Showing papers in "Environmental Science: Processes & Impacts in 2016"
TL;DR: A first theoretical assessment of microplastics release on land, storage in soils and sediments and transport by run-off and rivers was described and it was anticipated that high flow periods can remobilize this pool of MPs.
Abstract: The presence of microplastics (MPs) in the environment is a problem of growing concern. While research has focused on MP occurrence and impacts in the marine environment, very little is known about their release on land, storage in soils and sediments and transport by run-off and rivers. This study describes a first theoretical assessment of these processes. A mathematical model of catchment hydrology, soil erosion and sediment budgets was upgraded to enable description of MP fate. The Thames River in the UK was used as a case study. A general lack of data on MP emissions to soils and rivers and the mass of MPs in agricultural soils, limits the present work to serve as a purely theoretical, nevertheless rigorous, assessment that can be used to guide future monitoring and impact evaluations. The fundamental assumption on which modelling is based is that the same physical controls on soil erosion and natural sediment transport (for which model calibration and validation are possible), also control MP transport and storage. Depending on sub-catchment soil characteristics and precipitation patterns, approximately 16-38% of the heavier-than-water MPs hypothetically added to soils (e.g. through routine applications of sewage sludge) are predicted to be stored locally. In the stream, MPs < 0.2 mm are generally not retained, regardless of their density. Larger MPs with densities marginally higher than water can instead be retained in the sediment. It is, however, anticipated that high flow periods can remobilize this pool. Sediments of river sections experiencing low stream power are likely hotspots for deposition of MPs. Exposure and impact assessments should prioritize these environments.
454 citations
TL;DR: It is proposed that through the use of appropriate sets of probe compounds and model photosensitizers an improved estimation of the distribution of triplet energies and one-electron reduction potentials of 3CDOM* can be achieved.
Abstract: Excited triplet states of chromophoric dissolved organic matter (3CDOM*) play a major role among the reactive intermediates produced upon absorption of sunlight by surface waters. After more than two decades of research on the aquatic photochemistry of 3CDOM*, the need for improving the knowledge about the photophysical and photochemical properties of these elusive reactive species remains considerable. This critical review examines the efforts to date to characterize 3CDOM*. Information on 3CDOM* relies mainly on the use of probe compounds because of the difficulties associated with directly observing 3CDOM* using transient spectroscopic methods. Singlet molecular oxygen (1O2), which is a product of the reaction between 3CDOM* and dissolved oxygen, is probably the simplest indicator that can be used to estimate steady-state concentrations of 3CDOM*. There are two major modes of reaction of 3CDOM* with substrates, namely triplet energy transfer or oxidation (via electron transfer, proton-coupled electron transfer or related mechanisms). Organic molecules, including several environmental contaminants, that are susceptible to degradation by these two different reaction modes are reviewed. It is proposed that through the use of appropriate sets of probe compounds and model photosensitizers an improved estimation of the distribution of triplet energies and one-electron reduction potentials of 3CDOM* can be achieved.
363 citations
TL;DR: It is found that in most cases attempts to promote DIET in mixed culture systems do not yield the improvements expected based on defined culture studies, and areas of future research related to DIET and its application in biological treatment processes are identified.
Abstract: Multicellular microbial communities are important catalysts in engineered systems designed to treat wastewater, remediate contaminated sediments, and produce energy from biomass Understanding the interspecies interactions within them is therefore essential to design effective processes The flow of electrons within these communities is especially important in the determination of reaction possibilities (thermodynamics) and rates (kinetics) Conventional models of electron transfer incorporate the diffusion of metabolites generated by one organism and consumed by a second, frequently referred to as mediated interspecies electron transfer (MIET) Evidence has emerged in the last decade that another method, called direct interspecies electron transfer (DIET), may occur between organisms or in conjunction with electrically conductive materials Recent research has suggested that DIET can be stimulated in engineered systems to improve desired treatment goals and energy recovery in systems such as anaerobic digesters and microbial electrochemical technologies In this review, we summarize the latest understanding of DIET mechanisms, the associated microorganisms, and the underlying thermodynamics We also critically examine approaches to stimulate DIET in engineered systems and assess their effectiveness We find that in most cases attempts to promote DIET in mixed culture systems do not yield the improvements expected based on defined culture studies Uncertainties of other processes that may be co-occurring in real systems, such as contaminant sorption and biofilm promotion, need to be further investigated We conclude by identifying areas of future research related to DIET and its application in biological treatment processes
147 citations
TL;DR: In this article, a comprehensive literature review on the occurrence of pesticide residues in Brazilian freshwaters was provided, and risk quotients were calculated to assess the potential risk posed to aquatic life by the individual pesticides based on their levels of water contamination.
Abstract: The widespread use of pesticides in agriculture can lead to water contamination and cause adverse effects on non-target organisms. Brazil has been the world's top pesticide market consumer since 2008, with 381 approved pesticides for crop use. This study provides a comprehensive literature review on the occurrence of pesticide residues in Brazilian freshwaters. We searched for information in official agency records and peer-reviewed scientific literature. Risk quotients were calculated to assess the potential risk posed to aquatic life by the individual pesticides based on their levels of water contamination. Studies about the occurrence of pesticides in freshwaters in Brazil are scarce and concentrated in few sampling sites in 5 of the 27 states. Herbicides (21) accounted for the majority of the substances investigated, followed by fungicides (11), insecticides (10) and plant growth regulators (1). Insecticides are the class of major concern. Brazil would benefit from the implementation of a nationwide pesticide freshwater monitoring program to support preventive, remediation and enforcement actions.
140 citations
TL;DR: It is concluded that the selective enrichment of freshwater DOM by SPE is less critical for subsequent FT-ICR MS analysis, because those fractions that are not sufficiently recovered have comparatively small effects on the mass spectra.
