Neonicotinoid insecticides (NNIs) are extensively used insecticides worldwide, yet the data on NNIs residues in the Yangtze River, China is scarce. Occurrence and distribution of six NNIs and a ...metabolite (desmethyl-acetamiprid) in surface water were investigated in the central Yangtze River, China at 20 sites from March to July and September 2015. Acetamiprid (ACE), imidacloprid (IMI) and thiamethoxam (THM) were the most frequently detected NNIs and IMI had a highest median concentration of 4.37 ng/L, followed by ACE (2.50 ng/L), THM (1.10 ng/L), nitenpyram (NTP; 0.34 ng/L), clothianidin (CLO; 0.10 ng/L), and thiacloprid (THCP; 0.02 ng/L). Significantly higher concentrations and detection frequencies of NNIs were observed in the summer than in the spring, which may be explained by the heavier precipitation in summer. Spatial variation with higher levels among the lower sites than the upper sites may be related with the agriculture land use. NNI contamination presented a low risk to aquatic life according to the risk quotient method, while IMI had potential risk to aquatic life according to the threshold of IMI (8.3 ng/L) in freshwater recommended in Netherland. Using the relative potency factors method for chronic cumulative risk assessment for NNIs, potential exposure to NNIs through water ingestion are three orders of magnitude lower than the recommended relative chronic reference dose. Ongoing environmental monitoring of NNIs is needed due to the increase use of NNIs in China.
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•Six typical NNIs were found in the central Yangtze River, and ACE, IMI and THM were the highest.•DM-ACE was found in surface water for the first time.•Higher NNIs levels were found in the summer than in the spring, with the highest observed in June.•Spatial variations of neonicotinoid contamination were observed.•Potential risk of NNIs to aquatic ecosystem and human were assessed.
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•DN-IMI, IMI-olefin, and DM-ACE had high detection frequencies.•Fair-to-good inter-day reliability was found for DN-IMI, IMI-olefin, and DM-ACE.•DN-IMI and IMI-olefin were identified ...in human urine for the first time.•Higher urinary NNI concentrations were found in urban areas and in autumn.
While neonicotinoid insecticides (NNIs) have been widely used worldwide, limited studies have measured specific metabolites of imidacloprid (IMI, the most commonly used NNI) in human urine. To better understand human exposure to NNIs, 10 parent compounds, and 6 of their metabolites were analyzed in 408 urine samples collected from 129 healthy adults in Wuhan, Central China, during autumn and winter of 2018. These specimens included repeated urine samples taken in 3 d from 75 volunteers. The urinary concentrations of desnitro-imidacloprid (DN-IMI), imidacloprid-olefin (IMI-olefin), and desmethyl-acetamiprid (DM-ACE) were higher (4–40 times) than those of their parent compounds (IMI and acetamiprid, ACE). DN-IMI and IMI-olefin accounted for 92% of the urinary Σ3IMI (the sum of IMI and its specific metabolites measured). Positive correlations (r) were observed between DN-IMI and IMI (0.50), IMI-olefin and IMI (0.75), and DM-ACE and ACE (0.53). Good to excellent inter-day reliabilities (unadjusted intraclass correlation coefficients) were observed for IMI-olefin (0.61) and DM-ACE (0.81), while moderate inter-day reliability was observed for DN-IMI (0.43). The urinary NNI concentrations were significantly higher in autumn than in winter, and higher in urban areas than in rural areas, while no significant gender or age-related differences were observed. To our knowledge, this is the first report on DN-IMI and IMI-olefin in human urine.
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•Benzothiazoles were determined in 81 indoor air samples.•Benzothiazole concentrations ranged 4.36–2229ng/m3 with the highest in cars.•Inhalation exposure to benzothiazoles ranged ...from 5.13 to 18.3ng/kg bw/d.•Contribution of inhalation to total benzothiazole intake was approximately 10%.
Benzothiazole and its derivatives (collectively referred to BTHs) are used widely in many consumer (e.g., textiles) and industrial (e.g., rubber) products. Very little is known about the occurrence of BTHs in indoor air and the inhalation exposure of humans to these substances. In this study, 81 indoor air samples collected from various locations in Albany, New York, USA, in 2014 were analyzed for BTHs by high-performance liquid chromatography-tandem mass spectrometry (HPLC–MS/MS). BTHs were found in all indoor air samples, and the overall concentrations in bulk air (vapor plus particulate phases) were in the range of 4.36–2229ng/m3 (geometric mean: 32.7ng/m3). The highest concentrations (geometric mean: 148ng/m3) were found in automobiles, followed by homes (49.5)>automobile garages (46.0)>public places, e.g., shopping malls (24.2)>barbershops (18.9) >offices (18.8)>laboratories (15.1). The estimated geometric mean daily intake (EDI) of BTHs for infants, toddlers, children, teenagers, and adults through indoor air inhalation from homes was 27.7, 26.3, 17.9, 10.5, and 7.77ng/kg-bw/day, respectively. The estimated contribution of indoor air to total BTHs intake was approximately 10%. This is the first study on the occurrence of BTHs in indoor air.
