From the shop to the drain — Volatile methylsiloxanes in cosmetics and personal care products

Organosiloxanes are widely used in the formulation of a broad range of cosmetic and personal care products (PCPs), including creams and lotions, bath soaps, shampoo and hair care products to soften, smooth, and moisten. In fact, the intensive and widespread use of organosiloxanes combined with their lipophilic nature, makes them interesting targets for future research, particularly in the toxicology area.This study focused on determining the concentration levels of these compounds in the bestselling brands of PCPs in the Oporto region (Portugal), allowing the estimation of dermal and inhalation exposure to siloxanes and the evaluation of the quantities released to the environment “down-the-drain” and to air. To accomplish this task, a QuEChERS technique (“Quick, Easy, Cheap, Effective, Rugged, and Safe”) was employed to extract the siloxanes from the target PCPs, which has never been tested before. The resulting extract was analysed by gas chromatography–mass spectrometry (GC–MS). The limits of detection varied between 0.17 (L2) and 3.75 ng g^− 1 (L5), being much lower than any values reported in the literature for this kind of products. In general, satisfactory precision (< 10%) and accuracy values (average recovery of 84%) were obtained.123 PCPs were analysed (moisturizers, deodorants, body and hair washes, toilet soaps, toothpastes and shaving products) and volatile methylsiloxanes were detected in 96% of the samples, in concentrations between 0.003 μg g^− 1 and 1203 μg g^− 1. Shampoo exhibited the highest concentration for cyclic and aftershaves for linear siloxanes. Combining these results with the daily usage amounts, an average daily dermal exposure of 25.04 μg kg_bw^− 1 day^− 1 for adults and 0.35 μg kg_bw^− 1 day^− 1 for baby/children was estimated. The main contributors for adult dermal exposure were body moisturizers, followed by facial creams and aftershaves, while for babies/children were body moisturizers, followed by shower gel and shampoo. Similarly, the average daily inhalation exposure was also estimated. Values of 1.56 μg kg_bw^− 1 day^− 1 for adults and 0.03 μg kg_bw^− 1 day^− 1 for babies/children were calculated. An estimate of the siloxanes amount released “down-the-drain” into the sewage systems through the use of toiletries was also performed. An emission per capita between 49.25 and 9574 μg day^− 1 (mean: 1817 μg day^− 1) is expected and shampoo and shower gel presented the higher mean total values (1008 μg day^− 1 and 473.3 μg day^− 1, respectively). In the worst-case scenario, D5 and D3 were the predominant siloxanes in the effluents with 3336 μg day^− 1 and 3789 μg day^− 1, respectively. Regarding the air emissions per capita, values between 8.33 and 6109 μg day^− 1 (mean: 1607 μg day^− 1) are expected and D5 and D6 were the predominant siloxanes.     

A geographical comparison of mercury in seabirds in the eastern Canadian Arctic

Mercury (Hg) is a potentially toxic metal ubiquitous in arctic biota. Livers of adult thick-billed murres (Uria lomvia) and northern fulmars (Fulmarus glacialis) sampled from several locations in the eastern Canadian Arctic during 2007–2008 were analyzed for total Hg in order to assess geographical patterns. Thick-billed murres were collected from five colonies (Coats Island, Digges Island, Akpatok Island, Prince Leopold Island, Minarets) and northern fulmars from two colonies (Prince Leopold Island, Minarets). Murres at the two high Arctic colonies of Prince Leopold Island and the Minarets had significantly higher (two-fold) Hg concentrations (4.13 ± 019 μg g^− 1 dw and 4.41 ± 0.33 μg g^− 1 dw, respectively) than at the three low Arctic colonies (colony means of 1.62, 1.99 and 2.15 μg g^− 1 dw). The differences in Hg concentrations observed between high and low Arctic murre colonies may reflect a combination of different source regions for Hg, as well as a recent dietary shift among low Arctic murres. Fulmars from Prince Leopold Island had significantly higher Hg levels (6.99 ± 1.13 μg g^− 1 dw) than those from the Minarets (3.42 ± 0.53 μg g^− 1 dw) which may reflect different Hg deposition and methylation patterns on both summer and winter feeding areas. Although there is no evidence linking Hg to adverse population effects in either murres or fulmars at the colonies sampled, levels in some Canadian Arctic marine birds have increased over recent decades and, therefore, continued monitoring, particularly of the high Arctic colonies, is warranted.     