Abstract: Solid phase extraction (SPE) is often used for enrichment and clean-up prior to analysis of dissolved organic matter (DOM) by electrospray ionization (ESI) coupled to ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). It is generally accepted that extraction by SPE is not quantitative with respect to carbon concentration. However, little information is available on the selectivity of different SPE sorbents and the resulting effect for the acquired DOM mass spectra. Freshwater samples were extracted by the widely used PPL, HLB and C18 sorbents and the molecular composition and size distribution of the DOM in the extracts and in the permeates was compared to the original sample. Dissolved organic carbon (DOC) recoveries ranged between 20% and 65% for the three tested SPE sorbents. Size-exclusion chromatography coupled to organic carbon detection (SEC-OCD) revealed that limited recovery by PPL and HLB was primarily due to incomplete elution of a fraction of apparent high molecular weight from the solid phase. In contrast, incomplete retention on the solid phase, mainly observed for the C18 cartridge, was attributed to a fraction of low molecular weight. The FT-ICR mass spectra of the original sample and the SPE extracts did not differ significantly in their molecular weight distribution, but they showed sorbent specific differences in the degree of oxygenation and saturation. We concluded that the selective enrichment of freshwater DOM by SPE is less critical for subsequent FT-ICR MS analysis, because those fractions that are not sufficiently recovered have comparatively small effects on the mass spectra. This was confirmed by the extraction of model compounds, showing that very polar and small molecules are poorly extracted, but also have a low response in ESI-MS. Of the three tested SPE cartridges the PPL material offered the best properties for DOM enrichment for subsequent FT-ICR MS analysis as it minimizes too strong and too weak DOM–sorbent interactions.
128 citations
TL;DR: In this paper, the authors investigated the microbial toxicity and susceptibility to microbial degradation of PFOS and several related fluorinated compounds, i.e., short-chain perfluoroalkyl and polyfluoro-alkyl sulfonic and carboxylic acids.
Abstract: Perfluorooctane sulfonate (PFOS) and related perfluoroalkyl and polyfluoroalkyl substances (PFASs) are emerging contaminants that have been widely applied in consumer and industrial applications for decades. However, PFOS has raised public concern due to its high bioaccumulative character, environmental persistence, and toxicity. Shorter PFASs such as perfluorobutane sulfonate (PFBS) and polyfluoroalkyl compounds have been proposed as alternatives to PFOS but it is unclear whether these fluorinated substances pose a risk for public health and the environment. The objective of this research was to investigate the microbial toxicity and the susceptibility to microbial degradation of PFOS and several related fluorinated compounds, i.e., short-chain perfluoroalkyl and polyfluoroalkyl sulfonic and carboxylic acids. None of the compounds tested were toxic to the methanogenic activity of anaerobic wastewater sludge even at very high concentrations (up to 500 mg L−1). All PFASs evaluated were highly resistant to microbial degradation. PFOS was not reductively dehalogenated by the anaerobic microbial consortium even after very long periods of incubation (3.4 years). Similarly, the tested short chain perfluoroalkyl substances (i.e., PFBS and trifluoroacetic acid) and a polyfluoroalkyl PFOS analogue, 6 : 2 fluorotelomer sulfonic acid (FTSA) were also resistant to anaerobic biodegradation. Likewise, no conclusive evidence of microbial degradation was observed under aerobic conditions for any of the short-chain perfluoroalkyl and polyfluoroalkyl carboxylic acids tested after 32 weeks of incubation. Collectively, these results indicate that PFOS and its alternatives such as short chain perfluoroalkyl sulfonates and carboxylates and their polyfluorinated homologues are highly resistant to microbial degradation.
85 citations
TL;DR: The theme of this Perspective is that greater reductions in diarrheal disease transmission in LMICs can be achieved by designing interventions to interrupt the most important environmental transmission pathways.
Abstract: Every year, more than half a million children die due to diarrheal diseases. Recent studies have identified the most important etiologies of diarrheal disease are enterotoxigenic and enteropathogenic E. coli, Shigella spp., rotavirus, norovirus and Cryptosporidium spp. These etiologies are unsurprisingly characterized by a combination of high shedding, high infectivity, and transmissibility through multiple environmental reservoirs. The relative importance of the transmission routes is likely site-specific. So the impact of interventions, which typically target only one or two environmental reservoirs, is likely also site-specific. The factors influencing the transmission routes most important for diarrheal disease are complex, including – at a minimum – etiology of endemic disease; and water, sanitation, and hygiene infrastructure and practices. The site-specific nature – and complexity of transmission – helps explain the observed variation in impacts of water, sanitation, and hygiene interventions. It may also render efforts to estimate or quantify global means for interventions' impacts irrelevant. The theme of this Perspective is that greater reductions in diarrheal disease transmission in LMICs can be achieved by designing interventions to interrupt the most important environmental transmission pathways. Intervention choice should be informed by site-specific conditions, most notably: diarrheal etiology and existing water, sanitation, and hygiene infrastructure and practices. The theme is discussed through the lens of the characteristics of the most important diarrheal diseases (shedding, infectivity, growth, and persistence) and the general characteristics of environmental reservoirs (exposure pathways and fecal contamination). The discussion highlights when interventions – and combinations of interventions – will be most effective at reducing diarrheal disease burden.
81 citations
TL;DR: The fine particles showed a strong positive exponential correlation with the air exchange rates under different ventilation settings compared with coarse particles showing an opposite trend, suggesting that the ventilation system of the car was relatively more efficient in removing coarse particles from the incoming outside air.
