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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 [-]Improved estimation of air pollutant emissions from landing and takeoff cycles of civil aircraft in China
2019
Zhou, Ying | Jiao, Yufang | Lang, Jianlei | Chen, Dongsheng | Huang, Cheng | Wei, Peng | Li, Shengyue | Cheng, Shuiyuan
Civil aircraft emissions during landing and takeoff (LTO) are important air pollutant sources, but have been given insufficient attention in China. Accurate estimation of these emissions is limited by a lack of important parameters, such as detailed flight information and the dynamic time in climb and approach modes during LTO that are dependent on mixing layer height (MLH). We developed a flight-time/flight-height relationship using real-time height information in Aircraft Meteorological Data Relay data, and then calculated the actual time for each flight in those two modes based on the actual MLH from meteorological observation. Hourly emissions of civil aircraft were then estimated based on the database of each flight. Total emissions of NOx, CO, SO2, HC and PM from LTO cycles of domestic flights in China during 2015 were 37.78 Gg, 30.25 Gg, 12.00 Gg, 2.38 Gg and 0.75 Gg, respectively. Substantial monthly, daily and hourly variations of emissions due to the flight schedule as well as MLH were calculated. Large differences were found between the new estimation and emissions calculated based on traditional method. Compared with the emissions estimated based on default parameter obtained from International Civil Aviation Organization, the average difference of annual emission among airports with new estimation for various pollutants was approximately 30.3% in climb mode and 81.4% in approach mode; compared with the emissions estimated based on the method proposed by China National Guide, the average difference of annual emission among airports were 37.4% (NOx), 8.4% (CO), 73.1% (HC) and 58.1% (PM) during LTO process. The monthly airport-specific emissions per LTO were also proposed. These can provide necessary and meaningful support for the revision of the values in National Guide.
Show more [+] Less [-]Infiltration behavior of heavy metals in runoff through soil amended with biochar as bulking agent
2019
Zhao, Ling | Nan, Hongyan | Kan, Yue | Xu, Xiaoyun | Qiu, Hao | Cao, Xinde
Biochar as a porous carbon material could be used for improving soil physical and chemical properties, while insufficient attention has been paid to potential risks induced by infiltration of heavy metals in the runoff water flowing through biochar-amended soil. Four different soil-biochar matrices with same volumes were constructed including soil alone (M1), biochar alone (M2), soil-biochar layering (M3) and soil-biochar mixing (M4). Leaching experiments were conducted with Pb, Cu, and Zn contaminated runoff water. Results showed that biochar amendment greatly improved the water permeation, and the infiltration rates in M2, M3, and M4 were 2.85–23.0 mm min⁻¹, being much higher than those in M1 (1.33–4.05 mm min⁻¹), though the rates decreased as the leaching volumes increased. However, biochar induced more Pb, Cu, and Zn infiltrated through soil-biochar matrix. After 350-L leaching, M1 retained about 95% Pb, 90% Cu, and 36% Zn, while M2 only retained 4.80% Pb, 17.4% Cu, and 4.01% Zn; about 30% Pb, 80% Cu, and 15% Zn were retained in M3 and M4. Notably, Zn was trapped first and then re-leached into the filtrate, which resulted in a much higher effluent Zn than the influent Zn at the later stage. However, the unit weight of biochar showed a higher capacity for retaining heavy metals compared to per unit of soil. Under the dynamic water flow, all benefits and disadvantages induced by biochar were weakened with its physical disintegration. Biochar as soil amendment can enhance plant growth via ameliorating soil structure, while it would pose risks to environment because of large penetration of heavy metals. If biochar was compacted to form a denser physical structure, perhaps more heavy metals could be retained.
Show more [+] Less [-]Evaluation on the stabilization of Zn/Ni/Cu in spinel forms: Low-cost red mud as an effective precursor
2019
Su, Minhua | Liao, Chang-Zhong | Ma, Shengshou | Zhang, Kuibao | Tang, Jinfeng | Liu, Chengshuai | Shih, Kaimin
Red mud, which is from the aluminum industry, is a potentially under-utilized resource. Technological processes for using low-cost red mud as an alternative precursor for detoxifying metal pollutants urgently need to be developed. In this study, we systematically investigated the feasibility of using red mud to detoxify metal-containing wastes (e.g., fly ash) via the formation of preferable crystalline phases. To understand the mechanism of metal detoxification by red mud, CuO, NiO, and ZnO were blended with red mud at different weight ratios and the mixtures were then subjected to ceramic-sintering. After sintering, the X-ray diffraction results revealed that all of the metals (i.e., Cu, Ni, and Zn) were able to be crystallographically incorporated into spinel lattices. Sintering the red mud at 1100 °C for 3 h effectively converted the metals into spinels. The mixing weight ratios strongly affected the efficiency of the metal incorporation. The red mud was able to incorporate 15 wt% of metal oxides. The incorporation mechanisms mainly occurred between the metal oxide(s) and hematite. Modified TCLP tests were conducted to further evaluate the metal stabilization performance of the red mud, which demonstrated the leachabilities of ZnO and the sintered red mud + ZnO product. The concentration of leached metal was substantially reduced after the incorporation process, thus demonstrating that red mud can be successfully used to detoxify metals. The results of this study reveal that waste red mud can be feasibly reused as a promising waste-to-resource strategy for stabilizing heavy metal wastes.
