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Ambient volatile organic compounds (VOCs) in communities of the Athabasca oil sands region: Sources and screening health risk assessment
2018
Bari, Md Aynul | Kindzierski, Warren B.
An investigation of ambient levels and sources of volatile organic compounds (VOCs) and associated public health risks was carried out at two northern Alberta oil sands communities (Fort McKay and Fort McMurray located < 25 km and >30 km from oil sands development, respectively) for the period January 2010–March 2015. Levels of total detected VOCs were comparatively similar at both communities (Fort McKay: geometric mean = 22.8 μg/m³, interquartile range, IQR = 13.8–41 μg/m³); (Fort McMurray: geometric mean = 23.3 μg/m³, IQR = 12.0–41 μg/m³). In general, methanol (24%–50%), alkanes (26%–32%) and acetaldehyde (23%–30%) were the predominant VOCs followed by acetone (20%–24%) and aromatics (∼9%). Mean and maximum ambient concentrations of selected hazardous VOCs were compared to health risk screening criteria used by United States regulatory agencies. The Positive matrix factorization (PMF) model was used to identify and apportion VOC sources at Fort McKay and Fort McMurray. Five sources were identified at Fort McKay, where four sources (oil sands fugitives, liquid/unburned fuel, ethylbenzene/xylene-rich and petroleum processing) were oil sands related emissions and contributed to 70% of total VOCs. At Fort McMurray six sources were identified, where local sources other than oil sands development were also observed. Contribution of aged air mass/regional transport including biomass burning emissions was ∼30% of total VOCs at both communities. Source-specific carcinogenic and non-carcinogenic risk values were also calculated and were below acceptable and safe levels of risk, except for aged air mass/regional transport (at both communities), and ethylbenzene/xylene-rich (only at Fort McMurray).
Show more [+] Less [-]Correlations and adsorption mechanisms of aromatic compounds on biochars produced from various biomass at 700 °C
2018
Yang, Kun | Jiang, Yuan | Yang, Jingjing | Lin, Daohui
Knowledge of adsorption behavior of organic contaminants on high heat temperature treated biochars is essential for application of biochars as adsorbents in wastewater treatment and soil remediation. In this study, isotherms of 25 aromatic compounds adsorption on biochars pyrolyzed at 700 °C from biomass including wood chips, rice straw, bamboo chips, cellulose, lignin and chitin were investigated to establish correlations between adsorption behavior and physicochemical properties of biochars. Isotherms were well fitted by Polanyi theory-based Dubinin-Ashtakhov (DA) model with three parameters, i.e., adsorption capacity (Q⁰) and adsorption affinity (E and b). Besides the negative correlation of Q⁰ with molecular maximum cross-sectional areas (σ) of organic compounds, positive correlations of Q⁰ with total pore volume (Vₜₒₜₐₗ) and average diameter of micropore (D) of biochars were observed, indicating that adsorption by biochars is captured by the pore-filling mechanism with molecular sieving effect in biochar pores. Linear solvation energy relationships (LSERs) of adsorption affinity (E) with solvatochromic parameters of organic compounds (i. e., αₘ and π∗) were established, suggesting that hydrophobic effect, π-π interaction and hydrogen-bonding interaction are the main forces responsible for adsorption. The regression coefficient (π₁) and intercept (C) of obtained LSERs are correlated with biochar H/C and Rₘᵢcᵣₒ, respectively, implying that biochars with higher aromaticity and more micropores have stronger π-π bonding potential and hydrophobic effect potential with aromatic molecule, respectively. However, hydrogen-bonding potential of biochars for organic molecules is not changed significantly with properties of biochars. A negative correlation of b with biochar H/C is also obtained. These correlations could be used to predict the adsorption behavior of organic compounds on high heat temperature treated biochars from various biomass for the application of biochars as sorbents and for the estimating of environmental risks of organic compounds in the present of biochars.