Abstract: The understanding of rapidly evolving concentrations of particulate matter (PMC) at signalised traffic intersections (TIs) is limited, but it is important for accurate exposure assessment. We performed “mobile” and “fixed-site” monitoring of size-resolved PMCs in the 0.25–34 μm range at TIs. On-road mobile measurements were made inside a car under five different ventilation settings on a 6 km long round route, passing through 10 different TIs. Fixed-site measurements were conducted at two types (3- and 4-way) of TIs. The aims were to assess the effects of different ventilation settings on in-vehicle PMCs and their comparison during delay conditions at the TIs with those experienced by pedestrians while crossing these TIs. We also estimated the zone of influence (ZoI) for PM10, PM2.5 and PM1 under different driving conditions and fitted the probability distribution functions to fixed-site data to understand the concentration and exposure dynamics of coarse and fine particles around the studied (3- and 4-way) TIs. The fine particles (PM2.5) showed a strong positive exponential correlation with the air exchange rates under different ventilation settings compared with coarse particles (PM2.5–10) showing an opposite trend. This suggested that the ventilation system of the car was relatively more efficient in removing coarse particles from the incoming outside air. On-road median PM10, PM2.5 and PM1 during delays at the TIs were ∼40%, 16% and 17% higher, respectively, compared with free-flow conditions on the rest of the route. About 7% of the average commuting time spent during delay conditions over all the runs at the TIs corresponded to 10, 7 and 8% of the total respiratory deposition dose (RDD) for PM10, PM2.5 and PM1, respectively. The maximum length of the ZoI for PM2.5 and PM1 was highest at the 4-way TI and the maximum length of the ZoI for PM10 was highest at the 3-way TI. The on-road average RDD rate of PM10 inside the cabin when windows were fully open was up to ∼7-times that for pedestrians at the TIs.
80 citations
TL;DR: A historical perspective on the development of criteria for PBT chemicals and POPs is offered, suggestions for rationalization of protection goals are offered, some emerging procedures for identification of compounds of concern are described, and information that needs to be considered when applying criteria to screening and/or evaluation of new chemicals is proposed.
Abstract: General public concern over the effects of persistent chemicals began in the early 1960s. Since then, significant scientific advances have increased our understanding of persistent, bioaccumulative, and toxic (PBT) chemicals and the properties and processes that influence their fates in, and adverse effects on, human health and the environment. In addition to the scientific advances, a number of legislations and agreements for national, international, and global identification and control of PBT chemicals have been adopted. However, some of the rationales and thoughts that were relied upon when the first criteria were developed to identify and categorize PBT chemicals and then POPs (persistent organic pollutants) have not been carried forward. Criteria have been based upon available data of neutral hydrophobic substances as reference chemicals, derived under laboratory conditions. They evolved over the last decades due to the diversification of the protection aims under various national regulatory frameworks and international agreements, advances in methods for estimation of physical/chemical properties, and the identification of chemicals which are non-traditional POPs. Criteria are not defined purely by science; they also are subject to the aims of policy. This paper offers a historical perspective on the development of criteria for PBT chemicals and POPs. It also offers suggestions for rationalization of protection goals, describes some emerging procedures for identification of compounds of concern, and proposes information that needs to be considered when applying criteria to screening and/or evaluation of new chemicals.
78 citations
TL;DR: The composition of microbial communities present in home, school and outdoor air samples are determined by amplifying and sequencing regions of rRNA genes from bacteria (16S) and fungi (18S and ITS) and how whole communities of microbes (including unculturable taxa) influence human health is studied.
Abstract: Environmental microbes have been associated with both protective and adverse health effects in children and adults. Epidemiological studies often rely on broad biomarkers of microbial exposure (i.e. endotoxin, 1 → 3-beta-d-glucan), but fail to identify the taxonomic composition of the microbial community. Our aim was to characterize the bacterial and fungal microbiome in different types of environmental samples collected in studies of human health effects. We determined the composition of microbial communities present in home, school and outdoor air samples by amplifying and sequencing regions of rRNA genes from bacteria (16S) and fungi (18S and ITS). Samples for this pilot study included indoor settled dust (from both a Boston area birth cohort study on Home Allergens and Asthma (HAA) (n = 12) and a study of school exposures and asthma symptoms (SICAS) (n = 1)), as well as fine and coarse concentrated outdoor ambient particulate (CAP) samples (n = 9). Sequencing of amplified 16S, 18S, and ITS regions was performed on the Roche-454 Life Sciences Titanium pyrosequencing platform. Indoor dust samples were dominated by Gram-positive bacteria (Firmicutes and Actinobacteria); the most abundant bacterial genera were those related to human flora (Streptococcus, Staphylococcus, Corynebacterium and Lactobacillus). Outdoor CAPs were dominated by Gram-negative Proteobacteria from water and soil sources, in particular the genera Acidovorax, and Brevundimonas (which were present at very low levels or entirely absent in indoor dust). Phylum-level fungal distributions identified by 18S or ITS regions showed very similar findings: a predominance of Ascomycota in indoor dust and Basidiomycota in outdoor CAPs. ITS sequencing of fungal genera in indoor dust showed significant proportions of Aureobasidium and Leptosphaerulina along with some contribution from Cryptococcus, Epicoccum, Aspergillus and the human commensal Malassezia. ITS sequencing detected more than 70 fungal genera in indoor dust not observed by culture. Microbiome sequencing is feasible for different types of archived environmental samples (indoor dust, and low biomass air particulate samples), and offers the potential to study how whole communities of microbes (including unculturable taxa) influence human health.
67 citations
TL;DR: Wang et al. as discussed by the authors evaluated the occurrence, spatio-temporal distribution, mass balance and ecological risks of 43 commonly used human and veterinary antibiotics in both aqueous and sedimentary phases in a large subtropical shallow lake, Lake Taihu.