Show more [+] Less [-]Apportionment of sources of heavy metals to agricultural soils using isotope fingerprints and multivariate statistical analyses
2019
Wang, Pengcong | Li, Zhonggen | Liu, Jinling | Bi, Xiangyang | Ning, Yongqiang | Yang, Shaochen | Yang, Xiaojing
Apportioning sources of environmental pollutants is key to controlling pollution. In this study, the sources of heavy metals to 234 agricultural soils from the Jianghan Plain (JHP) (∼22454 km2) in central China were discriminated between using Cd and Pb isotope compositions and multivariate statistical analyses. Concentrations of some metals in JHP soils (0.48 ± 0.2, 48.2 ± 15.9, 0.12 ± 0.23, 48.8 ± 16.4, 36.5 ± 9.8, and 96.8 ± 42.2 mg kg−1 for Cd, Cu, Hg, Ni, Pb, and Zn, respectively) were higher than background concentrations in Chinese soil. The Cd isotope compositions for the JHP soils (δ114/110Cd values −0.76‰ to −0.25‰) were similar to Cd isotope compositions found for smelter dust and incinerator fly ash, indicating Cd was supplied to the JHP soils by ore smelting and/or refining processes. The Pb isotope compositions for the JHP soils (206Pb/207Pb 1.182–1.195 and 208Pb/206Pb 2.078–2.124) were between the Pb isotope compositions found for Chinese coal and natural sources, which a binary isotope mixing model indicated contributed 52% and 48%, respectively, of the Pb in JHP soils. Cluster analysis and positive matrix factorization indicated that the sources of heavy metals in JHP soils may consist of smelting and/or refining activities, coal combustion, agricultural activities, and natural sources (including Han River sediment and soil parent materials). The isotope fingerprints and multivariate statistical analyses together indicated that coal combustion and smelting and/or refining activities were the main anthropogenic sources of heavy metals polluting JHP soils.
Show more [+] Less [-]Vertical mixing with return irrigation water the cause of arsenic enrichment in groundwater of district Larkana Sindh, Pakistan
2019
Ali, Waqar | Mushtaq, Nisbah | Javed, Tariq | Zhang, Hua | Ali, Kamran | Rasool, Atta | Farooqi, Abida
Stable isotopes ratios (‰) of Hydrogen (δ2H) and Oxygen (δ1⁸O) were used to trace the groundwater recharge mechanism and geochemistry of arsenic (As) contamination in groundwater from four selected sites (Larkana, Naudero, Ghari Khuda Buksh and Dokri) of Larkana district. The stable isotope values of δ2H and δ1⁸O range from 70.78‰ to −56.01‰ and from −10.92‰ to −7.35‰, relative to Vienna Standard for Mean Ocean Water (VSMOW) respectively, in all groundwater samples, thus indicating the recharge source of groundwater from high-salinity older water. The concentrations of As in all groundwater samples were ranged from 2 μg/L to 318 μg/L, with 67% of samples exhibited As levels exceeding than that of World Health Organization (WHO) permissible limit 10 μg/L and 42% of samples expressed the As level exceeding than that of the National Environmental Quality Standard (NEQS) 50 μg/L. The leaching and vertical mixing with return irrigation water are probably the main processes controlling the enrichment of As in groundwater of Larkana, Naudero, Ghari Khuda Buksh and Dokri. The weathering of minerals mostly controlled the overall groundwater chemistry; rock-water interactions and silicate weathering generated yielded solutions that were saturated in calcite and dolomite in two areas while halite dissolution is prominent with high As area.
Show more [+] Less [-]Widespread occurrence and spatial distribution of glyphosate, atrazine, and neonicotinoids pesticides in the St. Lawrence and tributary rivers
2019
Montiel-León, Juan Manuel | Muñoz, Gabriel | Vo Duy, Sung | Do, Dat Tien | Vaudreuil, Marc-Antoine | Goeury, Ken | Guillemette, François | Amyot, Marc | Sauvé, Sébastien
The occurrence and spatial distribution of selected pesticides were investigated along a 200-km reach of the St. Lawrence River (SLR) and tributaries in Quebec, Canada. Surface water samples (n = 68) were collected in the summer 2017 and analyzed for glyphosate, atrazine (ATZ), 8 systemic insecticides (acetamiprid, clothianidin, dinotefuran, fipronil, imidacloprid, nitenpyram, thiacloprid, and thiamethoxam) and some metabolites. Overall, 99% of the surface water samples were positive to at least one of the targeted pesticides. The most recurrent compounds were glyphosate (detection frequency: 84%), ATZ (82%), thiamethoxam (59%), desethylatrazine (DEA: 47%), and clothianidin (46%). Glyphosate displayed variable levels (4–3,000 ng L−1), with higher concentrations in south tributaries (e.g., Nicolet and Yamaska). In positive samples, the sum of ATZ and DEA varied between 5 and 860 ng L−1, and the sum of 6 priority neonicotinoids between 1.5 and 115 ng L−1. From Repentigny to the Sorel Islands, the spatial distribution of pesticides within the St. Lawrence River was governed by the different upstream sources (i.e., Great Lakes vs. Ottawa River) due to the limited mixing of the different water masses. Cross-sectional patterns revealed higher concentrations of glyphosate and neonicotinoids in the north portions of transects, while the middle and south portions showed higher levels of atrazine. In Lake St. Pierre and further downstream, cross-sections revealed higher levels of the targeted pesticides near the southern portions of the SLR. This may be due to the higher contributions from south shore tributaries impacted by major agricultural areas, compared to north shore tributaries with forest land and less cropland use. Surface water samples were compliant with guidelines for the protection of aquatic life (chronic effects) for glyphosate and atrazine. However, 31% of the samples were found to surpass the guideline value of 8.3 ng L−1 for the sum of six priority neonicotinoids.
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