Uranium in drinking-water: A unique case of guideline value increases and discrepancies between chemical and radiochemical guidelines

BackgroundUranium represents a unique case for an element naturally present in the environment, as its chemical guideline value in drinking water significantly increased from 2 μg/L in 1998 up to 15 μg/L in 2004 and then to 30 μg/L in 2011, to date corresponding to a multiplication factor of 15 within a period of just 13 years.ObjectivesIn this commentary we summarize the evolution of uranium guideline values in drinking-water based on both radiological and chemical aspects, emphasizing the benefit of human studies and their contribution to recent recommendations. We also propose a simpler and better consistency between radiological and chemical values.DiscussionThe current chemical guideline value of 30 μg/L is still designated as provisional because of scientific uncertainties regarding uranium toxicity. During the same period, the radiological guideline for ²³⁸U increased from 4 Bq/L to 10 Bq/L while that for ²³⁴U decreased from 4 Bq/L to 1 Bq/L. These discrepancies are discussed here, and a value of 1 Bq/L for all uranium isotopes is proposed to be more consistent with the current chemical value of 30 μg/L.ConclusionContinuous progress in the domains of toxicology and speciation should enable a better interpretation of the biological effects of uranium in correlation with epidemiological human studies. This will certainly aid future proposals for uranium guideline values.     

Monocyclic and bicyclic monoterpenes in air of German daycare centers and human biomonitoring in visiting children,the LUPE 3 study

To investigate the assumed association between indoor air pollution with monoterpenes (MTps) and the internal MTp exposure of occupants, a comparative study was performed in daycare centers in two federal states of Germany. Three well-known monoterpenoid air pollutants, viz. α-pinene (αPN), Δ³-carene (CRN), and R-limonene (LMN), were measured in indoor air in 45 daycare centers. Additionally, urine samples of 222 children visiting these facilities were collected in the evening after a full-day stay. Altogether 11 MTp metabolites were analyzed in the urine samples using a novel highly sensitive and selective gas chromatographic–tandem-mass spectrometric procedure. The medians (95th percentiles) of the MTp levels in indoor air were 9.1 μg m^− 3 (94 μg m^− 3) for LMN, 2.6 μg m^− 3 (13 μg m^− 3) for αPN, and < 1.0 μg m^− 3 (3.2 μg m^− 3) for CRN. None of the day care centers exceeded the German health precaution or hazard guide value. In spite of the low MTp air exposure, the urine analyses revealed an exposure to the three monoterpenes in almost all children. The median levels of MTp metabolites in urine were 0.11 mg L^− 1 for LMN-8,9-OH, 0.10 mg L^− 1 for LMN-1,2-OH, 49 μg L^− 1 for PA, 2.9 μg L^− 1 for POH, 5.2 μg L^− 1 for tCAR, and 4.1 μg L^− 1 for cCAR (LMN metabolites), 7.2 μg L^− 1 for MYR, 19 μg L^− 1 for tVER, and 19 μg L^− 1 for cVER (αPN metabolites), as well as 8.2 μg L^− 1 for CRN-10-COOH (CRN metabolite). Statistically significant and strong correlations among the urinary metabolites of each MTp were found. Moreover, statistical associations between LMN metabolites and the LMN indoor air levels were revealed. However, the weakness of the associations indicates a considerable impact of other MTp sources, e.g. diet and consumer products, on the internal exposure.     

Radium dial watches,a potentially hazardous legacy?

This study re-examines the risk to health from radium (²²⁶Ra) dial watches. Ambient dose equivalent rates have been measured for fifteen pocket watches giving results of up to 30 μSv h^− 1 at a distance of 2 cm taken with a series 1000 mini-rad from the front face (arithmetic mean ambient dose equivalent for pocket watches being 13.2 μSv h^− 1). A pocket compass gave rise to a similar ambient dose equivalent rate, of 20 μSv h^− 1, to the pocket watches, with its cover open. Eighteen wristwatches have also been assessed, but their dose rates are generally much lower (the arithmetic mean being 3.0 μSv h^− 1), although the highest ambient dose equivalent rate noted was 20 μSv h^− 1. A phantom experiment using a TLD suggested an effective dose equivalent of 2.2 mSv/y from a 1 μCi (37 kBq) radium dial worn for 16 h/day throughout the year (dose rate 0.375 μSv h^− 1). For this condition we estimated maximum skin dose for our pocket watches as 16 mSv per year, with effective doses of 5.1 mSv and 1.169 mSv when worn in vest and trouser pockets respectively. This assumes exposure from the back of the watch which is generally around 60–67% of that from the front. The maximum skin dose from a wristwatch was 14 mSv, with 4.2 mSv effective dose in vest pocket. Radium (²²⁶Ra) decays to the radioactive gas radon (²²²Rn), and atmospheric radon concentration measurements taken around a pocket watch in a small sealed glass sphere recorded 18,728 Bq m^− 3. All watches were placed in a room with a RAD7 real-time radon detector. Radon concentration average was 259 ± 9 Bq m^− 3 over 16 h, compared to background average over 24 h of 1.02 Bq m^− 3. Over 6 weeks highs of the order of 2000 Bq m^− 3 were routinely recorded when the heating/ventilation system in the room was operating at reduced rates, peaking at over 3000 Bq m^− 3 on several occasions. Estimates of the activity of ²²⁶Ra in the watches ranged from 0.063 to 1.063 μCi (2.31 to 39.31 kBq) for pocket watches and from 0.013 to 0.875 μCi (0.46 to 32.38 kBq) for wrist watches. The risk from old watches containing radium appears to have been largely forgotten today. This paper indicates a health risk, particular to collectors, but with knowledge and appropriate precautions the potential risks can be reduced.     

