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Chemical composition and source apportionment of PM10 at an urban background site in a high–altitude Latin American megacity (Bogota, Colombia)
2018
Ramírez R., Omar | Sánchez de la Campa, A.M. | Amato, F. (Fulvio) | Catacolí, Ruth A. | Rojas, Néstor Y. | Rosa, Jesús de la
Bogota registers frequent episodes of poor air quality from high PM₁₀ concentrations. It is one of the main Latin American megacities, located at 2600 m in the tropical Andes, but there is insufficient data on PM₁₀ source contribution. A characterization of the chemical composition and the source apportionment of PM₁₀ at an urban background site in Bogota was carried out in this study. Daily samples were collected from June 2015 to May 2016 (a total of 311 samples). Organic carbon (OC), elemental carbon (EC), water soluble compounds (SO₄²⁻, Cl⁻, NO₃⁻, NH₄⁺), major elements (Al, Fe, Mg, Ca, Na, K, P) and trace metals (V, Cd, Pb, Sr, Ba, among others) were analyzed. The results were interpreted in terms of their variability during the rainy season (RS) and the dry season (DS). The data obtained revealed that the carbonaceous fraction (∼51%) and mineral dust (23%) were the main PM₁₀ components, followed by others (15%), Secondary Inorganic Compounds (SIC) (11%) and sea salt (0.4%). The average concentrations of soil, SIC and OC were higher during RS than DS. However, peak values were observed during the DS due to photochemical activity and forest fires. Although trace metals represented <1% of PM₁₀, high concentrations of toxic elements such as Pb and Sb on RS, and Cu on DS, were obtained. By using a PMF model, six factors were identified (∼96% PM₁₀) including fugitive dust, road dust, metal processing, secondary PM, vehicles exhaust and industrial emissions. Traffic (exhaust emissions + road dust) was the major PM₁₀ source, accounting for ∼50% of the PM₁₀. The results provided novel data about PM₁₀ chemical composition, its sources and its seasonal variability during the year, which can help the local government to define control strategies for the main emission sources during the most critical periods.
Show more [+] Less [-]Diverse mechanisms drive fluoride enrichment in groundwater in two neighboring sites in northern China
2018
Li, Danni | Gao, Xubo | Wang, Yanxin | Luo, Wenting
Excessive amounts of fluoride in drinking groundwater are harmful to human health, but the mechanisms responsible for fluoride enrichment in groundwater are not fully understood. Samples from two neighboring areas with endemic fluorosis were collected to test the hypothesis that there are distinctly different mechanisms responsible for the enrichment of fluoride in these groundwater. Hydrochemistry, stable isotopes and geochemical simulation were conducted together to investigate the fluoride spatial distribution and the diversity of responsible mechanisms. Our results showed that the spatial distributions of fluoride are different: I) high [F] in fresh shallow groundwater (SGQJ) and II) medium [F] in fresh to brackish deep groundwater (DGQJ) in the Qiji area; and III) medium [F] in brackish shallow groundwater (SGYH) and IV) low [F] in fresh deep groundwater (DGYH) in the Yanhu area. We also found that the fluoride concentration in groundwater is primarily controlled by the dissolution equilibrium of fluorite, as suggested by the correlation between [F] and [Ca]. However, there are other significant mechanisms: 1) for SGQJ, fluoride-bearing minerals (such as fluorite) dissolution, along with moderate evaporation, cation exchange and the more alkaline conditions are the driving factors; 2) for SGYH, the contributing factors are strong evaporation, the salt effect, dissolution of evaporites, gypsum and dolomite, bicarbonate-fluoride competition and anthropogenic activity; 3) for DGQJ, cation exchange, alkaline conditions and competitive adsorption are major factors; and 4) dolomite dissolution promotes the [F] increase in DGYH. Our findings suggest that the hydrogeochemical conditions play key roles in the enrichment of fluoride and that caution should be taken in the future when evaluating fluoride occurrence in groundwater, even in nearby areas.
