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1.
Environ Sci Pollut Res Int ; 30(42): 96290-96300, 2023 Sep.
Article in English | MEDLINE | ID: mdl-37567994

ABSTRACT

Caenorhabditis elegans is used for assessing the toxicity of chemicals in aqueous medium. However, chemicals can absorb to the bacterial food, which reduces the freely dissolved concentrations of the tested compounds. Thus, based on total or nominal concentrations, toxicity is underestimated, resulting in misleading assumptions on toxicity mechanisms or comparisons to other test organisms. As the verification of freely dissolved exposure concentrations (Cfree) is challenging in small test systems, simple partitioning models might by a good option for estimating Cfree. Therefore, C. elegans was exposed to seven differently acting organic chemicals with varying hydrophobicities, thus also different affinities to bind to the food of C. elegans. Measured concentrations of the dissolved aqueous and the bacterial-bound fraction allowed the calculation of binding constants (Kb). Experimental Kb were comparable to literature data of hydrophobic chemicals and correlated well with their hydrophobicity, expressed as log KOW. The chronic toxicity of the various compounds on C. elegans' reproduction, based on their aqueous concentration, was weakly related to their log KOW. Toxicity expressed based on chemical activity and comparisons with a baseline toxicity model, nevertheless, suggested a narcotic mode of action for most hydrophobic compounds (except methylisothiazolinone and trichlorocarbanilide). Although revealing a similar toxicity ranking than Daphnia magna, C. elegans was less sensitive, probably due to its ability to reduce its internal concentrations by means of its very impermeable cuticle or by efficient detoxification mechanisms. It could be shown that measured aqueous concentrations in the nematode test system corresponded well with freely dissolved concentrations that were modeled using simple mass-balance models from nominal concentrations. This offers the possibility to estimate freely dissolved concentrations of chemicals from nominal concentrations, making routine testing of chemicals and their comparison to other species more accurate.


Subject(s)
Caenorhabditis elegans , Organic Chemicals , Animals , Organic Chemicals/toxicity , Water/chemistry , Hydrophobic and Hydrophilic Interactions , Reproduction , Bacteria
2.
Chemosphere ; 330: 138752, 2023 Jul.
Article in English | MEDLINE | ID: mdl-37086980

ABSTRACT

The activated sludge process at wastewater treatment plants is important to prevent discharge of organic pollutants to the environment. Determination of biodegradation kinetics in activated sludge is challenging for mixtures that cover a diverse range of structures. The aims of this study were to (1) design a closed aerobic biodegradation batch test with activated sludge and (2) develop a sample preparation procedure that is compatible with LC-MS and Solid Phase Microextraction (SPME) coupled to GC-MS. A headspace:sludge ratio of 4:1 was sufficient to ensure aerobic conditions in activated sludge for 7 days at co-solvent concentrations <0.01%. Ethanol was added to sub-samples (50%) to stop biodegradation, extract sorbed chemicals and allow storage at -18 °C without ice formation. The ethanol extracted the chemicals from the sludge before filtration (0.2 µm). The filtrate was diluted in ultrapure water to <12% ethanol before analysis by SPME GC-MS/MS and was suitable for direct injection on LC-MS/MS. Biodegradation was distinguished from sorption through abiotic controls using autoclaved poisoned sludge. Linalool, naphthalene, α-isomethylionone, phenanthrene, citronellol, drometrizole, 2-ethylhexyl 4-methoxycinnamate, dicyclohexyl phthalate, BP-1, BP-3, methyl-, ethyl-, propylparaben, alkyl sulfates and isethionates degraded within 48 h in activated sludge, while musk ketone, tonalide and 1,3,5-trichlorobenzene did not. A 10 times reduction of sludge density did not markedly affect the microbial diversity but slowed biodegradation kinetics (partly explained by theory). This study demonstrated a 'cold' alternative to an OECD 314b test and how biodegradation kinetics can be determined for mixtures of diverse chemicals in closed batch tests with activated sludge.