Determination of heavy metals in indoor dust from Istanbul,Turkey: Estimation of the health risk

Levels of eight potentially toxic heavy metals in indoor dust from homes and offices in Istanbul were investigated. The concentrations of heavy metals in indoor dust from homes + office ranged from 62 to 1800 μg g^− 1 for Cu, 3–200 μg g^− 1 for Pb, 0.4–20 μg g^− 1 for Cd, 210–2800 μg g^− 1 for Zn, 2.8–460 μg g^− 1 for Cr, 8–1300 μg g^− 1 for Mn, 2.4–25 μg g^− 1 for Co, 120–2600 μg g^− 1 for Ni. Results of the study were comparable to other studies conducted on indoor dust and street dust from a variety of cities globally. Considering only ingestion + inhalation, the carcinogenic risk level of Cr for adults and children (3.7 × 10^− 5 and 2.7 × 10^− 5) in Istanbul was in the range of EPA's safe limits (1 × 10^− 6 and 1 × 10^− 4), indicating that cancer risk of Cr due to exposure to indoor dust in Istanbul can be acceptable. According to calculated Hazard Quotient (HQ), for non-cancer effects, the ingestion of indoor dust appears to be the major route of exposure to the indoor dust that results in a higher risk for heavy metals, followed by dermal contact and inhalation pathways. However, compared to ingestion and dermal contact exposure, exposure through inhalation is almost negligible. Hazard Index (HI) values for all studied elements were lower than safe limit of 1 and this result suggested that none of the population groups would likely to experience potential health risk due to exposure to heavy metals from indoor dust in the study area.     

Acute respiratory response to traffic-related air pollution during physical activity performance

BackgroundPhysical activity (PA) has beneficial, whereas exposure to traffic related air pollution (TRAP) has adverse, respiratory effects. Few studies, however, have examined if the acute effects of TRAP upon respiratory outcomes are modified depending on the level of PA.ObjectivesThe aim of our study was to disentangle acute effects of TRAP and PA upon respiratory outcomes and assess the impact of participants TRAP pre-exposure.MethodsWe conducted a real-world crossover study with repeated measures of 30 healthy adults. Participants completed four 2-h exposure scenarios that included either rest or intermittent exercise in high- and low-traffic environments. Measures of respiratory function were collected at three time points. Pre-exposure to TRAP was ascertained from land-use-modeled address-attributed values. Mixed-effects models were used to estimate the impact of TRAP and PA on respiratory measures as well as potential effect modifications.ResultsWe found that PA was associated with a statistically significant increases of FEV₁ (48.5 mL, p = 0.02), FEV₁/FVC (0.64%, p = 0.005) and FEF_25–75% (97.8 mL, p = 0.02). An increase in exposure to one unit (1 μg/m³) of PM_coarse was associated with a decrease in FEV₁ (− 1.31 mL, p = 0.02) and FVC (− 1.71 mL, p = 0.01), respectively. On the other hand, for an otherwise equivalent exposure an increase of PA by one unit (1%Heart rate max) was found to reduce the immediate negative effects of particulate matter (PM) upon PEF (PM_2.5, 0.02 L/min, p = 0.047; PM₁₀, 0.02 L/min p = 0.02; PM_coarse, 0.03 L/min, p = 0.02) and the several hours delayed negative effects of PM upon FVC (PM_coarse, 0.11 mL, p = 0.02). The negative impact of exposure to TRAP constituents on FEV₁/FVC and PEF was attenuated in those participants with higher TRAP pre-exposure levels.ConclusionsOur results suggest that associations between various pollutant exposures and respiratory measures are modified by the level of PA during exposure and TRAP pre-exposure of participants.     