Show more [+] Less [-]Transport and retention of surfactant- and polymer-stabilized engineered silver nanoparticles in silicate-dominated aquifer material
2018
Adrian, Yorck F. | Schneidewind, Uwe | Bradford, Scott A. | Simunek, Jirka | Fernandez-Steeger, Tomas M. | Azzam, R. (Rafig)
Packed column experiments were conducted to investigate the transport and blocking behavior of surfactant- and polymer-stabilized engineered silver nanoparticles (Ag-ENPs) in saturated natural aquifer media with varying content of material < 0.063 mm in diameter (silt and clay fraction), background solution chemistry, and flow velocity. Breakthrough curves for Ag-ENPs exhibited blocking behavior that frequently produced a delay in arrival time in comparison to a conservative tracer that was dependent on the physicochemical conditions, and then a rapid increase in the effluent concentration of Ag-ENPs. This breakthrough behavior was accurately described using one or two irreversible retention sites that accounted for Langmuirian blocking on one site. Simulated values for the total retention rate coefficient and the maximum solid phase concentration of Ag-ENPs increased with increasing solution ionic strength, cation valence, clay and silt content, decreasing flow velocity, and for polymer-instead of surfactant-stabilized Ag-ENPs. Increased Ag-ENP retention with ionic strength occurred because of compression of the double layer and lower magnitudes in the zeta potential, whereas lower velocities increased the residence time and decreased the hydrodynamics forces. Enhanced Ag-ENP interactions with cation valence and clay were attributed to the creation of cation bridging in the presence of Ca2+. The delay in breakthrough was always more pronounced for polymer-than surfactant-stabilized Ag-ENPs, because of differences in the properties of the stabilizing agents and the magnitude of their zeta-potential was lower. Our results clearly indicate that the long-term transport behavior of Ag-ENPs in natural, silicate dominated aquifer material will be strongly dependent on blocking behavior that changes with the physicochemical conditions and enhanced Ag-ENP transport may occur when retention sites are filled.
Show more [+] Less [-]Concurrent aggregation and transport of graphene oxide in saturated porous media: Roles of temperature, cation type, and electrolyte concentration
2018
Wang, Mei | Gao, Bin | Tang, Deshan | Yu, Congrong
Simultaneous aggregation and retention of nanoparticles can occur during their transport in porous media. In this work, the concurrent aggregation and transport of GO in saturated porous media were investigated under the conditions of different combinations of temperature, cation type (valence), and electrolyte concentration. Increasing temperature (6–24 °C) at a relatively high electrolyte concentration (i.e., 50 mM for Na⁺, 1 mM for Ca²⁺, 1.75 mM for Mg²⁺, and 0.03 and 0.05 mM for Al³⁺) resulted in enhanced GO retention in the porous media. For instance, when the temperature increased from 6 to 24 °C, GO recovery rate decreased from 31.08% to 6.53% for 0.03 mM Al³⁺ and from 27.11% to 0 for 0.05 mM Al³⁺. At the same temperature, increasing cation valence and electrolyte concentration also promoted GO retention. Although GO aggregation occurred in the electrolytes during the transport, the deposition mechanisms of GO retention in the media depended on cation type (valence). For 50 mM Na⁺, surface deposition via secondary minima was the dominant GO retention mechanism. For multivalent cation electrolytes, GO aggregation was rapid and thus other mechanisms such as physical straining and sedimentation also played important roles in controlling GO retention in the media. After passing through the columns, the GO particles in the effluents showed better stability with lower initial aggregation rates. This was probably because less stable GO particles with lower surface charge densities in the porewater were filtered by the porous media, resulting in more stable GO particle with higher surface charge densities in the effluents. An advection–dispersion-reaction model was applied to simulate GO breakthrough curves and the simulations matched all the experimental data well.