Show more [+] Less [-]Vertical characteristics of VOCs in the lower troposphere over the North China Plain during pollution periods
2018
Sun, Jie | Wang, Yuesi | Wu, Fangkun | Tang, Guiqian | Wang, Lili | Wang, Yinghong | Yang, Yuan
In recent years, photochemical smog and gray haze-fog have frequently appeared over northern China. To determine the spatial distribution of volatile organic compounds (VOC) during a pollution period, tethered balloon flights were conducted over a suburban site on the North China Plain. Statistical analysis showed that the VOCs concentrations peaked at the surface, and decreased with altitude. A rapid decrease appeared from the surface to 400 m, with concnetrations of alkanes, alkenes, aromatics and halocarbons decreasing by 48.0%, 53.3%, 43.3% and 51.1%, respectively. At heights in the range of 500–1000 m, alkenes concnetrations decline by 40.2%; alkanes and halocarbons concnetrations only decreased by 24.8% and 6.4%, respectively; and aromatics increased slightly by 5.5%. High concentrations VOCs covered a higher range of height (400 m) on heavy pollution days due to lacking of diffusion power. The VOCs concentrations decreased by 50% at 200 m on light pollution days. The transport of air mass affected the composition and concentration of high-altitude VOCs, especially on lightly polluted days. These air masses originated in areas with abundant traffic and combustion sources. Reactive aromatics (kOH>20,000 ppm−1 min−1 and kOH<20,000 ppm−1 min−1) were the main contributor to the ozone formation, accounting for 37%, on the surface on light pollution days. The contribution increased to 52% with pollution aggravated, and increased to 64% with height. The contributions of reactive aromatics were influenced by the degree of air mass aging. Under the umbrella of aging air mass, the contribution of reactive aromatics increased with height.
Show more [+] Less [-]Reproductive and developmental changes in tree swallows (Tachycineta bicolor) are influenced by multiple stressors, including polycyclic aromatic compounds, in the Athabasca Oil Sands
2018
Fernie, K.J. | Marteinson, S.C. | Soos, C. | Chen, D. | Cruz-Martinez, L. | Smits, J.E.G.
Mining in the Athabasca Oil Sands Region (AOSR) has contributed extensively to increased exposure of wildlife to naturally occurring polycyclic aromatic compounds (PACs), yet little is known about the toxicity of PACs to wildlife in this region. We identified reproductive and developmental changes in tree swallows (Tachycineta bicolor) breeding in close proximity to mining-related activities in the AOSR, and determined these changes in relation to the birds' exposure and accumulation of 41 PACs (parent-, alkylated-PAHs), dibenzothiophenes (DBTs; previously published), diet (carbon (δ13C), nitrogen (δ15N)), volatile organic compounds, and weather variables. Tree swallow pairs (N = 43) were compared among mining-related (OS1, OS2) and reference (REF1, REF2) sites. At OS2, clutch initiation was slightly advanced (2012) but reproductive success (65%) was much lower than at the other sites (≥ 79%). Fledgling production by each pair was influenced by the timing of clutch initiation (years combined); in a highly inclement brood rearing period (2013), additional influences included the nestlings' exposure to ΣDBTs, accumulation of C1-naphthalene, the trophic position of the prey in their diet (δ15N), and record-breaking rainfall. Nestlings at OS2 were significantly lighter at day (d) 9 and d14, and in poorer body condition (d9). Nestling body mass was influenced by multiple stressors that varied by site: mass of younger nestlings (d9) was related to dietary source (δ13C; e.g., wetlands, terrestrial fields), exposure and/or accumulation of C1-phenanthrenes, C2-fluorenes, Σalkyl-PAHs and ΣDBTs, while for older nestlings (d14), body mass was related to sex, hatch date and/or rainfall during brood rearing. The swallows' exposure and accumulation of parent-PACs, alkyl-PACs and DBTs, the timing of hatching, their diet and exposure to highly inclement rains, contributed to their reproductive and developmental changes.
Show more [+] Less [-]Seasonal cycles of secondary organic aerosol tracers in rural Guangzhou, Southern China: The importance of atmospheric oxidants
2018
Yuan, Qi | Lai, Senchao | Song, Junwei | Ding, Xiang | Zheng, Lishan | Wang, Xinming | Zhao, Yan | Zheng, Junyu | Yue, Dingli | Zhong, Liuju | Niu, Xiaojun | Zhang, Yingyi
Thirteen secondary organic aerosol (SOA) tracers of isoprene (SOAI), monoterpenes (SOAM), sesquiterpenes (SOAS) and aromatics (SOAA) in fine particulate matter (PM2.5) were measured at a Pearl River Delta (PRD) regional site for one year. The characteristics including their seasonal cycles and the factors influencing their formation in this region were studied. The seasonal patterns of SOAI, SOAM and SOAS tracers were characterized over three enhancement periods in summer (I), autumn (II) and winter (III), while the elevations of SOAA tracer (i.e., 2,3-dihydroxy-4-oxopentanoic acid, DHOPA) were observed in Periods II and III. We found that SOA formed from different biogenic precursors could be driven by several factors during a one-year seasonal cycle. Isoprene emission controlled SOAI formation throughout the year, while monoterpene and sesquiterpene emissions facilitated SOAM and SOAS formation in summer rather than in other seasons. The influence of atmospheric oxidants (Ox) was found to be an important factor of the formation of SOAM tracers during the enhancement periods in autumn and winter. The formation of SOAS tracer was influenced by the precursor emissions in summer, atmospheric oxidation in autumn and probably also by biomass burning in both summer and winter. In this study, we could not see the strong contribution of biomass burning to DHOPA as suggested by previous studies in this region. Instead, good correlations between observed DHOPA and Ox as well as [NO2][O3] suggest the involvement of both ozone (O3) and nitrogen dioxide (NO2) in the formation of DHOPA. The results showed that regional air pollution may not only increase the emissions of aromatic precursors but also can greatly promote the formation processes.