Boron exposure through drinking water during pregnancy and birth size

BackgroundBoron is a metalloid found at highly varying concentrations in soil and water. Experimental data indicate that boron is a developmental toxicant, but the few human toxicity data available concern mostly male reproduction.ObjectivesTo evaluate potential effects of boron exposure through drinking water on pregnancy outcomes.MethodsIn a mother-child cohort in northern Argentina (n = 194), 1–3 samples of serum, whole blood and urine were collected per woman during pregnancy and analyzed for boron and other elements to which exposure occurred, using inductively coupled plasma mass spectrometry. Infant weight, length and head circumference were measured at birth.ResultsDrinking water boron ranged 377–10,929 μg/L. The serum boron concentrations during pregnancy ranged 0.73–605 μg/L (median 133 μg/L) and correlated strongly with whole-blood and urinary boron, and, to a lesser extent, with water boron. In multivariable-adjusted linear spline regression analysis (non-linear association), we found that serum boron concentrations above 80 μg/L were inversely associated with birth length (B − 0.69 cm, 95% CI − 1.4; − 0.024, p = 0.043, per 100 μg/L increase in serum boron). The impact of boron appeared stronger when we restricted the exposure to the third trimester, when the serum boron concentrations were the highest (0.73–447 μg/L). An increase in serum boron of 100 μg/L in the third trimester corresponded to 0.9 cm shorter and 120 g lighter newborns (p = 0.001 and 0.021, respectively).ConclusionsConsidering that elevated boron concentrations in drinking water are common in many areas of the world, although more screening is warranted, our novel findings warrant additional research on early-life exposure in other populations.     

Body burden of metals and persistent organic pollutants among Inuit in the Canadian Arctic

Inuit living in the Arctic are exposed to elevated levels of environmental contaminants primarily due to long-range atmospheric transport. Blood sampling and contaminant biomonitoring was conducted as part of the International Polar Year Inuit Health Survey in 2007-2008. The body burden of metals (e.g. Cd, Pb) and persistent organic pollutants (e.g. PCBs, DDT & DDE, toxaphene, chlordane, PBDEs) were measured for Inuit participants (n = 2172) from 36 communities in Nunavut, Nunatsiavut, and the Inuvialuit Settlement Region, in Canada. The geometric mean of blood concentrations for Cd, Pb, PCBs, DDE & DDT, toxaphene, and chlordane were higher than those in the Canadian general population. A total of 9% of study participants exceeded the intervention guideline of 100 μg L^− 1 for Pb, 11% of participants exceeded the trigger guideline of 5 μg L^− 1 for Cd, and 1% exceeded the intervention guideline of 100 μg L^− 1 for PCBs. Also, 3% of women of child-bearing age exceeded blood Pb of 100 μg L^− 1 while 28% of women of child-bearing age exceeded 5 μg L^− 1 of PCBs. This work showed that most Inuit Health Survey participants were below blood contaminant guidelines set by Health Canada but that metal and POP body burdens commonly exceed exposures observed in the general population of Canada.     

Elevated childhood exposure to arsenic despite reduced drinking water concentrations — A longitudinal cohort study in rural Bangladesh

ObjectivesThe aim of this study was to evaluate the massive efforts to lower water arsenic concentrations in Bangladesh.MethodsIn our large mother–child cohort in rural Matlab, we measured the arsenic concentrations (and other elements) in drinking water and evaluated the actual exposure (urinary arsenic), from early gestation to 10 years of age (n = 1017).ResultsMedian drinking water arsenic decreased from 23 (2002–2003) to < 2 μg/L (2013), and the fraction of wells exceeding the national standard (50 μg/L) decreased from 58 to 27%. Still, some children had higher water arsenic at 10 years than earlier. Installation of deeper wells (> 50 m) explained much of the lower water arsenic concentrations, but increased the manganese concentrations. The highest manganese concentrations (~ 900 μg/L) appeared in 50–100 m wells. Low arsenic and manganese concentrations (17% of the children) occurred mainly in > 100 m wells. The decrease in urinary arsenic concentrations over time was less apparent, from 82 to 58 μg/L, indicating remaining sources of exposure, probably through food (mean 133 μg/kg in rice).ConclusionDespite decreased water arsenic concentrations in rural Bangladesh, the children still have elevated exposure, largely from food. Considering the known risks of severe health effects in children, additional mitigation strategies are needed.     

Priority and emerging flame retardants in rivers: Occurrence in water and sediment,Daphnia magna toxicity and risk assessment

The occurrence, partitioning and risk of eight polybrominated diphenyl ethers (PBDEs), nine new brominated (NBFRs) and ten organophosphorus flame retardants (OPFRs) were evaluated in three Spanish rivers suffering different anthropogenic pressures (Nalón, Arga and Besòs). OPFRs were ubiquitous contaminants in water (ΣOPFRs ranging from 0.0076 to 7.2 μg L^− 1) and sediments (ΣOPFRs ranging 3.8 to 824 μg kg^− 1). Brominated flame retardants were not detected in waters, whereas ΣPBDEs ranged from 88 to 812 μg kg^− 1 and decabromodiphenyl ethane (DBDPE) reached 435 μg kg^− 1 in sediments from the River Besòs, the most impacted river. The occurrence of flame retardants in river water and sediment was clearly associated with human activities, since the highest levels occurred near urban and industrial zones and after wastewater treatment plants discharge. Daphnia magna toxicity was carried out for OPFRs, the most ubiquitous flame retardants, considering individual compounds and mixtures. Toxicity of nine tested OPFRs differed largely among compounds, with EC₅₀ values ranging over three magnitude orders (0.31–381 mg L^− 1). Results evidenced that these compounds act by non-polar narcosis, since their toxicity was proportional to their lipophilicity (K_ow). Furthermore, their joint toxicity was additive, which means that single and joint toxicity can be predicted knowing their concentration levels in water using quantitative structure activity relationships (QSARs) and predictive mixture models. Based on these results, a risk assessment considering joint effect was performed calculating and summing risk quotients (RQs) for the water and sediment samples. No significant risk to D. magna (ΣRQs < 1) was observed for any of the monitored rivers.     