Show more [+] Less [-]Physiochemical characteristics of aerosol particles collected from the Jokhang Temple indoors and the implication to human exposure
2018
Cui, Lulu | Duo, Bu | Zhang, Fei | Li, Chunlin | Fu, Hongbo | Chen, Jianmin
This paper presents a detailed study on the indoor air pollution in the Jokahng Temple at Tibet Plateau, and its implication to human health. The mean concentrations of PM1.0 and PM2.5 were 435.0 ± 309.5 and 483.0 ± 284.9 μg/m3, respectively. The PM2.5 concentration exceeded the National Ambient Air Quality Standard (75 μg/m3) by 6.4 times. The size-segregated aerosols displayed a bimodal distribution. One peak was observed in the fine mode (0.4–2.1 μm) and the other peak appeared in the coarse mode (2.1–9.0 μm). The concentration of the total size-resolved PM was 794.3 ± 84.9 μg/m3. The mass fraction of coarse particles shared by 41.1%, apparently higher than that reported at low altitudes, probably due to incomplete combustion at Tibet Plateau with hypoxic atmospheric environment. The total concentration of polycyclic aromatic hydrocarbons (PAHs) was 331.2 ± 60.3 ng/m3, in which the concentration of benzo(a)pyrene (BaP) was 18.5 ± 4.3 ng/m3, over ten times higher than the maximum permissible risk value of 1 ng/m3 on account of carcinogenic potency of particulate PAHs through inhalation. PAHs exhibited a trimodal distribution, of which two peaks were observed in the fine mode and one peak in the coarse mode. With the aromatic rings increasing, the peak intensity increased in the fine mode. Na, Ca, Al, Mg and K dominated the elemental mass profiles, and metals displayed a bimodal distribution with a dominant peak in the coarse range. The total PAH deposition flux was 123.6 and 53.1 ng/h for adults and children, respectively. Coarse particles contributed most deposition flux in the head region, while fine particles contribute most deposition flux in the alveolar region. The increment lifetime cancer risk (ILCR) of PAHs ranaged at 10−5-10−4, indicating potential cancer risk to human health. The total deposition flux of metals was estimated at 1.4–13.2 ng/h. With the size increasing, deposition flux increased in the head region while decreased in the alveolar region. The highest ILCR of Cr and Ni were 4.9 × 10−5 and 1.5 × 10−6, respectively, exceeding the permissible risk of 10−6. The hazard quotient (HQ) of Fe (10−5-10−4) and Zn (10−6-10−5) were much lower than the safe level of 1.0, and thus they were not considered as a health concern.
Show more [+] Less [-]Indoor air pollution affects hypertension risk in rural women in Northern China by interfering with the uptake of metal elements: A preliminary cross-sectional study
2018
Wang, Bin | Zhu, Yibing | Pang, Yiming | Xie, Jing | Hao, Yongxiu | Yan, Huina | Li, Zhiwen | Ye, Rongwei
Coal combustion and passive smoking are two important contributors to indoor air pollution (IAP) in rural areas of northern China. Although the association between outdoor air pollutants and hypertension risk had been widely reported, fewer studies have examined the relationship between IAP and hypertension risk. This study evaluated the association between IAP and hypertension risk in housewives in rural areas of northern China and the potential mediation pathway of metal elements. Our cross-sectional study, conducted in Shanxi Province, China, enrolled 367 subjects without taking anti-hypertensive drugs, including 142 subjects with hypertension (case group) and 225 subjects without hypertension (control group). We collected information on energy use characteristics and lifestyle using questionnaires. An IAP exposure index was developed to indicate the population exposure to coal combustion and passive smoking. Scalp hair samples were collected from the housewives and various trace and major metal elements were measured. Our results revealed that the IAP index was positively correlated with systolic and diastolic blood pressure. A significant association between the IAP index and hypertension risk was found both without [odds ratio (95% confidence interval, CI) = 2.08 (1.30–3.31)] and with [OR (95% CI) = 2.52 (1.46–4.36)] adjustment for confounders. We also observed that the IAP index was positively correlated with the arsenic, lead, and rare earth element levels in hair samples, and negatively correlated with the levels of some other trace elements (i.e., chromium, cobalt, nickel, and tin) and alkaline earth elements (i.e., calcium, magnesium, and barium) with an overall p value of <0.01. We concluded that IAP may contribute to the development of hypertension in rural housewives in northern China, possibly by interfering with the uptake of metal elements.