Subject(s)
Sewage , Water Pollutants, Chemical , Sewage/chemistry , Chromatography, Liquid , Tandem Mass Spectrometry , Biodegradation, Environmental , Kinetics
3.
Environ Sci Technol ; 56(1): 293-301, 2022 01 04.
Article in English | MEDLINE | ID: mdl-34936331

ABSTRACT

Biodegradation of organic chemicals emitted to the environment is carried out by mixed microbial communities growing on multiple natural and xenobiotic substrates at low concentrations. This study aims to (1) perform simulation type biodegradation tests at a wide range of mixture concentrations, (2) determine the concentration effect on the biodegradation kinetics of individual chemicals, and (3) link the mixture concentration and degradation to microbial community dynamics. Two hundred ninety-four parallel test systems were prepared using wastewater treatment plant effluent as inoculum and passive dosing to add a mixture of 19 chemicals at 6 initial concentration levels (ng/L to mg/L). After 1-30 days of incubation at 12 °C, abiotic and biotic test systems were analyzed using arrow solid phase microextraction and GC-MS/MS. Biodegradation kinetics at the highest test concentrations were delayed for several test substances but enhanced for the reference chemical naphthalene. Test concentration thus shifted the order in which chemicals were degraded. 16S rRNA gene amplicon sequencing indicated that the highest test concentration (17 mg C/L added) supported the growth of the genera Acidovorax, Novosphingobium, and Hydrogenophaga, whereas no such effect was observed at lower concentrations. The chemical and microbial results confirm that too high mixture concentrations should be avoided when aiming at determining environmentally relevant biodegradation data.


Subject(s)
Odorants , Plasticizers , Biodegradation, Environmental , Kinetics , RNA, Ribosomal, 16S , Tandem Mass Spectrometry
4.
Sci Total Environ ; 749: 141397, 2020 Dec 20.
Article in English | MEDLINE | ID: mdl-32841855

ABSTRACT

The physical and biological attributes of riverine ecosystems interact in a complex manner which can affect the hydrodynamic behaviour of the system. This can alter the mixing characteristics of a river at the sediment-water interface. Research on hyporheic exchange has increased in recent years driven by a greater appreciation for the importance of this dynamic ecotone in connecting and regulating river systems. An understanding of process-based interactions driving hyporheic exchange is still limited, specifically the feedbacks between the physical and biological controlling factors. The interplay between bed morphology and sediment size on biofilm community development and the impact on hyporheic exchange mechanisms, was experimentally considered. Purpose built recirculating flume systems were constructed and three profiles of bedform investigated: i) flat, ii) undulating λ = 1 m, ii) undulating λ = 0.2 m, across two different sized sediments (0.5 mm and 5 mm). The influence of biofilm growth and bedform interaction on hyporheic exchange was explored, over time, using discrete repeat injections of fluorescent dye into the flumes. Hyporheic exchange rates were greatest in systems with larger sediment sizes (5 mm) and with more bedforms (undulating λ = 0.2). Sediment size was a dominant control in governing biofilm growth and hyporheic exchange in systems with limited bedform. In systems where bedform was prevalent, sediment size and biofilm appeared to no longer be a control on exchange due to the physical influence of advective pumping. Here, exchange rates within these environments were more consistent overtime, despite greater microbial growth. As such, bedform has the potential to overcome the rate limiting effects of biotic factors on hyporheic exchange and sediment size on microbial penetration. This has implications for pollutant and nutrient penetration; bedforms increase hydrological connectivity, generating the opportunity to support microbial communities at depth and as such, improve the self-purification ability of river systems.


Subject(s)
Microbiota , Rivers , Biofilms , Geologic Sediments , Hydrology
5.
Environ Toxicol Chem ; 39(10): 2076-2089, 2020 10.
Article in English | MEDLINE | ID: mdl-32681761

ABSTRACT

Fish acute toxicity tests are conducted as part of regulatory hazard identification and risk-assessment packages for industrial chemicals and plant protection products. The aim of these tests is to determine the concentration which would be lethal to 50% of the animals treated. These tests are therefore associated with suffering in the test animals, and Organisation for Economic Co-operation and Development test guideline 203 (fish, acute toxicity) studies are the most widely conducted regulatory vertebrate ecotoxicology tests for prospective chemical safety assessment. There is great scope to apply the 3Rs principles-the reduction, refinement, and replacement of animals-in this area of testing. An expert ecotoxicology working group, led by the UK National Centre for the Replacement, Refinement and Reduction of Animals in Research, including members from government, academia, and industry, reviewed global fish acute test data requirements for the major chemical sectors. The present study highlights ongoing initiatives and provides an overview of the key challenges and opportunities associated with replacing, reducing, and/or refining fish acute toxicity studies-without compromising environmental protection. Environ Toxicol Chem 2020;39:2076-2089. © 2020 The Authors. Environmental Toxicology and Chemistry published by Wiley Periodicals LLC on behalf of SETAC.