Measurement and health risk assessment of PM2.5, flame retardants,carbonyls and black carbon in indoor and outdoor air in kindergartens in Hong Kong

Indoor air pollution is closely related to children's health. Polybrominated diphenyl ethers (PBDEs) and dechlorane plus (DP) transmitted through indoor PM_2.5 and dust, along with carbonyl compounds and black carbon (BC) aerosol were analysed in five Hong Kong kindergartens. The results showed that 60% of the median PM_2.5 levels (1.3 × 10¹ to 2.9 × 10¹ μg/m³ for indoor; 9.5 to 8.8 × 10¹ μg/m³ for outdoor) in the five kindergartens were higher than the guidelines set by the World Health Organization (2.5 × 10¹ μg/m³). Indoor PM_2.5 mass concentrations were correlated with outdoor PM_2.5 in four of the kindergartens. The PBDEs (0.10–0.64 ng/m³ in PM_2.5; 0.30–2.0 × 10² ng/g in dust) and DP (0.05–0.10 ng/m³ in PM_2.5; 1.3–8.7 ng/g in dust) were detected in 100% of the PM_2.5 and dust samples. Fire retardant levels in the air were not correlated with the levels of dust in this study. The median BC concentrations varied by > 7-fold from 8.8 × 10² ng/m^− 3 to 6.7 × 10³ ng/m^− 3 and cooking events might have caused BC concentrations to rise both indoors and outdoors. The total concentrations of 16 carbonyls ranged from 4.7 × 10¹ μg/m³ to 9.3 × 10¹ μg/m³ indoors and from 1.9 × 10¹ μg/m³ to 4.3 × 10¹ μg/m³ outdoors, whilst formaldehyde was the most abundant air carbonyl. Indoor carbonyl concentrations were correlated with outdoor carbonyls in three kindergartens. The health risk assessment showed that hazard indexes (HIs) HIs of non-cancer risks from PBDEs and DPs were all lower than 0.08, whilst non-cancer HIs of carbonyl compounds ranged from 0.77 to 1.85 indoors and from 0.50 to 0.97 outdoors. The human intake of PBDEs and DP through inhalation of PM_2.5 accounted for 78% to 92% of the total intake. The cancer hazard quotients (HQs) of formaldehyde ranged from 4.5E − 05 to 2.1E − 04 indoors and from 1.9E − 05 to 6.2E − 05 outdoors. In general, the indoor air pollution in the five Hong Kong kindergartens might present adverse effects to children, although different schools showed distinct pollution levels, so indoor air quality might be improved through artificial measures. The data will be useful to developing a feasible management protocol for indoor environments.     

Novel exposure biomarkers of N,N-diethyl-m-toluamide (DEET): Data from the 2007–2010 National Health and Nutrition Examination Survey

BackgroundN,N-diethyl-m-toluamide (DEET) is a widely used insect repellent in the United States.ObjectivesTo assess exposure to DEET in a representative sample of persons 6 years and older in the U.S. general population from the 2007–2010 National Health and Nutrition Examination Survey.MethodsWe analyzed 5348 urine samples by using online solid-phase extraction coupled to isotope dilution-high-performance liquid chromatography-tandem mass spectrometry. We used regression models to examine associations of various demographic parameters with urinary concentrations of DEET biomarkers.ResultsWe detected DEET in ~ 3% of samples and at concentration ranges (> 0.08 μg/L–45.1 μg/L) much lower than those of 3-(diethylcarbamoyl)benzoic acid (DCBA) (> 0.48 μg/L–30,400 μg/L) and N,N-diethyl-3-hydroxymethylbenzamide (DHMB) (> 0.09 μg/L–332 μg/L). DCBA was the most frequently detected metabolite (~ 84%). Regardless of survey cycle and the person's race/ethnicity or income, adjusted geometric mean concentrations of DCBA were higher in May–Sep than in Oct–Apr. Furthermore, non-Hispanic whites in the warm season were more likely than in the colder months [adjusted odds ratio (OR) = 10.83; 95% confidence interval (CI), 3.28–35.79] and more likely than non-Hispanic blacks (OR = 3.45; 95% CI, 1.51–7.87) to have DCBA concentrations above the 95th percentile.ConclusionsThe general U.S. population, including school-age children, is exposed to DEET. However, reliance on DEET as the sole urinary biomarker would likely underestimate the prevalence of exposure. Instead, oxidative metabolites of DEET are the most adequate exposure biomarkers. Differences by season of the year based on demographic variables including race/ethnicity likely reflect different lifestyle uses of DEET-containing products.     

