processing increases oxidant fluxes from the canyon to the overlying boundary layer, and this effect is greater for deeper street canyons (as found in many traditional European urban centres) than shallower (lower aspect ratio) streets. There is clear evidence of distinct behaviours for emitted chemical species and entrained chemical species, and positive (or negative) values of intensities of segregations are found between pairs of species with similar (or opposite) behaviour. The simplified two-box model underestimated NO and O3 levels, but overestimated NO2 levels for both the lower and upper canyon compared with the more realistic LES-chemistry model. This suggests that the segregation effect due to incomplete mixing reduces the chemical conversion rate of NO to NO2. This study reveals the impacts of nonlinear O3-NOx-VOC photochemical processes in the incomplete mixing environment and provides a better understanding of the pre-processing of emissions within canyons, prior to their release to the urban boundary layer, through the coupling of street canyon dynamics and chemistry.
Show more [+] Less [-]Seasonal variation in the nature of DOM in a river and drinking water reservoir of a closed catchment
2017
Awad, John | Leeuwen, John van | Chow, Christopher W.K. | Smernik, Ronald J. | Anderson, Sharolyn J. | Cox, Jim W.
Dissolved organic matter (DOM) in surface waters used for drinking purposes can vary markedly in character depending on its source within catchments and the timing and intensity of rainfall events. Here we report the findings of a study on the character and concentration of DOM in waters collected during different seasons from Myponga River and Reservoir, South Australia. The character of DOM was assessed in terms of its treatability by enhanced coagulation and potential for disinfection by-product i.e. trihalomethane (THM) formation. During the wet seasons (winter and spring), water samples from the river had higher DOC concentrations (X¯: 21 mg/L) and DOM of higher average molecular weight (AMW: 1526 Da) than waters collected during the dry seasons (summer and autumn: DOC: 13 mg/L; AMW: 1385 Da). Even though these features led to an increase in the percentage removal of organics by coagulation with alum (64% for wet compared with 53% for dry season samples) and a lower alum dose rate (10 versus 15 mg alum/mg DOC removal), there was a higher THM formation potential (THMFP) from wet season waters (treated waters: 217 μg/L vs 172 μg/L). For reservoir waters, samples collected during the wet seasons had an average DOC concentration (X¯: 15 mg/L), percentage removal of organics by alum (54%), alum dose rates (13 mg/mg DOC) and THMFP (treated waters: 207 μg/L) that were similar to samples collected during the dry seasons (mean DOC: 15 mg/L; removal of organics: 52%; alum dose rate: 13 mg/mg DOC; THMFP: 212 μg/L for treated waters). These results show that DOM present in river waters and treatability by alum are highly impacted by seasonal environmental variations. However these in reservoir waters exhibit less seasonal variability. Storage of large volumes of water in the reservoir enables mixing of influent waters and stabilization of water quality.
Show more [+] Less [-]Coupling dynamics and chemistry in the air pollution modelling of street canyons: A review
2016
Zhong, Jian | Cai, Xiao-Ming | Bloss, William James
Air pollutants emitted from vehicles in street canyons may be reactive, undergoing mixing and chemical processing before escaping into the overlying atmosphere. The deterioration of air quality in street canyons occurs due to combined effects of proximate emission sources, dynamical processes (reduced dispersion) and chemical processes (evolution of reactive primary and formation of secondary pollutants). The coupling between dynamics and chemistry plays a major role in determining street canyon air quality, and numerical model approaches to represent this coupling are reviewed in this article. Dynamical processes can be represented by Computational Fluid Dynamics (CFD) techniques. The choice of CFD approach (mainly the Reynolds-Averaged Navier-Stokes (RANS) and Large-Eddy Simulation (LES) models) depends on the computational cost, the accuracy required and hence the application. Simplified parameterisations of the overall integrated effect of dynamics in street canyons provide capability to handle relatively complex chemistry in practical applications. Chemical processes are represented by a chemical mechanism, which describes mathematically the chemical removal and formation of primary and secondary species. Coupling between these aspects needs to accommodate transport, dispersion and chemical reactions for reactive pollutants, especially fast chemical reactions with time scales comparable to or shorter than those of typical turbulent eddies inside the street canyon. Different approaches to dynamical and chemical coupling have varying strengths, costs and levels of accuracy, which must be considered in their use for provision of reference information concerning urban canopy air pollution to stakeholders considering traffic and urban planning policies.