Subject(s)
Animal Testing Alternatives/methods , Ecotoxicology/methods , Fishes , Hazardous Substances/toxicity , Toxicity Tests, Acute/methods , Animal Testing Alternatives/legislation & jurisprudence , Animals , Ecotoxicology/legislation & jurisprudence , Lethal Dose 50 , Organisation for Economic Co-Operation and Development , Risk Assessment , Toxicity Tests, Acute/standards
6.
Toxicol In Vitro ; 67: 104905, 2020 Sep.
Article in English | MEDLINE | ID: mdl-32497684

ABSTRACT

Genotoxicity testing methods in vitro provide a means to predict the DNA damaging effects of chemicals on human cells. This is hindered in the case of hydrophobic test compounds, however, which will partition to in vitro components such as plastic-ware and medium proteins, in preference to the aqueous phase of the exposure medium. This affects the freely available test chemical concentration, and as this freely dissolved aqueous concentration is that bioavailable to cells, it is important to define and maintain this exposure. Passive dosing promises to have an advantage over traditional 'solvent spiking' exposure methods and involves the establishment and maintenance of known chemical concentrations in the in vitro medium, and therefore aqueous phase. Passive dosing was applied in a novel format to expose the MCL-5 human lymphoblastoid cell line to the pro-carcinogen, benzo[a]pyrene (B[a]P) and was compared to solvent (dimethyl sulphoxide) spiked B[a]P exposures over 48 h. Passive dosing induced greater changes, at lower concentrations, to micronucleus frequency, p21 mRNA expression, cell cycle abnormalities, and cell and nuclear morphology. This was attributed to a maintained, definable, free chemical concentration using passive dosing and the presence or absence of solvent, and highlights the influence of exposure choice on genotoxic outcomes.


Subject(s)
Carcinogens/administration & dosage , Dimethyl Sulfoxide/administration & dosage , Solvents/administration & dosage , Benzo(a)pyrene/administration & dosage , Benzo(a)pyrene/toxicity , Carcinogens/toxicity , Cell Cycle/drug effects , Cell Line , DNA Damage , Dimethyl Sulfoxide/toxicity , Humans , Micronucleus Tests , Solvents/toxicity
7.
Integr Environ Assess Manag ; 16(1): 66-77, 2020 Jan.
Article in English | MEDLINE | ID: mdl-31436368

ABSTRACT

Aquatic risk assessment of personal care chemicals requires quantifying the contribution of all product types containing these ingredients to down-the-drain emissions. We developed a probabilistic model framework embracing stochastic variability associated with individual consumers and their behaviors in the European Union, as well as other sources of uncertainty related to losses following applications (e.g., volatilization). The model was applied to decamethylcyclopentasoloxane (D5), an emollient used in wash-off (WO) and leave-on (LO) products. Quantifying contributions from each product category containing D5 to down-the-drain emissions is necessary to inform optimal risk management options. Simulation results for the baseline scenario in 2012 support the argument that LO products make up a minor contribution (7.1%) to down-the-drain emissions of D5, with only 0.20% of the D5 used in LO products being released to wastewater. The most influential model parameters are the release factor from WO products and the time between application and use for various LO product types, stressing the importance of embracing stochastic variability across individuals' behavior when assessing contributions of various product types to environmental emissions. The downward trend in WO use from 2010 to 2016 is reflected in declining concentrations in wastewater influent during the same period. Uncertainty remains about future levels of D5, once phasing out WO products is complete. The probabilistic model in conjunction with high-tier data of consumer habits is a promising high-tier tool for the characterization of complex emission scenarios of personal care ingredients. Integr Environ Assess Manag 2019;00:1-12. © 2019 SETAC.