Cleaning-induced arsenic mobilization and chromium oxidation from CCA-wood deck: Potential risk to children

Concern about children's exposure to arsenic (As) from wood treated with chromated-copper-arsenate (CCA) led to its withdrawal from residential use in 2004. However, due to its effectiveness, millions of American homes still have CCA-wood decks on which children play. This study evaluated the effects of three deck-cleaning methods on formation of dislodgeable As and hexavalent chromium (CrVI) on CCA-wood surfaces and in leachate. Initial wipes from CCA-wood wetted with water showed 3–4 times more dislodgeable As than on dry wood. After cleaning with a bleach solution, 9.8–40.3 μg/100 cm² of CrVI was found on the wood surface, with up to 170 μg/L CrVI in the leachate. Depending on the cleaning method, 699–2473 mg of As would be released into the environment from cleaning a 18.6-m²-deck. Estimated As doses in children aged 1–6 after 1 h of playing on a wet CCA-wood deck were 0.25–0.41 μg/kg. This is the first study to identify increased dislodgeable As on wet CCA-wood and to evaluate dislodgeable CrVI after bleach application. Our data suggest that As and CrVI in 25-year old CCA-wood still show exposure risks for children and potential for soil contamination.     

The contributions to long-term health-relevant particulate matter at the UK EMEP supersites between 2010 and 2013: Quantifying the mitigation challenge

Human health burdens associated with long-term exposure to particulate matter (PM) are substantial. The metrics currently recommended by the World Health Organization for quantification of long-term health-relevant PM are the annual average PM₁₀ and PM_2.5 mass concentrations, with no low concentration threshold. However, within an annual average, there is substantial variation in the composition of PM associated with different sources. To inform effective mitigation strategies, therefore, it is necessary to quantify the conditions that contribute to annual average PM₁₀ and PM_2.5 (rather than just short-term episodic concentrations). PM₁₀, PM_2.5, and speciated water-soluble inorganic, carbonaceous, heavy metal and polycyclic aromatic hydrocarbon components are concurrently measured at the two UK European Monitoring and Evaluation Programme (EMEP) ‘supersites’ at Harwell (SE England) and Auchencorth Moss (SE Scotland). In this work, statistical analyses of these measurements are integrated with air-mass back trajectory data to characterise the ‘chemical climate’ associated with the long-term health-relevant PM metrics at these sites. Specifically, the contributions from different PM concentrations, months, components and geographic regions are detailed. The analyses at these sites provide policy-relevant conclusions on mitigation of (i) long-term health-relevant PM in the spatial domain for which these sites are representative, and (ii) the contribution of regional background PM to long-term health-relevant PM.At Harwell the mean (± 1 sd) 2010–2013 annual average concentrations were PM₁₀ = 16.4 ± 1.4 μg m^− 3 and PM_2.5 = 11.9 ± 1.1 μg m^− 3 and at Auchencorth PM₁₀ = 7.4 ± 0.4 μg m^− 3 and PM_2.5 = 4.1 ± 0.2 μg m^− 3. The chemical climate state at each site showed that frequent, moderate hourly PM₁₀ and PM_2.5 concentrations (defined as approximately 5–15 μg m^− 3 for PM₁₀ and PM_2.5 at Harwell and 5–10 μg m^− 3 for PM₁₀ at Auchencorth) determined the magnitude of annual average PM₁₀ and PM_2.5 to a greater extent than the relatively infrequent high, episodic PM₁₀ and PM_2.5 concentrations. These moderate PM₁₀ and PM_2.5 concentrations were derived across the range of chemical components, seasons and air-mass pathways, in contrast to the highest PM concentrations which tended to associate with specific conditions. For example, the largest contribution to moderate PM₁₀ and PM_2.5 concentrations – the secondary inorganic aerosol components, specifically NO₃⁻ – were accumulated during the arrival of trajectories traversing the spectrum of marine, UK, and continental Europe areas. Mitigation of the long-term health-relevant PM impact in the regions characterised by these two sites requires multilateral action, across species (and hence source sectors), both nationally and internationally; there is no dominant determinant of the long-term PM metrics to target.     