Show more [+] Less [-]Rapidly probing the interaction between sulfamethazine antibiotics and fulvic acids
2018
Xu, Juan | Hu, Yan-Yun | Li, Xiu-Yan | Chen, Jie-Jie | Sheng, Guo-Ping
Antibiotics residuals in the environments receive wide concerns due to the high risk of generating antibiotic resistance. Natural organic matters (NOM) existed in the environments are considered to have the capacity of binding with organic contaminants, consequently influencing their speciation and transformation in the natural environments. To assess the migration of antibiotics in the environments, it is crucial to understand the binding mechanisms between NOM and antibiotics, which is still unclear due to the limit of available research methods. In this study, the interaction between fulvic acids (FA), one of the main components of NOM, and sulfamethazine (SMZ) was characterized by nuclear magnetic resonance (NMR) combined with surface plasmon resonance (SPR) and isothermal titration calorimetry (ITC) technology. The parameters related to kinetics and thermodynamics of the interaction were determined, and the possible mechanisms driving the interaction were also proposed. In addition, density functional theory (DFT) was used to predict the binding mode between FA and SMZ to reveal the interaction mechanism. Results indicate that FA can effectively bound with SMZ to form a stable complex with a binding constant at the level of 10³ L/mol. The kinetic parameters including association and dissociation constants were 29.4 L/mol/s and 6.64 × 10⁻³ 1/s, respectively. Hydrophobic interaction might play significant roles in the binding interaction with ancillary contribution of π-π conjunction arising from the aromatic rings stacking of FA and SMZ.
Show more [+] Less [-]Hydrocarbon-degradation and MOS-formation capabilities of the dominant bacteria enriched in sea surface oil slicks during the Deepwater Horizon oil spill
2018
Gutiérrez, Tony | Morris, Gordon | Ellis, Dave | Bowler, Bernard | Jones, Martin | Salek, Karina | Mulloy, Barbara | Teske, Andreas.
A distinctive feature of the Deepwater Horizon (DwH) oil spill was the formation of significant quantities of marine oil snow (MOS), for which the mechanism(s) underlying its formation remain unresolved. Here, we show that Alteromonas strain TK-46(2), Pseudoalteromonas strain TK-105 and Cycloclasticus TK-8 – organisms that became enriched in sea surface oil slicks during the spill – contributed to the formation of MOS and/or dispersion of the oil. In roller-bottle incubations, Alteromonas cells and their produced EPS yielded MOS, whereas Pseudoalteromonas and Cycloclasticus did not. Interestingly, the Cycloclasticus strain was able to degrade n-alkanes concomitantly with aromatics within the complex oil mixture, which is atypical for members of this genus. Our findings, for the first time, provide direct evidence on the hydrocarbon-degrading capabilities for these bacteria enriched during the DwH spill, and that bacterial cells of certain species and their produced EPS played a direct role in MOS formation.
Show more [+] Less [-]Microbial community and metagenome dynamics during biodegradation of dispersed oil reveals potential key-players in cold Norwegian seawater
2018
Ribicic, Deni | Netzer, Roman | Hazen, Terry C. | Techtmann, Stephen M. | Drabløs, Finn | Brakstad, Odd Gunnar
Oil biodegradation as a weathering process has been extensively investigated over the years, especially after the Deepwater Horizon blowout. In this study, we performed microcosm experiments at 5 °C with chemically dispersed oil in non-amended seawater. We link biodegradation processes with microbial community and metagenome dynamics and explain the succession based on substrate specialization. Reconstructed genomes and 16S rRNA gene analysis revealed that Bermanella and Zhongshania were the main contributors to initial n-alkane breakdown, while subsequent abundances of Colwellia and microorganisms closely related to Porticoccaceae were involved in secondary n‑alkane breakdown and beta‑oxidation. Cycloclasticus, Porticoccaceae and Spongiiabcteraceae were associated with degradation of mono- and poly-cyclic aromatics. Successional pattern of genes coding for hydrocarbon degrading enzymes at metagenome level, and reconstructed genomic content, revealed a high differentiation of bacteria involved in hydrocarbon biodegradation. A cooperation among oil degrading microorganisms is thus needed for the complete substrate transformation.