Subject(s)
Cosmetics , Risk Assessment , Wastewater , Environmental Monitoring , European Union , Humans , Models, Statistical
8.
Chemosphere ; 164: 355-362, 2016 Dec.
Article in English | MEDLINE | ID: mdl-27596822

ABSTRACT

In order to predict the fate of chemicals in the environment, a range of regulatory tests are performed with microbial inocula collected from environmental compartments to investigate the potential for biodegradation. The abundance and distribution of microbes in the environment is affected by a range of variables, hence diversity and biomass of inocula used in biodegradation tests can be highly variable in space and time. The use of artificial or natural biofilms in regulatory tests could enable more consistent microbial communities be used as inocula, in order to increase test consistency. We investigated spatial and temporal variation in composition, biomass and chemical biodegradation potential of bacterial biofilms formed in river water. Sampling time and sampling location impacted the capacity of biofilms to degrade p-nitrophenol (PNP). Biofilm bacterial community structure varied across sampling times, but was not affected by sampling location. Degradation of PNP was associated with increased relative abundance of Pseudomonas syringae. Partitioning of the bacterial metacommunity into core and satellite taxa revealed that the P. syringae could be either a satellite or core member of the community across sampling times, but this had no impact on PNP degradation. Quantitative PCR analysis of the pnpA gene showed that it was present in all samples irrespective of their ability to degrade PNP. River biofilms showed seasonal variation in biomass, microbial community composition and PNP biodegradation potential, which resulted in inconsistent biodegradation test results. We discuss the results in the context of the mechanisms underlying variation in regulatory chemical degradation tests.


Subject(s)
Biofilms/growth & development , Fresh Water/analysis , Nitrophenols/metabolism , Pseudomonas syringae/metabolism , Water Pollutants, Chemical/metabolism , Biodegradation, Environmental , Biomass , Nitrophenols/analysis , Pseudomonas syringae/isolation & purification , Rivers , Seasons , Water Pollutants, Chemical/analysis
9.
Integr Environ Assess Manag ; 12(3): 417-21, 2016 Jul.
Article in English | MEDLINE | ID: mdl-26440537

ABSTRACT

The ecotoxicity testing of chemicals for prospective environmental safety assessment is an area in which a high number of vertebrates are used across a variety of industry sectors. Refining, reducing, and replacing the use of animals such as fish, birds, and amphibians for this purpose addresses the ethical concerns and the increasing legislative requirements to consider alternative test methods. Members of the UK-based National Centre for the Replacement, Refinement and Reduction of Animals in Research (NC3Rs) Ecotoxicology Working Group, consisting of representatives from academia, government organizations, and industry, have worked together over the past 6 y to provide evidence bases to support and advance the application of the 3Rs in regulatory ecotoxicity testing. The group recently held a workshop to identify the areas of testing, demands, and drivers that will have an impact on the future of animal use in regulatory ecotoxicology. As a result of these discussions, we have developed a pragmatic approach to prioritize and realistically address key opportunity areas, to enable progress toward the vision of a reduced reliance on the use of animals in this area of testing. This paper summarizes the findings of this exercise and proposes a pragmatic strategy toward our key long-term goals-the incorporation of reliable alternatives to whole-organism testing into regulations and guidance, and a culture shift toward reduced reliance on vertebrate toxicity testing in routine environmental safety assessment. Integr Environ Assess Manag 2016;12:417-421. © 2015 SETAC.


Subject(s)
Ecotoxicology , Environmental Policy , Animals , Prospective Studies , Risk Assessment , Toxicity Tests
10.
Environ Sci Technol ; 49(20): 12289-96, 2015 Oct 20.
Article in English | MEDLINE | ID: mdl-26378470

ABSTRACT

Toxicological research in the 1930s gave the first indications of the link between narcotic toxicity and the chemical activity of organic chemicals. More recently, chemical activity has been proposed as a novel exposure parameter that describes the fraction of saturation and that quantifies the potential for partitioning and diffusive uptake. In the present study, more than 2000 acute and chronic algal, aquatic invertebrates and fish toxicity data, as well as water solubility and melting point values, were collected from a series of sources. The data were critically reviewed and grouped by mode of action (MoA). We considered 660 toxicity data to be of acceptable quality. The 328 data which applied to the 72 substances identified as MoA 1 were then evaluated within the activity-toxicity framework: EC50 and LC50 values for all three taxa correlated generally well with (subcooled) liquid solubilities. Acute toxicity was typically exerted within the chemical activity range of 0.01-0.1, whereas chronic toxicity was exerted in the range of 0.001-0.01. These results confirm that chemical activity has the potential to contribute to the determination, interpretation and prediction of toxicity to aquatic organisms. It also has the potential to enhance regulation of organic chemicals by linking results from laboratory tests, monitoring and modeling programs. The framework can provide an additional line of evidence for assessing aquatic toxicity, for improving the design of toxicity tests, reducing animal usage and addressing chemical mixtures.