The bioavailability of selenium and risk assessment for human selenium poisoning in high-Se areas,China

Enshi prefecture of Hubei Province is well known for human selenium (Se) poisoning in the early 1960s in China. Sporadic cases of Se poisoning in livestocks are still being found. In this study, Se levels in water, cropland soils and various crops from high-Se areas of Enshi were measured to investigate the distribution and bioavailability of Se in the environments, as well as probable daily intake (PDI) of Se for local residents. The total Se in surface water ranged from 2.0 to 519.3 μg/L with a geometric mean of 46.0 ± 127.8 μg/L (n = 48), 70.5–99.5% of which was present in the form of Se(VI). The soil Se concentration varied from 2.89 to 87.3 μg/g with a geometric mean of 9.36 ± 18.6 μg/g (n = 45), and most of Se was associated with organic matter (OM-Se). The total Se in rice, corn, and vegetable samples were 2.11 ± 2.87 μg/g (n = 21), 3.76 ± 11.6 μg/g (n = 16), and 2.09 ± 3.38 μg/g (n = 25), respectively. Stream water Se is likely leached from carbonaceous shale and mine wastes, leading to Se accumulation in paddy soils. OM-Se may play an important role in Se uptake by rice plant in high-Se area of Enshi.The PDI of Se is approximately 2144 μg/day, and Se concentration in blood is estimated at about 3248 μg/L, posing a potential chronic Se poisoning risk to local residents. Cereal consumption (48.5%) makes a great contribution to human daily Se intake, followed by vegetables (36.6%), meats (8.5%), and drinking water (6.4%). However, when assessing health risk on human in high-Se areas, the contribution of drinking water to daily Se intake cannot be ignored due to high Se content and dominant Se(VI) species. Local inhabitants should be advised not to grow crops in high-Se lands or irrigate using high-Se water. If possible, they should drink pipe water and consume foods mixed with those from outside the high-Se areas.     

Environmental exposure to lithium during pregnancy and fetal size: A longitudinal study in the Argentinean Andes

BackgroundLithium, used for treating bipolar disease, crosses freely the placenta and is classified as teratogenic. It is unclear to what extent environmental lithium exposure may affect fetal growth and development.ObjectivesTo elucidate potential effects of lithium exposure through drinking water during pregnancy on fetal size.MethodsWe developed a prospective population-based mother–child cohort (N = 194) in an area with highly varying drinking water lithium concentrations (5-1600 μg/L) in northern Argentinean Andes. Blood and urinary lithium concentrations (sampled repeatedly during pregnancy) were measured using inductively coupled plasma mass spectrometry. We measured fetal size by ultrasound in second and third trimesters, and weight, length and head circumference at birth. Multivariable models were used to examine associations between lithium exposure (continuous and in tertiles) and fetal size measures.ResultsLithium in maternal blood (median 25; range 1.9–145 μg/L) and urine (1645; 105–4600 μg/L) was inversely associated (apparently linearly) with all fetal measures (body, head and femur) in the second trimester, and with birth length (β − 0.53 cm per 25 μg/L increase in blood lithium, 95%CI − 1.0; − 0.052). An increase of 100 μg/L in blood was associated with 2 cm shorter newborns (about one standard deviation).ConclusionsLithium exposure through drinking water was associated with impaired fetal size and this seemed to be initiated in early gestation. Further studies are warranted to confirm causality and to understand the mechanisms. If confirmed, these findings have public health relevance and emphasize the need for more data on lithium concentrations in drinking water, including bottled water.     

Can car air filters be useful as a sampling medium for air pollution monitoring purposes?

Urban air quality and real human exposure to chemical environmental stressors is an issue of high scientific and political interest. In an effort to find innovative and inexpensive means for air quality monitoring, the ability of car engine air filters (CAFs) to act as efficient samplers collecting street level air, to which people are exposed to, was tested. In particular, in the case of taxis, air filters are replaced after regular distances, the itineraries are almost exclusively urban, cruising mode is similar and, thus, knowledge of the air flow can provide with an integrated city air sample. The present pilot study focused on polycyclic aromatic hydrocarbons (PAHs), the most important category of organic pollutants associated with traffic emissions. Concentrations of ΣPAHs in CAFs ranged between 650 and 2900 μg CAF^− 1, with benzo[b]fluoranthene, benzo[k]fluoranthene and indeno[123-cd]pyrene being the most abundant PAHs. Benzo[a]pyrene (BaP) ranged between 110 and 250 μg CAF^− 1, accounting regularly for 5–15% of the total carcinogenic PAHs. The CAF PAH loads were used to derive road-level atmospheric PAH concentrations from a standard formula relating to the CAF air flow. Important parameters/assumptions for these estimates are the cruising speed and the exposure duration of each CAF. Based on information obtained from the garage experts, an average ‘sampled air volume’ of 48,750 m³ per CAF was estimated, with uncertainty in this calculation estimated to be about a factor of 4 between the two extreme scenarios. Based on this air volume, ΣPAHs ranged between 13 and 56 ng m^− 3 and BaP between 2.1 and 5.0 ng m^− 3, suggesting that in-traffic BaP concentrations can be many times higher than the limit values set by the UK (0.25 ng m^− 3) and the European Union (1.0 ng m^− 3), or from active sampling stations normally cited on building roof tops or far from city centres.Notwithstanding the limitations of this approach, the very low cost, the continuous availability of very high amounts of “sample”, and the “retroactivity” render it very useful and complementary to existing passive sampling techniques. This approach yields estimated air concentrations that reflect the pollutant concentrations to which taxi drivers, pedestrians, cyclists and road-related professionals are exposed.     