Abstract: The objective of this study was to evaluate the occurrence, spatiotemporal distribution, mass balance and ecological risks of 43 commonly used human and veterinary antibiotics in both aqueous and sedimentary phases in a large subtropical shallow lake, Lake Taihu. In the aqueous phase, sulfonamides (2.64-344 ng L(-1)), lincomycin (ND to 53.8 ng L(-1)) and florfenicol (0.15-963 ng L(-1)) were the main compounds with high concentrations and detection frequencies. In the sedimentary phase, fluoroquinolones (ND to 174 ng g(-1), dry weight) and tetracyclines (ND to 39.6 ng g(-1), dry weight) were the predominant compounds. Antibiotic concentrations in Lake Taihu were generally lower relative to data documented in previous studies on China and other countries. The composition of antibiotics showed that livestock wastewater might be the main source of antibiotics in Lake Taihu, followed by domestic wastewater. Antibiotics in the lake water showed slight spatial variation in summer and significant spatial variation in winter; whereas, antibiotic concentrations in the sediments varied obviously, with high concentrations found in the sites close to potential pollution sources. Mass balance showed that sediments are an important sink and potential source for fluoroquinolones and tetracyclines. In addition to antibiotics' physicochemical properties, the spatiotemporal distribution of antibiotics in the lake was influenced by both pollution sources and lake hydrodynamics. The environmental risk assessment results showed that sulfamethoxazole could pose high risks on the algae in the aquatic ecosystem, followed by tetracyclines (algae) and fluoroquinolones (bacteria). Overall, our study reveals complex compositions and clear spatiotemporal dynamics in Lake Taihu, which were the consequence of pollution sources and lake hydrodynamics.
TL;DR: According to the environmental risk assessment results, caffeine, trimethoprim and metoprolol were found to be the most critical compounds, due to their high risk quotient values.
Abstract: This study analyzed 15 pharmaceuticals and personal care products (PPCPs) in two rivers with different urbanization levels in the surrounding watershed (urban and suburb) in Beijing, China. Along the rivers, effluent samples from wastewater treatment plants (WWTPs) and wastewater samples from direct discharge outlets were also collected to reveal their possible contribution to the occurrence of PPCPs in these two rivers. Among the 15 PPCPs, 14 compounds were detected with caffeine (maximum 11,900 ng L(-1)) being the dominant compound. The total concentration of the detected PPCPs in direct discharge outlets (median 4706 ng L(-1)) was much higher than that in river waters (2780 ng L(-1)) and WWTP effluents (1971 ng L(-1)). The suburban-influenced Liangshui River had significantly higher PPCP concentrations compared to the urban-influenced Qing River due to more input of untreated wastewater from direct discharge outlets. Source apportionment showed that approximately 55% of the total PPCPs were contributed by untreated wastewater in the suburban-influenced river. Finally, ecological risk assessment has been regarded as a necessary part of general research. According to the environmental risk assessment results, caffeine, trimethoprim and metoprolol were found to be the most critical compounds, due to their high risk quotient values. The results of the present study can provide useful information for future PPCP pollution control and sustainable water management in Beijing, China.
TL;DR: The findings clearly indicate an impact of construction activities on the nearby downwind areas and a need for developing mitigation measures to limit their escape from the construction sites.
Abstract: Construction activities are common across cities; however, the studies assessing their contribution to airborne PM10 (≤10 μm) and PM2.5 (≤2.5 μm) particles on the surrounding air quality are limited. Herein, we assessed the impact of PM10 and PM2.5 arising from construction works in and around London. Measurements were carried out at 17 different monitoring stations around three construction sites between January 2002 and December 2013. Tapered element oscillating microbalance (TEOM 1400) and OSIRIS (2315) particle monitors were used to measure the PM10 and PM2.5 fractions in the 0.1-10 μm size range along with the ambient meteorological data. The data was analysed using bivariate concentration polar plots and k-means clustering techniques. Daily mean concentrations of PM10 were found to exceed the European Union target limit value of 50 μg m(-3) at 11 monitoring stations but remained within the allowable 35 exceedences per year, except at two monitoring stations. In general, construction works were found to influence the downwind concentrations of PM10 relatively more than PM2.5. Splitting of the data between working (0800-1800 h; local time) and non-working (1800-0800 h) periods showed about 2.2-fold higher concentrations of PM10 during working hours when compared with non-working hours. However, these observations did not allow to conclude that this increase was from the construction site emissions. Together, the polar concentration plots and the k-means cluster analysis applied to a pair of monitoring stations across the construction sites (i.e. one in upwind and the other in downwind) confirmed the contribution of construction sources on the measured concentrations. Furthermore, pairing the monitoring stations downwind of the construction sites showed a logarithmic decrease (with R(2) about 0.9) in the PM10 and PM2.5 concentration with distance. Our findings clearly indicate an impact of construction activities on the nearby downwind areas and a need for developing mitigation measures to limit their escape from the construction sites.
TL;DR: This review provides a general overview on the recent developments in chemical treatment and electrokinetic remediation (EK) technologies related to PCBs remediation, and focuses on the fundamental principles and governing factors of chemical technologies, and EK/integrated EK technologies.
Abstract: Polychlorinated biphenyls (PCBs) are manmade organic compounds, and pollution due to PCBs has been a global environmental problem because of their persistence, long-range atmospheric transport and bioaccumulation. Many physical, chemical and biological technologies have been utilized to remediate PCBs contaminated soils and sediments, and there are some emerging new technologies and combined methods that may provide cost-effective alternatives to the existing remediation practice. This review provides a general overview on the recent developments in chemical treatment and electrokinetic remediation (EK) technologies related to PCBs remediation. In particular, four technologies including photocatalytic degradation of PCBs combined with soil washing, Fe-based reductive dechlorination, advanced oxidation process, and EK/integrated EK technology (e.g., EK coupled with chemical oxidation, nanotechnology and bioremediation) are reviewed in detail. We focus on the fundamental principles and governing factors of chemical technologies, and EK/integrated EK technologies. Comparative analysis of these technologies including their major advantages and disadvantages is summarized. The existing problems and future prospects of these technologies regarding PCBs remediation are further highlighted.