Subject(s)
Aquatic Organisms/drug effects , Ecotoxicology , Organic Chemicals/toxicity , Animals , Data Accuracy , Fishes , Invertebrates/drug effects , Models, Theoretical , Regression Analysis , Statistics as Topic , Toxicity Tests, Acute , Toxicity Tests, Chronic
11.
Appl Environ Microbiol ; 81(19): 6890-900, 2015 Oct.
Article in English | MEDLINE | ID: mdl-26209677

ABSTRACT

Microbial degradation is a major determinant of the fate of pollutants in the environment. para-Nitrophenol (PNP) is an EPA-listed priority pollutant with a wide environmental distribution, but little is known about the microorganisms that degrade it in the environment. We studied the diversity of active PNP-degrading bacterial populations in river water using a novel functional marker approach coupled with [(13)C6]PNP stable isotope probing (SIP). Culturing together with culture-independent terminal restriction fragment length polymorphism analysis of 16S rRNA gene amplicons identified Pseudomonas syringae to be the major driver of PNP degradation in river water microcosms. This was confirmed by SIP-pyrosequencing of amplified 16S rRNA. Similarly, functional gene analysis showed that degradation followed the Gram-negative bacterial pathway and involved pnpA from Pseudomonas spp. However, analysis of maleylacetate reductase (encoded by mar), an enzyme common to late stages of both Gram-negative and Gram-positive bacterial PNP degradation pathways, identified a diverse assemblage of bacteria associated with PNP degradation, suggesting that mar has limited use as a specific marker of PNP biodegradation. Both the pnpA and mar genes were detected in a PNP-degrading isolate, P. syringae AKHD2, which was isolated from river water. Our results suggest that PNP-degrading cultures of Pseudomonas spp. are representative of environmental PNP-degrading populations.


Subject(s)
Nitrophenols/metabolism , Pseudomonas/isolation & purification , Pseudomonas/metabolism , Rivers/microbiology , Bacterial Proteins/genetics , Bacterial Proteins/metabolism , Biodegradation, Environmental , Carbon Isotopes/analysis , Carbon Isotopes/metabolism , Molecular Sequence Data , Phylogeny , Pseudomonas/classification , Pseudomonas/genetics , RNA, Ribosomal, 16S/genetics
12.
Chemosphere ; 122: 38-44, 2015 Mar.
Article in English | MEDLINE | ID: mdl-25434262

ABSTRACT

Cyclic volatile methylsiloxanes (cVMS) are used in personal care products and are hydrophobic, volatile and persistent. Their environmental water concentrations are low and are difficult to detect using conventional sampling methods. This study shows the potential of passive sampling for cVMS. We used low-density polyethylene (LDPE) samplers and in-field calibration methods for octamethylcyclotetrasiloxane (D4) and decamethylcyclopentasiloxane (D5). (13)C-D4 and (13)C-D5, methyltris(trimethylsiloxy)silane (MT), tetrakis(trimethylsiloxy)silane (TK), and five deuterated polycyclic aromatic hydrocarbons (PAHs) were used as performance reference compounds (PRCs). Samplers were calibrated (7-d) using effluent at a treatment plant, with uptake of cVMS and losses of the PRCs measured at 12 time-points. Concentrations of D4 (53ngL(-1)) and D5 (1838ngL(-1)) were stable in the effluent. Uptake of D4 and loss of (13)C-D4 were isotropic and equilibrium was approached by 7-d. Two estimates of sampler uptake rate (Rs) were 2.1Ld(-1) and 2.5Ld(-1). The estimated log LDPE/water partition coefficient was 4.4. The uptake of D5 was slower (Rs=0.32Ld(-1)) and equilibrium was not reached. Offloading of (13)C-D5, MT and TK were slow, and isotropic behaviour was not demonstrated for D5. Offloading of PAHs followed the predicted pattern for LDPE. Uptake of cVMS appeared to be under membrane control, due to low diffusion coefficients in LDPE. Samplers can monitor time-weighted average concentrations of D4 for less than a week, and D5 for longer periods. LDPE samplers allow cVMS to be determined at lower concentrations than by spot sampling methods.