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•Concentrations of 19 urinary VOC metabolites decreased as pregnancy proceeded.•Exposure determinants such as education level, and sampling season were identified.•GAMA was a dominant ...contributor in association with oxidative stress biomarkers of DNA and RNA.•MU was a dominant contributor in association with a biomarker of lipid peroxidation.
Volatile organic compounds (VOCs) are a group of pollutants pervasive in daily life with identified adverse health effects. However, no study has investigated the variability in VOC metabolites during pregnancy and their relationships with oxidative stress biomarkers in pregnant women. In the present study, the variability of 21 selected VOC metabolites was examined and their relationships with three selected oxidative stress biomarkers measured in spot urine samples at three trimesters of 1094 pregnant women were analyzed. Nineteen VOC metabolites were ubiquitous in the urine samples with detection rates ranging from 75.9% to 100%. Monohydroxybutenyl mercapturic acid (MHBMA) and s-phenyl mercapturic acid (PMA) had detection rates lower than 1.00%. Intraclass correlation coefficients (ICCs) of the detected analytes at three trimesters ranged 0.07–0.24, and the concentrations were highest in the first trimester. Higher concentrations of some VOC metabolites were related with participant characteristics including higher pre-pregnancy body mass index (BMI), lower education level, unemployment during pregnancy, multiparity, and sampling season of summer or winter. In repeated cross-sectional analyses, interquartile range (IQR) increases in the 19 detected VOC metabolites were positively related with 8-hydroxy-2′-deoxyguanosine (8-OHdG), 8-hydroxyguanosine (8-OHG), and 4-hydroxy nonenal mercapturic acid (HNEMA) with the estimates ranging from 9.00% to 204%. The mixture effect of the VOC metabolites on the oxidative stress biomarkers was further assessed using weighted quantile sum regression (WQS) models and the results showed that the WQS index of VOC metabolite mixture was significantly associated with 8-OHdG (β: 0.37, 0,32, and 0.39 at the 1st, 2nd, and 3rd trimester, respectively), 8-OHG (0.38, 0.32, and 0.39) and HNEMA (1.21, 1.08, and 1.10). Glycidamide mercapturic acid (GAMA), and trans,trans-muconic acid (MU) were the strongest contributors of the mixture effect on 8-OHdG, 8-OHG, and HNEMA, respectively. Overall, urinary concentrations of the VOC metabolites during pregnancy were strongly associated with the oxidative stress biomarkers.
Phthalates are a family of endocrine disruptors with short elimination half-lives in the human body. To date, few epidemiological studies have examined repeated measures of maternal urinary ...phthalates and the combined effects of prenatal exposure to multiple phthalates on children's neurocognitive development.
We aimed to investigate the association between children's neurocognitive development at 2 years of age and prenatal phthalate exposure, as assessed by repeated measurements during pregnancy, and to further examine the effects of co-exposure to multiple phthalates using cumulative risk assessment.
Within a prenatal cohort in Wuhan, China, we measured five high-molecular-weight (HMW) phthalates and three low-molecular-weight (LMW) phthalate metabolites' concentrations in three urine samples collected in the 1st, 2nd, and 3rd trimester of pregnancy from each mother. We assessed neurocognitive development by Bayley Scales of Infant and Toddler Development (BSID) at 2 years of age (n = 476) to obtain the children's mental development index (MDI) and psychomotor development index (PDI).
Higher exposure levels to LMW phthalates compared to HMW phthalates were observed in our population. Ln-transformed averaged concentration of mono-n-butyl phthalate (MnBP), a metabolite of the LMW phthalate di-n-butyl phthalate (DnBP) during pregnancy, was associated with decreased PDI scores in all children (β = −1.90, 95% CI: −3.43, −0.37). Similarly, the averaged sum concentration of ∑dibutyl phthalate (∑DBP) was associated with decreased PDI scores in all children (β = −1.89, 95% CI: −3.63, −0.15). A negative trend of association between exposure to HMW phthalates and PDI scores was observed in girls, while a positive association was found in boys. In cumulative risk assessment analyses, we consistently observed that the hazard quotient of DnBP (the parent compound of MnBP) was inversely associated with PDI scores in all children, whereas the hazard quotient of di-2-ethylhexyl phthalate (DEHP), an HMW phthalate, was positively associated with PDI scores in boys only.