TL;DR: Fipronil is a recalcitrant phenylpyrazole-based pesticide used for flea/tick treatment and termite control that is distributed in urban aquatic environments via stormwater and contributes to stream toxicity, and integration of fungi in engineered natural treatment systems could be a viable strategy for pesticide removal from stormwater runoff.
Abstract: Fipronil is a recalcitrant phenylpyrazole-based pesticide used for flea/tick treatment and termite control that is distributed in urban aquatic environments via stormwater and contributes to stream toxicity. We discovered that fipronil is rapidly metabolized (t1/2 = 4.2 d) by the white rot fungus Trametes versicolor to fipronil sulfone and multiple previously unknown fipronil transformation products, lowering fipronil concentration by 96.5%. Using an LC-QTOF-MS untargeted metabolomics approach, we identified four novel fipronil fungal transformation products: hydroxylated fipronil sulfone, glycosylated fipronil sulfone, and two compounds with unresolved structures. These results are consistent with identified enzymatic detoxification pathways wherein conjugation with sugar moieties follows initial ring functionalization (hydroxylation). The proposed pathway is supported by kinetic evidence of transformation product formation. Fipronil loss by sorption, hydrolysis, and photolysis was negligible. When T. versicolor was exposed to the cytochrome P450 enzyme inhibitor 1-aminobenzotriazole, oxidation of fipronil and production of hydroxylated and glycosylated transformation products significantly decreased (p = 0.038, 0.0037, 0.0023, respectively), indicating that fipronil is metabolized intracellularly by cytochrome P450 enzymes. Elucidating fipronil transformation products is critical because pesticide target specificity can be lost via structural alteration, broadening classes of impacted organisms. Integration of fungi in engineered natural treatment systems could be a viable strategy for pesticide removal from stormwater runoff.
TL;DR: In this paper, a film-stacking technique was used to estimate diffusion coefficients of polybrominated diphenyl ethers (PBDEs) in low density polyethylene (LDPE) and silicone rubber.
Abstract: A film-stacking technique was used to estimate diffusion coefficients of polybrominated diphenyl ethers (PBDEs) in low density polyethylene (LDPE) and silicone rubber. Substantially higher PBDE diffusion coefficients were observed for silicone rubber (AlteSil™) than for LDPE. A much steeper decrease in LDPE diffusion coefficients was found with increasing PBDE molecular weight than that for silicone rubber. From a passive sampling point-of-view, this means that for equivalent polymer–water partition coefficients for these two materials, the mass transfer resistance for these substances in the LDPE will be significantly higher than that for silicone rubber. Boundary layer control of the uptake process for silicone rubber can be expected for PBDEs. With a microplastic perspective, the low diffusion coefficients of PBDEs and in particular of decabromo diphenyl ether (BDE 209) in LDPE imply that the polymer diffusion coefficients for these plastic additives used as flame retardants need to be taken into account when considering the risk posed by microplastic particle ingestion by marine organisms.
TL;DR: In this article, the possibility of such a redox process taking place at ambient environmental conditions is studied utilizing a surrogate soil system of phenol and iron-exchanged calcium montmorillonite clay, Fe(III)CaM.
Abstract: Environmentally persistent free radicals (EPFRs) have been found at a number of Superfund sites, with EPFRs being formed via a proposed redox process at ambient environmental conditions. The possibility of such a redox process taking place at ambient environmental conditions is studied utilizing a surrogate soil system of phenol and iron(III)-exchanged calcium montmorillonite clay, Fe(III)CaM. Sorption of phenol by the Fe(III)CaM is demonstrated by Fourier-transformed infra-red (FT-IR) spectroscopy, as evidenced by the peaks between 1345 cm−1 and 1595 cm−1, and at lower frequencies between 694 cm−1 and 806 cm−1, as well as X-ray diffraction (XRD) spectroscopy, as shown by an increase in interlayer spacing within Fe(III)CaM. The formation and characterization of the EPFRs is determined by electron paramagnetic resonance (EPR) spectroscopy, showing phenoxyl-type radical with a g-factor of 2.0034 and ΔHP-P of 6.1 G at an average concentration of 7.5 × 1017 spins per g. EPFRs lifetime data are indicative of oxygen and water molecules being responsible for EPFR decay. The change in the oxidation state of the iron redox center is studied by X-ray absorption near-edge structure (XANES) spectroscopy, showing that 23% of the Fe(III) is reduced to Fe(II). X-ray photoemission spectroscopy (XPS) results confirm the XANES results. These findings, when combined with the EPFR concentration data, demonstrate that the stoichiometry of the EPFR formation under the conditions of this study is 1.5 × 10−2 spins per Fe(II) atom.
TL;DR: The aggregate technical potential for land-based negative emissions technologies (NETs) in the UK is estimated to be 12-49 Mt C eq. per year, representing around 8-32% of current emissions as discussed by the authors.
Abstract: The aggregate technical potential for land-based negative emissions technologies (NETs) in the UK is estimated to be 12–49 Mt C eq. per year, representing around 8–32% of current emissions. The proportion of this potential that could be realized is limited by a number of cost, energy and environmental constraints which vary greatly between NETs.
TL;DR: This study investigated the sorption selectivity of birnessite particle edges by combining Cd (ii) and Pb(ii) adsorption isotherms at pH 5.5 with surface structural characterization by differential pair distribution function (d-PDF) analysis, and compared the Sorption reactivity of δ-MnO2 to that of the nanomineral, 2-line ferrihydrite, which exhibits only external surface sites.