Subject(s)
Polyethylene/chemistry , Siloxanes/analysis , Water Pollutants, Chemical/analysis , Calibration , Polycyclic Aromatic Hydrocarbons/analysis , Polycyclic Aromatic Hydrocarbons/chemistry , Siloxanes/chemistry , Wastewater/analysis , Water Pollutants, Chemical/chemistry
13.
Ecotoxicol Environ Saf ; 111: 9-22, 2015 Jan.
Article in English | MEDLINE | ID: mdl-25450910

ABSTRACT

Society's reliance upon chemicals over the last few decades has led to their increased production, application and release into the environment. Determination of chemical persistence is crucial for risk assessment and management of chemicals. Current established OECD biodegradation guidelines enable testing of chemicals under laboratory conditions but with an incomplete consideration of factors that can impact on chemical persistence in the environment. The suite of OECD biodegradation tests do not characterise microbial inoculum and often provide little insight into pathways of degradation. The present review considers limitations with the current OECD biodegradation tests and highlights novel scientific approaches to chemical fate studies. We demonstrate how the incorporation of molecular microbial ecology methods (i.e., 'omics') may improve the underlying mechanistic understanding of biodegradation processes, and enable better extrapolation of data from laboratory based test systems to the relevant environment, which would potentially improve chemical risk assessment and decision making. We outline future challenges for relevant stakeholders to modernise OECD biodegradation tests and put the 'bio' back into biodegradation.


Subject(s)
Biodegradation, Environmental , Bacteria/metabolism , Genomics , Metabolomics , Organisation for Economic Co-Operation and Development , Proteomics , Risk Assessment , Waste Disposal, Fluid
14.
Environ Toxicol Chem ; 33(11): 2551-9, 2014 Nov.
Article in English | MEDLINE | ID: mdl-25099165

ABSTRACT

Triclosan, an antimicrobial agent commonly used in down-the-drain consumer products, is toxic to freshwater microalgae. However, the rapid photolysis and pH-dependent dissociation of this compound may give rise to uncertainty in growth inhibition tests with freshwater microalgae, if these are not well characterized. Methods are presented to minimize these uncertainties by stabilizing pH with an organic buffering agent (Bis-Tris) and by the application of ultraviolet (UV) covers to remove UV wavelengths. Toxicity tests with these methods were in compliance with the validity criteria of the Organisation for Economic Co-operation and Development test 201, and no negative effects were seen in controls relative to the unmodified method. The methods were used for toxicity tests with triclosan at pH levels of 7.0, 8.0, and 8.5, yielding effective concentration, 10% values of 0.5 µg/L, 0.6 µg/L, and 12.1 µg/L, respectively. The observed change in toxicity with pH was proportional to the change in bioconcentration factor (BCF) as calculated using the cell model (a dynamic flux model based on the Fick-Nernst-Planck equations, in this case parameterized for an algal cell). Effect concentrations produced with the methods presented in the present study offer robust data on which to base risk assessment, and it is suggested that similar approaches be used to minimize uncertainty when other compounds that dissociate and photolyse are tested.


Subject(s)
Microalgae/drug effects , Photolysis/drug effects , Scenedesmus/drug effects , Triclosan/toxicity , Water Pollutants, Chemical/toxicity , Buffers , Environmental Monitoring , Fresh Water , Hydrogen-Ion Concentration , Ions , Ultraviolet Rays
15.
Chemosphere ; 93(5): 726-34, 2013 Oct.
Article in English | MEDLINE | ID: mdl-23177715

ABSTRACT

The cyclic volatile methylsiloxane, decamethylcyclopentasiloxane (D5) is used in a large variety of personal care products. Based on the physical-chemical properties of D5, it is likely that losses due to volatilisation may strongly influence the levels entering the aquatic environment. The aim of this study was to quantify the amount of D5 in waste wash water, after typical application and use in a range of deodorant and anti-perspirant (AP) products. Results implied significant losses after a 24h period (>99.9%), and suggest that the use of D5 in leave-on products, such as deodorants/AP is not likely to contribute a significant down-the-drain emission source. An illustrative example is presented, based on data reporting the use of D5 in a range of personal care products (both wash-off and leave-on), which suggests that the contribution of D5 used in wash-off products to the aquatic environment may be considerably more significant. Limitations associated with our understanding of the actual D5 inclusion levels in the products, the market share of the products containing D5, and the variability of consumer habits, are identified as data gaps that need to be addressed in order to better refine down-the-drain emission estimates.