This study is the first to use repeated measurement of maternal urinary phthalates in all three trimesters to assess prenatal exposure in relation to children's neurodevelopment. Our study suggested a negative association between prenatal exposure to MnBP and children's psychomotor development, and potentially sex-specific associations between HMW phthalates and neurocognitive development among boys and girls. These findings warrant further confirmation.
•We first evaluated the effect of repeated measurements of maternal urinary phthalates on child neurocognitive development.•Prenatal exposure to mono-n-butyl phthalate was negatively associated with children’s psychomotor development.•The sex-specific effect may exist between phthalates and neurocognitive development.
2,4-Dichlorophenoxyacetic acid (2,4-D) is a chlorophenoxy herbicide used worldwide. We describe a high-performance liquid chromatography (HPLC) method with UV detection for the determination of 2,4-D ...in female and male rat serum. This allows to observe the change of serum 2,4-D concentration in rats with time and its pharmacokinetics characteristics with a simple, rapid, optimized and validated method. The serum samples are pretreated and introduced into the HPLC system. The analytes are separated in a XDB-C18 column with a mobile phase of acetonitrile (solvent A) and 0.02 M ammonium acetate (containing 0.1% formic acid) (solvent B) using a gradient elution at a flow rate of 1.0 mL/min. The wavelength for UV detection was set at 230 nm. Calibration curve for 2,4-D was constructed over a range of 0.1-400 mg/L. The method was successfully applied to study the pharmacokinetics of 2,4-D in rats in this study. After oral administration of 300 mg/kg and 60 mg/kg 2,4-D, the mean Cmax values were 601.9 and 218.4 mg/L, the AUC0→∞ values were 23,722 and 4,127 mg×h/L and the clearance (Cl) were 1.10 and 0.02 L/(h×kg), respectively. The developed method was found to be specific, precise, reproducible and rapid.
Bentazone is a widely used post-emergence herbicide, while no data was available on its concentrations in tap water from China and in urine among the general population. It was determined in the ...source (Wuhan section of the Yangtze River watershed), treated, and tap water (
n
= 20, 20, and 170, respectively) in different seasons (2019) in Wuhan, central China. Also, urine samples (
n
= 38) collected from healthy adults in Wuhan (September 2020) were analyzed to characterize its urinary concentration. Bentazone was detected in all the source and treated water samples. Its concentrations in the source water in July were higher than those in February (median: 17.9 ng/L vs. 2.86 ng/L) (
p
< 0.05). It cannot be removed efficiently (27.8–27.9%) by conventional drinking water treatment using NaClO, but it can be efficiently removed by using chlorine dioxide or ozone combined with activated carbon. Bentazone was frequently detected (detection frequency: 96.3%) in 160 tap water samples (underwent conventional treatment) (median: 1.95 ng/L, range: <0.02–47.0 ng/L), while it was not detectable in tap water samples that underwent ozone combined with activated carbon. Seasonal variations were found, with the lowest median concentration (ng/L) in April (0.46) and the highest in July (17.6). In addition, bentazone was frequently (92.1%) detected in human urine samples (median: 0.02 ng/mL; range: < 0.01–0.11 ng/mL). The estimated daily intake of bentazone based on its median concentration in tap water (0.04 ng/kg-body weight bw/day) accounted for approximately 8% of that based on the median urinary concentration (0.48 ng/kg-bw/day). This is the first time to characterize its occurrence in drinking water from China and its occurrence in the urine of the general population.
Arsenic in fine air particulate matter (PM
2.5
) has been identified as an important factor responsible for the morbidity of lung cancer, which has increased sharply in many regions of China. Some ...reports in China have shown that arsenic in the air exceeds the ambient air quality standard value, while long-term airborne arsenic concentrations in central China and human exposure via inhalation of PM–bound arsenic (inhalable airborne PM) have not been well characterized. In this study, 579 outdoor air PM
2.5
samples from Wuhan, a typical city in central China, were collected from 2015 to 2017, and arsenic was measured by inductively coupled plasma-mass spectrometry. Personal exposure to PM-bound arsenic via inhalation and urinary arsenic concentration were also measured. The concentrations of arsenic in PM
2.5
were in the range of 0.42–61.6 ng/m
3
(mean 8.48 ng/m
3
). The average concentration of arsenic in 2015 (10.7 ng/m
3
) was higher than that in 2016 (6.81 ng/m
3
) and 2017 (8.18 ng/m
3
), exceeded the standard value. The arsenic concentrations in spring and winter were higher than those in summer and autumn. No significant differences (
p
> 0.05) were found among different sites. The daily intake of arsenic inhalation based on PM
10
samples collected by personal samplers (median, 10.8 ng/m
3
) was estimated. Urban residents inhaled higher levels of PM-bound arsenic than rural residents. Daily intake of arsenic via inhalation accounted for a negligible part (< 1%) of the total daily intake of arsenic (calculated based on excreted urinary arsenic); however, potential associations between the adverse effects (e.g., lung adenocarcinoma) and inhaled PM-bound arsenic require more attention, particularly for those who experience in long-term exposure. This study is the first report of a 3-year temporal trend of airborne PM
2.5
-bound arsenic in central China.