Abstract: Birnessite minerals (layer-type MnO2), which bear both internal (cation vacancies) and external (particle edges) metal sorption sites, are important sinks of contaminants in soils and sediments. Although the particle edges of birnessite minerals often dominate the total reactive surface area, especially in the case of nanoscale crystallites, the metal sorption reactivity of birnessite particle edges remains elusive. In this study, we investigated the sorption selectivity of birnessite particle edges by combining Cd(II) and Pb(II) adsorption isotherms at pH 5.5 with surface structural characterization by differential pair distribution function (d-PDF) analysis. We compared the sorption reactivity of δ-MnO2 to that of the nanomineral, 2-line ferrihydrite, which exhibits only external surface sites. Our results show that, whereas Cd(II) and Pb(II) both bind to birnessite layer vacancies, only Pb(II) binds extensively to birnessite particle edges. For ferrihydrite, significant Pb(II) adsorption to external sites was observed (roughly 20 mol%), whereas Cd(II) sorption was negligible. These results are supported by bond valence calculations that show comparable degrees of saturation of oxygen atoms on birnessite and ferrihydrite particle edges. Therefore, we propose that the sorption selectivity of birnessite edges follows the same order of that reported previously for ferrihydrite: Ca(II) < Cd(II) < Ni(II) < Zn(II) < Cu(II) < Pb(II).
TL;DR: The results obtained in this study clearly point to human impact on the natural environment in this region of Antarctica and the implementation of appropriate contamination control and remediation methods are recommended.
Abstract: The Ardley Cove area (located on the Maxwell Bay shoreline, Fildes Peninsula, King George Island, Antarctica) is characterized not only by its high biodiversity, but also by a high density of scientific stations, making it potentially one of the most impacted areas of Antarctica. In order to assess the source, contamination levels, distribution and availability of several trace elements (Cr, Ni, Cu, Zn, As, Pb, Cd and Hg) in and around Maxwell Bay, soil and seawater samples were collected. Soil samples were also collected in the study reference site near the Bellingshausen Dome area, as it lies far from centers of human activity and associated infrastructure. Enrichment factors (EFs) and sequential extractions were also used to assess the degree of contamination and availability of the trace elements under investigation. The results obtained in this study pointed to the existence of several contamination hotspots, mainly related to high levels of Zn, Pb, Cd, Cr and Ni. Comparison of the contaminant distribution patterns with data from earlier studies allowed the identification of anthropogenic sources. Use of the EF approach and sequential extractions confirmed these findings. In particular, higher extraction proportions were obtained for Zn and Pb (68 and 71%, respectively), which were also the same elements where the highest EFs were determined. The results obtained in this study clearly point to human impact on the natural environment in this region of Antarctica and we recommend the implementation of appropriate contamination control and remediation methods.
TL;DR: Based on these results, TCS should be included in studies and risk assessments that attempt to elucidate relationships between chemical stressors (e.g. antibiotics), antibiotic resistance genes, and public health.
Abstract: Triclosan, an antimicrobial chemical found in consumer personal care products, has been shown to stimulate antibiotic resistance in pathogenic bacteria. Although many studies focus on antibiotic resistance pertinent to medical scenarios, resistance developed in natural and engineered environments is less studied and has become an emerging concern for human health. In this study, the impacts of chronic triclosan (TCS) exposure on antibiotic resistance genes (ARGs) and microbial community structure were assessed in lab-scale anaerobic digesters. TCS concentrations from below detection to 2500 mg kg−1 dry solids were amended into anaerobic digesters over 110 days and acclimated for >3 solid retention time values. Four steady state TCS concentrations were chosen (30–2500 mg kg−1). Relative abundance of mexB, a gene coding for a component of a multidrug efflux pump, was significantly higher in all TCS-amended digesters (30 mg kg−1 or higher) relative to the control. TCS selected for bacteria carrying tet(L) and against those carrying erm(F) at concentrations which inhibited digester function; the pH decrease associated with digester failure was suspected to cause this selection. Little to no impact of TCS was observed on intI1 relative abundance. Microbial communities were also surveyed by high-throughput 16S rRNA gene sequencing. Compared to the control digesters, significant shifts in community structure towards clades containing commensal and pathogenic bacteria were observed in digesters containing TCS. Based on these results, TCS should be included in studies and risk assessments that attempt to elucidate relationships between chemical stressors (e.g. antibiotics), antibiotic resistance genes, and public health.
TL;DR: Comparison of the diluted effluent DEHP concentration with its environmental quality standards showed that the dilution in an effluent receiving water body can reduce the DEHP emissions to acceptable values.
Abstract: The contamination level of four phthalates in untreated and treated wastewater of fifteen wastewater treatment plants (WWTPs) and their fate in a full scale sequencing batch reactor (SBR) based WWTP was evaluated in this study. The four phthalates were diethyl phthalate (DEP), dibutyl phthalate (DBP), benzylbutyl phthalate (BBP) and diethylhexyl phthalate (DEHP). All compounds were present in untreated wastewater with DEHP being present in the highest mean concentration of 28.4 ± 5.3 μg L(-1). The concentration was in the range of 7.3 μg L(-1) (BBP) to 28.4 μg L(-1) (DEHP) in untreated wastewater and 1.3 μg L(-1) (DBP) to 2.6 μg L(-1) (DEHP) in treated wastewater. The nutrient removal process and advance tertiary treatment based WWTPs showed the highest phthalate removal efficiencies of 87% and 93%, respectively. The correlation between phthalate removal and conventional performance of WWTPs was positive. Fate analysis of these phthalates in a SBR based WWTP showed that total removal of the sum of phthalates in a primary settling tank and SBR was 84% out of which 55% is removed by biodegradation and 29% was removed by sorption to primary and secondary sludge. The percentage removal of four phthalates in primary settling tanks was 18%. Comparison of the diluted effluent DEHP concentration with its environmental quality standards showed that the dilution in an effluent receiving water body can reduce the DEHP emissions to acceptable values.
TL;DR: In this article, the long and short term inhibition impacts of Ag, CuO and CeO2 nanoparticles (NPs) on anaerobic digestion of waste activated sludge (WAS) were investigated.