Show more [+] Less [-]Photo-Assisted Degradation, Toxicological Assessment, and Modeling Using Artificial Neural Networks of Reactive Gray BF-2R Dye
2018
do Nascimento, Graziele Elisandra | Napoleão, Daniella Carla | de Aguiar Silva, Polyana Karynne | da Rocha Santana, Rayany Magali | Bastos, Ana Maria Ribeiro | Zaidan, Léa Elias Mendes Carneiro | de Moura, Maiara Celine | Coelho, Luana Cassandra Breitenbach Barroso | Duarte, Marta Maria Menezes Bezerra
This work investigates the degradation of Reactive Gray BF-2R dye (a blend of reactive yellow 145, reactive orange 122 and reactive black 5 dyes) using UV/H₂O₂, Fenton, and photo-Fenton-advanced oxidative processes, with artificial sunlight and UV-C radiations. The photo-Fenton process employing UV-C radiation was the most efficient under the conditions studied. The ideal conditions for the degradation of the dye, determined using a factorial design 2³ and a study of the concentration of hydrogen peroxide ([H₂O₂]), were [H₂O₂] equal to 40 mg L⁻¹, iron concentration [Fe] of 1 mg L⁻¹, and pH between 3 and 4. The Chan and Chu non-linear kinetic model predicted the kinetic data with a degradation of over 98% for color and 68% for aromatics after 60 min. The behavior of the chemical oxygen demand fitted the first-order kinetic model well, with a degradation of 64% after 60 min. The Multilayer Perceptron 7-11-2 artificial neural network model enabled to model the degradation process of the aromatics and accurately predict the experimental data. Toxicity tests indicated that the post-treatment samples were non-toxic for Escherichia coli bacteria, and Portulaca grandiflora and Basil sabory seeds. However, they inhibited the growth of Lactuca sativa seeds and Salmonella enteritidis bacteria. The photo-Fenton process with UV-C radiation degraded the dye studied efficiently and the degradation percentages were, on average, 7% and 5% higher for color than those observed when employing the Fenton and UV/H₂O₂ processes, respectively. With the aromatic, however, they were 84% and 62% higher, thus justifying the use of this process.
Show more [+] Less [-]Fodder radish seed cake biochar for soil amendment
2018
Silvestre, Wendel Paulo | Galafassi, Paula Lúcia | Ferreira, Suelem Daiane | Godinho, Marcelo | Pauletti, Gabriel Fernandes | Baldasso, Camila
In this work, fodder radish seed cake (FRSC) was pyrolyzed in a rotary kiln reactor at 0, 3, and 6 rpm, at final temperature of 500 °C. Maximum biochar yield was observed at 0 rpm (≈ 26 wt.%). Increase of the rotary speed decreased the volatile matter content and increased the ash content of the biochars. Biochars exhibited alkaline pH (≈ 9.0), low electrical conductivity (< 105.6 dS m⁻¹), and high cation exchange capacity (69 to 78 cmolc kg⁻¹), as well as high nitrogen contents (≈ 80 g kg⁻¹). FTIR analysis presented biochars with similar spectra, with carboxyl and carbonyl groups within the structure, along with aromatic rings and nitrogen containing functions (amides). Biochar incubation experiments in an acrisol at different biochar doses (5 g L⁻¹ soil to 40 g L⁻¹ soil) were performed in order to evaluate changes in soil fertility parameters caused by FRSC biochar application. Results indicated that most of macro (N, P, K, Ca, Mg) and micronutrients (S, Cu, Zn, Mn, B, Na) increased with increase of the dosage, along with the decrease in Al and H+ Al contents. An increase in pH (from 4.25 to 5.33) was also observed, in electric conductivity (from 30.0 to 45.7 dS m⁻¹), and a decrease in soil real density (from 3.67 to 2.99 kg L⁻¹) at the dosage of 40 g char L⁻¹ soil.
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