An interlaboratory comparison of nanosilver characterisation and hazard identification: Harmonising techniques for high quality data

Within the FP7 EU project NanoValid a consortium of six partners jointly investigated the hazard of silver nanoparticles (AgNPs) paying special attention to methodical aspects that are important for providing high-quality ecotoxicity data. Laboratories were supplied with the same original stock dispersion of AgNPs. All partners applied a harmonised procedure for storage and preparation of toxicity test suspensions. Altogether ten different toxicity assays with a range of environmentally relevant test species from different trophic levels were conducted in parallel to AgNP characterisation in the respective test media. The paper presents a comprehensive dataset of toxicity values and AgNP characteristics like hydrodynamic sizes of AgNP agglomerates and the share (%) of Ag⁺-species (the concentration of Ag⁺-species in relation to the total measured concentration of Ag). The studied AgNP preparation (20.4 ± 6.8 nm primary size, mean total Ag concentration 41.14 mg/L, 46–68% of soluble Ag⁺-species in stock, 123.8 ± 12.2 nm mean z-average value in dH₂O) showed extreme toxicity to crustaceans Daphnia magna, algae Pseudokirchneriella subcapitata and zebrafish Danio rerio embryos (EC50 < 0.01 mg total Ag/L), was very toxic in the in vitro assay with rainbow trout Oncorhynchus mykiss gut cells (EC50: 0.01–1 mg total Ag/L); toxic to bacteria Vibrio fischeri, protozoa Tetrahymena thermophila (EC50: 1–10 mg total Ag/L) and harmful to marine crustaceans Artemia franciscana (EC50: 10–100 mg total Ag/L). Along with AgNPs, also the toxicity of AgNO₃ was analyzed. The toxicity data revealed the same hazard ranking for AgNPs and AgNO₃ (i.e. the EC50 values were in the same order of magnitude) proving the importance of soluble Ag⁺-species analysis for predicting the hazard of AgNPs. The study clearly points to the need for harmonised procedures for the characterisation of NMs. Harmonised procedures should consider: (i) measuring the AgNP properties like hydrodynamic size and metal ions species in each toxicity test medium at a range of concentrations, and (ii) including soluble metal salt control both in toxicity testing as well as in Ag⁺-species measurements. The present study is among the first nanomaterial interlaboratory comparison studies with the aim to improve the hazard identification testing protocols.     

Risks associated with the transfer of toxic organo-metallic mercury from soils into the terrestrial feed chain

Although the transfer of organo-metallic mercury (OrgHg) in aquatic food webs has long been studied, it has only been recently recognized that there is also accumulation in terrestrial systems. There is still however little information about the exposure of grazing animals to OrgHg from soils and feed as well as on risks of exposure to animal and humans.In this study we collected 78 soil samples and 40 plant samples (Lolium perenne and Brassica juncea) from agricultural fields near a contaminated industrial area and evaluated the soil-to-plant transfer of Hg as well as subsequent trophic transfer. Inorganic Hg (IHg) concentrations ranged from 0.080 to 210 mg kg^− 1 d.w. in soils, from 0.010 to 84 mg kg^− 1 d.w. in roots and from 0.020 to 6.9 mg kg^− 1 d.w. in shoots. OrgHg concentrations in soils varied between 0.20 and 130 μg kg^− 1 d.w. representing on average 0.13% of the total Hg (THg). In root and shoot samples OrgHg comprised on average 0.58% (roots) and 0.66% (shoots) of THg. Average bioaccumulation factors (BAFs) for OrgHg in relation to soil concentrations were 3.3 (for roots) and 1.5 (for shoots).The daily intake (DI) of THg in 33 sampling sites exceeded the acceptable daily intake (ADI) of THg of both cows (ADI = 1.4 mg d^− 1) and sheep (ADI = 0.28 mg d^− 1), in view of food safety associated with THg in animal kidneys. Estimated DI of OrgHg for grazing animals were up to 220 μg d^− 1 (for cows) and up to 33 μg d^− 1 (for sheep).This study suggested that solely monitoring the levels of THg in soils and feed may not allow to adequately taking into account accumulation of OrgHg in feed crops and properly address risks associated with OrgHg exposure for animals and humans. Hence, the inclusion of limits for OrgHg in feed quality and food safety legislation is advised.