Abstract: In this study, long and short term inhibition impacts of Ag, CuO and CeO2 nanoparticles (NPs) on anaerobic digestion (AD) of waste activated sludge (WAS) were investigated. CuO NPs were detected as the most toxic NPs on AD. As the CuO NP concentration increased from 5 to 1000 mg per gTS, an increase in the inhibition of AD from 5.8 to 84.0% was observed. EC50 values of short and long term inhibitions were calculated as 224.2 mgCuO per gTS and 215.1 mgCuO per gTS, respectively. Ag and CeO2 NPs did not cause drastic impacts on AD as compared to CuO NPs. In the long term test, Ag NPs created 12.1% decrease and CeO2 NPs caused 9.2% increase in the methane production from WAS at the highest dosage. FISH imaging also revealed that the abundance of Archaea in raw WAS was similar in short and long term tests carried out with WAS containing Ag and CeO2 NPs. On the other hand, CuO NPs caused inhibition of Archaea in the long term test. Digestion kinetics of WAS containing Ag, CeO2, CuO NPs were also evaluated with Gompertz, Logistic, Transference and First Order models. The hydrolysis rate constant (kH) for each concentration of Ag and CeO2 NPs and the raw WAS was 0.027745 d−1 while the kH of WAS containing high concentrations of CuO NPs was found to be 0.001610 d−1.
TL;DR: In this paper, a critical review is aimed at studying immobilized materials as potential remediation agents for the elimination of numerous toxic metal (e.g. Pb, Cd, Hg, and As) ions from polluted streams.
Abstract: Heavy metals from industrial processes are of special concern because they produce chronic poisoning in the aquatic environment. More strict environmental regulations on the discharge of toxic metals require the development of various technologies for their removal from polluted streams (i.e. industrial wastewater, mine waters, landfill leachate, and groundwater). The separation of toxic metal ions using immobilized materials (novel sorbents and membranes with doped ligands), due to their high selectivity and removal efficiency, increased stability, and low energy requirements, is promising for improving the environmental quality. This critical review is aimed at studying immobilized materials as potential remediation agents for the elimination of numerous toxic metal (e.g. Pb, Cd, Hg, and As) ions from polluted streams. This study covers the general characteristics of immobilized materials and separation processes, understanding of the metal ion removal mechanisms, a review of the application of immobilized materials for the removal of toxic metal ions, as well as the impacts of various parameters on the removal efficiency. In addition, emerging trends and opportunities in the field of remediation technologies using these materials are addressed.
TL;DR: The amount of (137)Cs released by the FNPP1 accident increased the North Pacific inventory of ( 137)Cs due to bomb testing during the 1950s and early 1960s by 20%.
Abstract: Optimal interpolation (OI) analysis was used to investigate the oceanic distributions of 134Cs and 137Cs released from the Tokyo Electric Power Company Fukushima Daiichi Nuclear Power Plant (FNPP1) accident. From the end of March to early April 2011, extremely high activities were observed in the coastal surface seawater near the FNPP1. The high activities spread to a region near 165°E in the western North Pacific Ocean, with a latitudinal center of 40°N. Atmospheric deposition also caused high activities in the region between 180° and 130°W in the North Pacific Ocean. The inventory of FNPP1-released 134Cs in the North Pacific Ocean was estimated to be 15.3 ± 2.6 PBq. About half of this activity (8.4 ± 2.6 PBq) was found in the coastal region near the FNPP1. After 6 April 2011, when major direct releases ceased, the FNPP1-released 134Cs in the coastal region decreased exponentially with an apparent half-time of about 4.2 ± 0.5 days and declined to about 2 ± 0.4 PBq by the middle of May 2011. Taking into account that the 134Cs/137Cs activity ratio was about 1 just after release and was extremely uniform during the first month after the accident, the amount of 137Cs released by the FNPP1 accident increased the North Pacific inventory of 137Cs due to bomb testing during the 1950s and early 1960s by 20%.
TL;DR: The uptake of gadolinium containing chelates by plants and animals grown in exposed water or on soil irrigated with exposed water was investigated and it was shown that the CAs can be taken up from plants.
Abstract: Gadolinium (Gd) based contrast agents (CA) are used to enhance magnetic resonance imaging. As a consequence of excretion by patients and insufficient elimination in wastewater treatment plants they are detected in high concentrations in surface water. At present, little is known about the uptake of these species by living organisms in aquatic systems. Therefore the uptake of gadolinium containing chelates by plants and animals grown in exposed water or on soil irrigated with exposed water was investigated. For this purpose two types of plants were treated with two different contrast agents. The uptake of the Gd contrast agents was studied by monitoring the elemental distribution with laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). This technique allows the multi-elemental analysis of solid samples with high resolution and little sample preparation. The analysis of L. minor showed that the uptake of Gd correlated with the concentration of gadodiamide in the water. The higher the concentration in the exposed water, the larger the Gd signal in the LA-ICP-MS acquired image. Exposure time experiments showed saturation within one day. The L. minor had contact with the CAs through roots and fronds, whereas the L. sativum only showed uptake through the roots. These results show that an external absorption of the CA through the leaves of L. sativum was impossible. All the analyzed parts of the plant showed Gd signal from the CA; the highest being at the main vein of the leaf. It is shown that the CAs can be taken up from plants. Furthermore, the uptake and distribution of Gd in Daphnia magna were shown. The exposure via cultivation medium is followed by Gd signals on the skin and in the area of the intestine, while the uptake via exposed nutrition algae causes the significantly highest Gd intensities in the area of the intestine. Because there are hints of negative effects for human organism these findings are important as they show that Gd based CAs may reach the human food chain via plants and animals growing in contaminated water or plants growing in fields which are irrigated with surface water.
TL;DR: Three recent publications that explore the interactions of microplastics with planktonic organisms to clarify the effects of these pollutants on some of the ocean's smallest and most important inhabitants are featured.