Subject(s)
Antiperspirants/analysis , Models, Chemical , Siloxanes/analysis , Water Pollutants, Chemical/analysis
16.
Chemosphere ; 93(5): 757-65, 2013 Oct.
Article in English | MEDLINE | ID: mdl-23177718

ABSTRACT

Monitoring of cyclic volatile methylsiloxanes (cVMS) carried out at Anglian Water's Broadholme sewage treatment plant (STP) is described. The method deployed used headspace gas chromatography/mass spectrometry (HS-GC/MS) and the addition of isotopically labelled cVMS to correct for partitioning in samples containing high levels of particulate and dissolved organic carbon. The method was capable of measuring cVMS in raw sewage samples, with recoveries of 80%, 85% and 71% respectively, for D4, D5 and D6. The limit of quantification was 0.2µgL(-1) for all three substances. Recoveries close to 100% were observed for all cVMS spiked into treated effluent (LOQ=0.01µgL(-1)). Despite the volatile nature of cVMS and its ubiquitous presence in the ambient atmosphere, the methods deployed showed excellent recoveries, reproducibility and quantification limits. A distinct diurnal variation in cVMS concentration, probably linked with the use of personal care products was observed for raw sewage but not in treated sewage effluent. The estimated per capita consumption of D5 (∼2.7mgcap(-1)d(-1)) derived for the population served by this plant was significantly lower than that derived in the Environment Agency (UK) risk assessment (11.6mgcap(-1)d(-1)). The cVMS were highly removed during sewage treatment with efficiencies greater than 98%. The methods and findings of this pilot study can be used as the basis for future studies on the fate of cVMS substances in STPs.


Subject(s)
Environmental Monitoring , Models, Chemical , Sewage/chemistry , Siloxanes/analysis , Waste Disposal, Fluid , Water Pollutants, Chemical/analysis , Gas Chromatography-Mass Spectrometry
17.
Chemosphere ; 93(5): 735-40, 2013 Oct.
Article in English | MEDLINE | ID: mdl-23186890

ABSTRACT

Decamethylcyclopentasiloxane, commonly known as D5 (cyclopentasiloxane) has a wide application of use across a multitude of personal care product categories. The relative volatility of D5 is one of the key properties attributed to this substance that provide for the derived performance benefits from the use of this raw material in personal care formulations. On this basis, rapid evaporative loss following use of many products comprising D5 is expected following typical use application and corresponding wear time. Studies were conducted on three key product categories containing D5 (antiperspirants, skin care products and hair care products) to characterize the amount of D5 that may be destined to 'go down the drain' following simulated typical personal care use scenarios. Marketed antiperspirants and skin care products were applied to human subjects and hair care products were applied to human hair tressesand subsequently rinsed off at designated time points representative of typical consumer cleansing and personal hygiene habits. Wash water was collected at 0, 8 and 24h (antiperspirant and hair care analysis) and additionally at 4h (skin care analysis) post product application and samples were analyzed by isotope dilution headspace gas chromatography/mass spectrometry (GC/MS) to quantify the concentration of D5 destined to be available to go down the drain in captured wash water. It is demonstrated that significant amounts of D5 in 'leave-on' application products evaporate during typical use and that the concentration of D5 available to go down the drain under such conditions of use is only a very small (negligible) fraction of that delivered immediately upon product application.


Subject(s)
Cosmetics/analysis , Siloxanes/analysis , Soaps/analysis , Water Pollutants, Chemical/analysis , Humans , Models, Chemical , Skin Care
18.
Environ Pollut ; 165: 208-14, 2012 Jun.
Article in English | MEDLINE | ID: mdl-22265345

ABSTRACT

China represents a significant market for the sale of personal care products (PCPs). Given the continuous emission of hundreds of chemicals used in PCPs to waste water and the aquatic environment after regular use, methods for prioritising the environmental risk assessment for China are needed. In an effort to assess the prioritisation of chemicals used in PCPs in China, we have identified the chemical ingredients used in 2500 PCPs released to the Chinese market in 2009, and estimated the annual emission of these chemicals. The physical-chemical property data for these substances have been estimated and used as model inputs in the RAIDAR model. In general, the RAIDAR model provides an overall assessment of the multimedia fate of chemicals, and provides a holistic approach for prioritising chemical ingredients. The prioritisation exercise conducted in this study is shown to be strongly influenced by loss processes, such as the removal efficiencies of WWT plants and biotransformation.