Show more [+] Less [-]Chemical composition and source-apportionment of sub-micron particles during wintertime over Northern India: New insights on influence of fog-processing
2018
Rajput, Prashant | Singh, Dharmendra Kumar | Singh, Amit Kumar | Gupta, Tarun
A comprehensive study was carried out from central part of Indo-Gangetic Plain (IGP; at Kanpur) to understand abundance, temporal variability, processes (secondary formation and fog-processing) and source-apportionment of PM₁-bound species (PM₁: particulate matter of aerodynamic diameter ≤ 1.0 μm) during wintertime. A total of 50 PM₁ samples were collected of which 33 samples represent submicron aerosol characteristics under non-foggy condition whereas 17 samples represent characteristics under thick foggy condition. PM₁ mass concentration during non-foggy episodes varied from 24–393 (Avg.: 247) μg m⁻³, whereas during foggy condition it ranged from 42–243 (Avg.: 107) μg m⁻³. With respect to non-foggy condition, the foggy conditions were associated with higher contribution of PM₁-bound organic matter (OM, by 23%). However, lower fractional contribution of SO₄²⁻, NO₃⁻ and NH₄⁺ during foggy conditions is attributable to wet-scavenging owing to their high affinity to water. Significant influence of fog-processing on organic aerosols composition is also reflected by co-enhancement in OC/EC and WSOC/OC ratio during foggy condition. A reduction by 5% in mineral dust fraction under foggy condition is associated with a parallel decrease in PM₁ mass concentration. However, mass fraction of elemental carbon (EC) looks quite similar (≈3% of PM₁) but the mass absorption efficiency (MAE) of EC is higher by 30% during foggy episodes. Thus, it is evident from this study that fog-processing leads to quite significant enhancement in OM (23%) contribution (and MAE of EC) with nearly equal and parallel decrease in SO₄²⁻, NO₃⁻ and NH₄⁺ and mineral dust fractions (totaling to 24%). Characteristic features of mineral dust remain similar under foggy and non-foggy conditions; inferred from similar ratios of Fe/Al (≈0.3), Ca/Al (0.35) and Mg/Al (0.22). Positive matrix factorization (PMF) resolves seven sources: biomass burning (19.4%), coal combustion (1.1%), vehicular emission (3%), industrial activities (6.1%), leather tanneries (4%), secondary transformations (46.2%) and mineral dust (20.2%).
Show more [+] Less [-]Ambient air quality in the holy city of Makkah: A source apportionment with elemental enrichment factors (EFs) and factor analysis (PMF)
2018
Nayebare, Shedrack R. | Aburizaiza, Omar S. | Siddique, Azhar | Carpenter, David O. | Hussain, Mirza M. | Zeb, Jahan | Aburiziza, Abdullah J. | Khwaja, Haider A.
Air pollution remains a major global public health and environmental issue. We assessed the levels of PM₂.₅ and delineated the major sources in Makkah, Saudi Arabia. Fine particulate matter (PM₂.₅) sampling was performed from February 26, 2014–January 27, 2015 in four cycles/seasons. Samples were analyzed for black carbon (BC) and trace elements (TEs). PM₂.₅ source apportionment was performed by computing enrichment factors (EFs) and positive matrix factorization (PMF). Backward-in time trajectories were used to assess the long-range transport. Significant seasonal variations in PM₂.₅ were observed, Spring: 113 ± 67.1, Summer: 88.3 ± 36.4, Fall: 67.8 ± 24, and Winter: 67.6 ± 36.9 μg m⁻³. The 24-h PM₂.₅ exceeded the WHO (25 μg m⁻³) and Saudi Arabia's (35 μg m⁻³) guidelines, with an air quality index (AQI) of “unhealthy to hazardous” to human health. Most delta–C computations were below zero, indicating minor contributions from bio-mass burning. TEs were primarily Si, Ca, Fe, Al, S, K and Mg, suggesting major contributions from soil (Si, Ca, Fe, Al, Mg), and industrial and vehicular emissions (S, Ca, Al, Fe, K). EF defined two broad categories of TEs as: anthropogenic (Cu, Zn, Eu, Cl, Pb, S, Br and Lu), and earth-crust derived (Al, Si, Na, Mg, Rb, K, Zr, Ti, Fe, Mn, Sr, Y, Cr, Ga, Ca, Ni and Ce). Notably, all the anthropogenic TEs can be linked to industrial and vehicular emissions. PMF analysis defined four major sources as: vehicular emissions, 30.1%; industrial-mixed dust, 28.9%; soil/earth-crust, 24.7%; and fossil-fuels/oil combustion, 16.3%. Plots of wind trajectories indicated wind direction and regional transport as major influences on air pollution levels in Makkah. In collusion, anthropogenic emissions contributed >75% of the observed air pollution in Makkah. Developing strategies for reducing anthropogenic emissions are paramount to controlling particulate air pollution in this region.