Abstract: Each year, millions of metric tons of the plastic produced for food packaging, personal care products, fishing gear, and other human activities end up in lakes, rivers, and the ocean. The breakdown of these primary plastics in the environment results in microplastics, small fragments of plastic typically less than 1–5 mm in size. These synthetic particles have been detected in all of the world's oceans and also in many freshwater systems, accumulating in sediment, on shorelines, suspended in surface waters, and being ingested by plankton, fish, birds, and marine mammals. While the occurrence of plastics in surface waters has been surveyed in a number of studies, the impacts of microplastics on marine organisms are still being elucidated. This highlight features three recent publications that explore the interactions of microplastics with planktonic organisms to clarify the effects of these pollutants on some of the ocean's smallest and most important inhabitants.
TL;DR: The influence of ingestion of uncontaminated polyethylene microspheres on the depuration rates of polychlorinated biphenyls (PCBs) in an in vivo fish feeding experiment was attempted and there was no significant difference in the elimination rate constants between the control and treatment groups, indicating that ingested plastic did not cause a measurable enhancement of depuration of PCBs by the fish in this study.
Abstract: Persistent hydrophobic chemicals sorbed to plastic can be transferred to fish and other aquatic organisms upon ingestion. However, ingestion of plastic could also lead to enhanced elimination of these chemicals if the plastic is less contaminated than the fish. Here, we attempted to measure the influence of ingestion of uncontaminated polyethylene microspheres on the depuration rates of polychlorinated biphenyls (PCBs) in an in vivo fish feeding experiment. Rainbow trout were given feed contaminated with PCBs for two consecutive days, then clean feed for three days to allow for egestion of the contaminated food. A control group of fish were then fed ordinary food pellets and a treatment group were fed pellets that additionally contained 40% by weight polyethylene microspheres. Condition factors and growth rates in both groups were similar, indicating no negative effect of the plastic microspheres on the nutritional status of the fish. Fish were sampled after zero, three, six and nine weeks, homogenized, solvent-extracted and analyzed by GC/MS. PCB concentrations declined in both groups at a rate consistent with growth dilution. There was no significant difference in the elimination rate constants between the control and treatment group, indicating that ingestion of uncontaminated plastic did not cause a measurable enhancement of depuration of PCBs by the fish in this study.
TL;DR: BPA and TCS exposure correlates with oxidative DNA damage, and significant dose-effects existed between the urinary BPA, TCS levels and the 8-OHdG concentrations.
Abstract: Both bisphenol A (BPA) and triclosan (TCS) are phenolic compounds widely used in a variety of household applications. These compounds could be released into the environment, enter the human body and cause a series of potential health hazards. Children are sensitive and susceptible to these contaminants. To investigate the potential oxidative DNA damage from exposure to BPA and TCS, ninety six urine samples of children (aged 3–6) and 57 dust samples were collected from a kindergarten in Guangzhou, China. The concentrations of urinary BPA, TCS and 8-hydroxy-2′-deoxyguanosine (8-OHdG, a biomarker of oxidative DNA damage) in urine were determined using a liquid chromatography tandem mass spectrometer. The geometric mean concentrations of urinary BPA, TCS and 8-OHdG were 1.08 μg L−1, 1.34 μg L−1 and 1.90 μg L−1, respectively. The results showed that both BPA and TCS exposures were associated with oxidative damage. Significant dose-effects existed between the urinary BPA, TCS levels and the 8-OHdG concentrations. Multiple linear regression analysis showed that one percent increase in BPA and in TCS could generate 0.15% and 0.081% increase in 8-OHdG in urine for children in Guangzhou. We also determined the concentrations of BPA in dust using high performance liquid chromatography. The mean concentration of BPA was 2.86 μg g−1 in indoor dust and 3.23 μg g−1 in outdoor dust. The dust contributes approximately 9.23% to the urinary BPA exposure for the children. In conclusion, BPA and TCS exposure correlates with oxidative DNA damage.
TL;DR: This study is the first to simultaneously monitor the PAHs in PM2.5 in three cities in Eastern China and may point to a long-range transportation of PM 2.5-PAHs from Beijing to Jinan and partially to Shanghai.
Abstract: This study investigated PM2.5-PAHs associations collected in Beijing, Jinan, and Shanghai in Eastern China. The results indicated that PM2.5 concentrations in Beijing, Jinan, and Shanghai were 125.7 μg m(-3) (18.6-355.5 μg m(-3)), 115.9 μg m(-3) (44.2-345.4 μg m(-3)), and 85.1 μg m(-3) (24.3-232.8 μg m(-3)), respectively. The PAH concentrations in terms of PM2.5 in Beijing, Jinan, and Shanghai ranged from 23.2 to 819.8 ng m(-3), 25.7 to 727.1 ng m(-3), and 8.5 to 133.9 ng m(-3), respectively. PAH concentrations were found to be positively correlated with PM2.5 concentration in Beijing and Shanghai. The compositions of PAHs in PM2.5 in Beijing and Jinan were almost the same: 11% low ring, 80-82% middle ring, and 7-9% high ring. However, Shanghai had a different composition. Source apportionment indicated that the incomplete combustion of coal and diesel and gasoline emissions were the main sources of PAHs in PM2.5 in all three cities, whereas Shanghai had a greater contribution from liquid fossil fuels. The values for the health risk assessment estimated by the benzo[a]pyrene equivalent concentration in Beijing and Jinan were 2.39 × 10(-6) and 2.57 × 10(-6), respectively, thus both exceeding the 1 × 10(-6) limit (USEPA) considered likely to pose an inhalation cancer risk to people. Shanghai, however, had a risk estimate of 5.05 × 10(-7), which is still in a safe range. This study is the first to simultaneously monitor the PAHs in PM2.5 in three cities in Eastern China and may point to a long-range transportation of PM2.5-PAHs from Beijing to Jinan and partially to Shanghai.