Show more [+] Less [-]Identification of the hydrogeochemical processes and assessment of groundwater quality using classic integrated geochemical methods in the Southeastern part of Ordos basin, China
2016
Yang, Qingchun | Li, Zijun | Ma, Hongyun | Wang, Luchen | Martín, Jordi Delgado
Insufficient understanding of the hydrogeochemistry of aquifers makes it necessary to conduct a preliminary water quality assessment in the southern region of Ordos Basin, an arid area in the world. In this paper, the major ions of groundwater have been studied aiming at evaluating the hydrogeochemical processes that probably affect the groundwater quality using 150 samples collected in 2015. The two prevalent hydrochemical facies, HCO3Mg·Na·Ca and HCO3Mg·Ca·Na type water, have been identified based on the hydrochemical analysis from Piper trilinear diagram. Compositional relations have been used to assess the origin of solutes and confirm the predominant hydrogeochemical processes responsible for the various ions in the groundwater. The results show that the ions are derived from leaching effect, evaporation and condensation, cation exchange, mixing effect and human activities. Finally groundwater quality was assessed with single factor and set pair methods, the results indicate that groundwater quality in the study region is generally poor in terms of standard of national groundwater quality. The results obtained in this study will be useful to understand the groundwater quality status for effective management and utilization of the groundwater resource.
Show more [+] Less [-]Light absorption enhancement of black carbon from urban haze in Northern China winter
2016
Chen, Bing | Bai, Zhe | Cui, Xinjuan | Chen, Jianmin | Andersson, August | Gustafsson, Örjan
Atmospheric black carbon (BC) is an important pollutant for both air quality and Earth's energy balance. Estimates of BC climate forcing remain highly uncertain, e.g., due to the mixing with non-absorbing components. Non-absorbing aerosols create a coating on BC and may thereby act as a lens which may enhance the light absorption. However, this absorption enhancement is poorly constrained. To this end a two-step solvent dissolution protocol was employed to remove both organic and inorganic coatings, and then investigate their effects on BC light absorption. Samples were collected at a severely polluted urban area, Jinan, in the North China Plain (NCP) during February 2014. The BC mass absorption cross-section (MAC) was measured for the aerosol samples before and after the solvent-decoating treatment, and the enhancement of MAC (EMAC) from the coating effect was defined as the ratio. A distinct diurnal pattern for the enhancement was observed, with EMAC 1.3 ± 0.3 (1 S.D.) in the morning, increasing to 2.2 ± 1.0 in the afternoon, after that dropping to 1.5 ± 0.8 in the evening-night. The BC absorption enhancement primarily was associated with urban-scale photochemical production of nitrate and sulfate aerosols. In addition to that, regional-scale haze plume with increasing sulfate levels strengthened the absorption enhancement. These observations offer direct evidence for an increased absorption enhancement of BC due to severe air pollution in China.
Show more [+] Less [-]Environmental controls on ozone fluxes in a poplar plantation in Western Europe
2014
Zona, D. | Gioli, B. | Fares, S. | De Groote, T. | Pilegaard, K. | Ibrom, A. | Ceulemans, R.
Tropospheric O3 is a strong oxidant that may affect vegetation and human health. Here we report on the O3 fluxes from a poplar plantation in Belgium during one year. Surprisingly, the winter and autumn O3 fluxes were of similar magnitude to ones observed during most of the peak vegetation development. Largest O3 uptakes were recorded at the beginning of the growing season in correspondence to a minimum stomatal uptake. Wind speed was the most important control and explained 44% of the variability in the nighttime O3 fluxes, suggesting that turbulent mixing and the mechanical destruction of O3 played a substantial role in the O3 fluxes. The stomatal O3 uptake accounted for a seasonal average of 59% of the total O3 uptake. Multiple regression and partial correlation analyses showed that net ecosystem exchange was not affected by the stomatal O3 uptake.
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