Subject(s)
Cosmetics/analysis , Environmental Pollutants/analysis , Models, Chemical , China , Cosmetics/standards , Cosmetics/toxicity , Environmental Exposure/statistics & numerical data , Environmental Pollutants/standards , Environmental Pollutants/toxicity , Environmental Pollution/statistics & numerical data , Risk Assessment
19.
Environ Sci Technol ; 45(14): 5936-42, 2011 Jul 15.
Article in English | MEDLINE | ID: mdl-21662991

ABSTRACT

Cyclic volatile methylsiloxanes are being subjected to regulatory scrutiny as possible PBT chemicals. The investigation of bioaccumulation has yielded apparently contradictory results, with high laboratory fish bioconcentration factors on the one hand and low field trophic magnification factors on the other. In this study, octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5), and dodecamethylcyclohexasiloxane (D6) were studied along with polychlorinated biphenyls (PCBs) in sediments, ragworm, and flounder from six sites in the Humber Estuary. Bioaccumulation was evaluated using multimedia bioaccumulation factors (mmBAFs) which quantified the fraction of the contaminant present in the aquatic environment that is transferred to the biota. PCB 180, a known strongly bioaccumulative chemical, was used as a benchmark. The mean mmBAF of D5 was about twice that of PCB 180 in both polycheates and flounder, while for D4 it was 6 and 14 times higher, respectively. The mmBAF of D6 was a factor 5-10 lower than that of PCB180. The comparatively strong multimedia bioaccumulation of D4 and D5, even in the absence of biomagnification, was explained by both compounds having a >100 times stronger tendency to partition into lipid rather than into organic carbon, while PCB 180 partitions to a similar extent into both matrices.


Subject(s)
Environmental Monitoring/statistics & numerical data , Flounder/metabolism , Geologic Sediments/chemistry , Hydrocarbons, Cyclic/pharmacokinetics , Polychaeta/metabolism , Siloxanes/pharmacokinetics , Volatile Organic Compounds/pharmacokinetics , Animals , England , Gas Chromatography-Mass Spectrometry , Hydrocarbons, Cyclic/analysis , Rivers , Seawater , Siloxanes/analysis , Volatile Organic Compounds/analysis
20.
Environ Sci Technol ; 45(8): 3349-54, 2011 Apr 15.
Article in English | MEDLINE | ID: mdl-21438524

ABSTRACT

The global distribution of linear and cyclic volatile methyl silxoanes (VMS) was investigated at 20 sites worldwide, including 5 locations in the Arctic, using sorbent-impregnated polyurethane foam (SIP) disk passive air samplers. Cyclic VMS are currently being considered for regulation because they are high production volume chemicals that are potentially persistent, bioaccumulative, and toxic. Linear and cyclic VMS (including L3, L4, L5, D3, D4, D5, and D6) were analyzed for in air at all urban, background, and Arctic sites. Concentrations of D3 and D4 are significantly correlated, as are D5 and D6, which suggests different sources for these two pairs of compounds. Elevated concentrations of D3 and D4 on the West coast of North America and at high elevation sites suggest these sites are influenced by trans-Pacific transport, while D5 and D6 have elevated concentrations in urban areas, which is most likely due to personal care product use. Measured concentrations of D5 were compared to modeled concentrations generated using both the Danish Eulerian Hemispheric Model (DEHM) and the Berkeley-Trent Global Contaminant Fate Model (BETR Global). The correlation coefficients (r) between the measured and modeled results were 0.73 and 0.58 for the DEHM and BETR models, respectively. Agreement between measurements and models indicate that the sources, transport pathways, and sinks of D5 in the global atmosphere are fairly well understood.


Subject(s)
Air Pollutants/analysis , Siloxanes/analysis , Volatile Organic Compounds/analysis , Air Pollutants/chemistry , Air Pollution/statistics & numerical data , Atmosphere/chemistry , Environmental Monitoring , Models, Chemical , Siloxanes/chemistry , Volatile Organic Compounds/chemistry
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