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•Pregnant women were widely exposed to paraben derivatives.•Urinary concentrations of p-HB and 3,4-DHB were much higher than those of others.•Paraben derivatives were associated with ...seasons, pre-pregnancy BMI, and infant sex.•Paraben derivatives are major contributors for oxidative damage compared to parabens.•The first study on profiles of urinary paraben derivatives at three trimesters.
Exposure to parabens has been shown to increase oxidative stress, which has a vital impact on the development of numerous diseases. However, few studies reported the effects of the paraben derivatives on oxidative stress, particularly among pregnant women. This study, using repeated measurements, aimed to understand the exposure profiles of urinary paraben derivative concentrations and their relationships with oxidative stress biomarkers (OSBs). A total of 861 pregnant women, who provided spot urine samples at three trimesters, were included, and 2583 urine samples were used to measure four paraben derivatives p-hydroxybenzoic acid (p-HB), 3,4-dihydroxybenzoic acid (3,4-DHB), methyl protocatechuate, and ethyl protocatechuate, four parabens (methyl, ethyl, propyl, and butyl), and three OSBs 8-hydroxy-2′-deoxyguanosine (for DNA), 8-hydroxyguanosine (for RNA), and 4-hydroxy nonenal mercapturic acid (for lipid). Pregnant women were extensively exposed to parabens and paraben derivatives with detection frequencies (DFs) of 86.1%–100%, except for butylparaben with a DF of 14.9%. p-HB and 3,4-DHB had relatively high urinary concentrations (specific gravity-adjusted median values: 1394 and 74.5 ng/mL, respectively). Low reproducibility in paraben derivatives was found across the three trimesters. Sampling season, pre-pregnancy body mass index, and infant sex were predictors of some paraben derivatives/parabens. Linear mixed model analyses showed that all target compounds (if DF > 50%) were associated with increases in all the selected OSBs, where the percent change in OSBs with an interquartile range increase in paraben concentration ranged from 9.85% to 24.7%, while those in paraben derivative concentration ranged from 13.8% to 72.1%. Weighted quantile sum model showed that joint exposure was significantly associated with increased OSBs, and paraben derivatives were stronger contributors to OSBs compared with parabens. Overall, urinary paraben derivatives were associated with increased oxidative stress of nucleic acids and lipid in pregnant women.
Prenatal cadmium (Cd) exposure has been associated with adverse birth outcomes, but the findings of previous studies are inconsistent. The aim of this study was to evaluate the association between ...prenatal Cd exposure and birth outcomes.
This study was conducted in 5364 pregnant women with a live singleton birth, who were recruited between September 2012 and October 2014 in the Healthy Baby Cohort (HBC) in Wuhan, China. Gestational age (in days) was estimated using both the woman's last menstrual period (LMP) and ultrasound data. All the birth outcomes including birth weight and birth length were measured in the hospital within one hour after birth through standardized procedures. Cd was measured in maternal urine collected before delivery with inductively coupled plasma mass spectrometry.
The geometric mean of Cd concentration in maternal urine was 0.55 (range 0.01–2.85) μg/g creatinine. We found each ln-unit increase in Cd concentration (μg/g creatinine) in maternal urine was associated with decreased gestational age adjusted β=−0.77day; 95% confidence interval (CI): −1.15, −0.39 for all infants; −0.77; 95% CI: −1.29, −0.25 for boys; and −0.80; 95% CI: −1.35, −0.25 for girls. Increased likelihood of preterm birth (PTB) was associated with ln-unit increase in urinary Cd (μg/g creatinine) adjusted odds ratio (OR)=1.78; 95% CI: 1.45, 2.19 for all infants; 1.97; 95% CI: 1.46, 2.65 for boys; and 1.67; 95% CI: 1.24, 2.25 for girls. Maternal urinary Cd was not significantly associated with low birth weight (LBW) and small for gestational age (SGA).
Maternal exposure to Cd during pregnancy was associated with decreased gestational age and increased likelihood of PTB.
•The largest study to investigate maternal cadmium exposure and birth outcomes.•Prenatal exposure to cadmium decreased gestational age.•Cadmium exposure during pregnancy increased the risk of preterm birth.
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