Show more [+] Less [-]Biouptake of a rare earth metal (Nd) by Chlamydomonas reinhardtii – Bioavailability of small organic complexes and role of hardness ions
2018
Yang, Guang | Wilkinson, Kevin J.
A green alga, Chlamydomonas reinhardtii, was used to verify whether a simple Biotic Ligand Model (BLM) could be used to predict carefully controlled short-term biouptake for the lanthanide, Nd. In the absence of ligands or competitors, Nd biouptake was well described by a Michaelis-Menten equation with an affinity constant, KNd, of 10⁶.⁸ M⁻¹ and a maximum internalization flux of Jₘₐₓ = 1.70 × 10⁻¹⁴ mol cm⁻² s⁻¹. For bi-metal mixtures containing Nd and Ca, Mg, Sm or Eu, Nd uptake could also be well modelled by assigning experimentally determined affinity constants of KCₐ = 10².⁶ M⁻¹, KMg = 10³.⁴ M⁻¹, KSₘ = 10⁶.⁵ M⁻¹ and KEᵤ = 10⁶.⁵ M⁻¹. The similar values of Kₘ and Jₘₐₓ for the three rare earth elements (REEs): Sm, Eu and Nd is consistent with them sharing a common metal uptake site. On the other hand, in the presence of the small organic ligands (citric or malic acid), neither, free or total Nd concentrations could be used to quantitatively predict Nd internalization fluxes. In other words, in order to predict biouptake by simple BLM determinations, it was necessary to consider that the Nd complexes were bioavailable. The data strongly suggest that risk evaluations of the REE will require a new paradigm and new tools for evaluating bioavailability.
Show more [+] Less [-]Uranium adsorption and subsequent re-oxidation under aerobic conditions by Leifsonia sp. - Coated biochar as green trapping agent
2018
Ding, Lei | Tan, Wen-fa | Xie, Shui-bo | Mumford, Kathryn | Lv, Jun-wen | Wang, Hong-qiang | Fang, Qi | Zhang, Xiao-wen | Wu, Xiao-yan | Li, Mi
It has generally been assumed that the immobilization of U(VI) via polyphosphate accumulating microorganisms may present a sink for uranium, but the potential mechanisms of the process and the stability of precipitated uranium under aerobic conditions remain elusive. This study seeks to explore the mechanism, capacity, and stability of uranium precipitation under aerobic conditions by a purified indigenous bacteria isolated from acidic tailings (pH 6.5) in China. The results show that over the treatment ranges investigated, maximum removal of U(VI) from aqueous solution was 99.82% when the initial concentration of U(VI) was 42 μM, pH was 3.5, and the temperature was with 30 °C much higher than that of other reported microorganisms. The adsorption mechanism was elucidated via the use of SEM-EDS, XPS and FTIR. SEM-EDS showed two peaks of uranium on the surface. A plausible explanation for this, supported by FTIR, is that uranium precipitated on the biosorbent surfaces. XPS measurements indicated that the uranium product is most likely a mixture of 13% U(VI) and 87% U(IV). Notably, the reoxidation experiment found that the uranium precipitates were stable in the presence of Ca²⁺ and Mg²⁺, however, U(IV) is oxidized to U(VI) in the presence of NO₃⁻ and Na⁺ ions, resulting in rapid dissolution. It implies that the synthesized Leifsonia sp. coated biochar could be utilized as a green and effective biosorbent. However, it may not a good choice for in-situ remediation due to the subsequent re-oxidation under aerobic conditions. These observations can be of some guiding significance to the application of the bioremediation technology in surface environments.
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