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Background: Toxicological studies indicate that neonicotinoids may be associated with disruptions in liver function due to an increase in oxidative stress. There are scant epidemiological studies investigating the chronic hepatotoxic effects of neonicotinoids. Objective: To examine the association between detectable concentrations of parent neonicotinoids and neonicotinoid metabolites with liver function markers among US adults, and whether sex modifies this association. Methods: National Health and Nutrition Examination Survey 2015-2016 data were used to estimate associations between detectable neonicotinoids and serum alkaline phosphatase (ALP), alanine aminotransferase, aspartate aminotransferase, gamma-glutamyl transaminase (GGT), albumin, total bilirubin, total protein, and Hepatic Steatosis Index (HSI) using multiple linear regression. Results: Detectable levels of N-desmethyl-acetamiprid were associated with a decrease in GGT (ß = -3.54 unit/l; 95% confidence interval [CI] = -6.48, -0.61) and detectable levels of 5-hydroxy-imidacloprid were associated with a decrease in HSI (ß = -1.11; 95% CI = -2.14, -0.07). Sex modified the association between any parent neonicotinoid and ALP (Pint = 0.064) and the association between clothianidin and ALP (Pint = 0.019), with a pattern of positive associations in males and inverse associations in females, though stratified associations did not reach statistical significance. Sex also modified the association between 5-hydroxy-imidacloprid and total protein (Pint = 0.062), with a significant positive association in females (ß = 0.14 g/dl; 95% CI = 0.03, 0.25) and a null association in males. Conclusion: Detectable concentrations of neonicotinoid metabolites were inversely associated with GGT and HSI in US adults. Evidence suggests neonicotinoids may influence liver function differently depending on sex. Future research is recommended to replicate the findings as the study was limited in its cross-sectional nature and inability to examine continuous neonicotinoid concentrations with liver function.

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In this work, a green analytical method was established for the simultaneous extraction and detection of 20 analytes-10 neonicotinoid insecticides and their 10 major toxic metabolites in edible herbs. QuEChERS and LC-MS/MS were used to analyze the 20 analytes in five edible herbs. The residues of the 20 neonicotinoid insecticides and their metabolites in 109 herbal samples were detected, of which 90 samples were positive, and the residue of total neonicotinoid insecticides ranged from 0.26 to 139.28 µg/kg. Acetamiprid (77.06 %, ≤85.95 µg/kg), imidacloprid (67.89 %, ≤32.49 µg/kg) and their metabolites (N-desmethyl-acetamiprid (44.04 %, ≤18.42 µg/kg) and desnitro imidacloprid (48.62 %, ≤16.55 µg/kg) were most frequently detected in herbs. Significant positive correlations were found between imidacloprid/acetamiprid and their metabolites in Lycii fructus and Citri reticulatae pericarpium. Therefore, more attention may be given to the neonicotinoid insecticide residues in edible herbs in the future.

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In recent years, the residues of neonicotinoid insecticide in food and environmental samples have attracted extensive attention. Neonicotinoids have many adverse effects on human health, such as cancer, chronic disease, birth defects, and infertility. They have substantial toxicity to some non-target organisms (especially bees). Hence, monitoring the residues of neonicotinoid insecticides in foodstuffs is necessary to guarantee public health and ecological stability. This review aims to summarize and assess the metabolic features, residue status, sample pretreatment methods (solid-phase extraction (SPE), Quick, Easy, Cheap, Effective, Rugged, and Safe (QuEChERS), and some novel pretreatment methods), and detection methods (instrument detection, immunoassay, and some innovative detection methods) for neonicotinoid insecticide residues in food and environmental samples. This review provides detailed references and discussion for the analysis of neonicotinoid insecticide residues, which can effectively promote the establishment of innovative detection methods for neonicotinoid insecticide residues.

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BACKGROUND: Toxicology studies suggest that neonicotinoids may be associated with adiposity development via thyroid hormone disruption and increased oxidative stress. Prior epidemiological studies report mixed results for the association between neonicotinoids and adiposity measures. OBJECTIVE: To examine the association between detectable concentrations of parent neonicotinoids (imidacloprid, acetamiprid, clothianidin) and neonicotinoid metabolites (5-hydroxy-imidacloprid, N-desmethyl-acetamiprid) with adiposity measures among US adults, and whether sex modifies the associations for neonicotinoid metabolites with adiposity. METHODS: National Health and Nutrition Examination Survey (NHANES) 2015-2016 data was utilized to estimate covariate-adjusted associations between detectable neonicotinoids and fat mass index (FMI), lean mass index (LMI), waist circumference, body fat percentage, and body mass index (BMI) using multiple linear regression. We estimated incidence rate ratios (IRRs) for overweight or obese status with detectable neonicotinoid concentrations using Poisson's modified regression. Sampling strategies were accounted for in the regression models. RESULTS: Detectable levels of acetamiprid were associated with a decrease in FMI (ß = -3.17 kg/m2, 95% CI [-4.79, -1.54]), LMI (ß = -3.17 kg/m2, 95% CI [-5.17, -1.17]), body fat percentage (ß = -4.41, 95% CI [-8.20, -0.62]), waist circumference (ß = -9.80 cm, 95% CI [-19.08, -0.51]), and BMI (ß = -3.88kg/m2, 95% CI [-7.25, -0.51]) among adults. In contrast, detectable levels of 5-hydroxy-imidacloprid were associated with greater rates of being overweight/obese (IRR = 1.11, 95% CI [1.04, 1.18)) and increased LMI (ß = 0.67 kg/m2, 95% CI [0.04, 1.29]). Sex modified the association between N-desmethyl-acetamiprid and LMI (pint = 0.075) with a positive association among males (ß = 1.14 kg/m2, 95% CI [0.38, 1.90]), and an insignificant inverse association in females. Sex also modified the association for N-desmethyl-acetamiprid with FMI (pint = 0.095) and body fat percentage (pint = 0.072), with suggestive evidence showing positive associations for males and inverse associations for females. CONCLUSION: Detectable concentrations of acetamiprid were inversely associated with adiposity, while there were mixed findings for 5-hydroxy-imidacloprid. Findings suggest sex differences, though results are not clear with regard to the directionality of the association by sex.

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BACKGROUND: Neonicotinoids (NN) are selective neurotoxic pesticides that bind to insect but also mammal nicotinic acetycholine receptors (nAChRs). As the most widely used class of insecticides worldwide, they are ubiquitously found in the environment, wildlife, and foods, and thus of special concern for their impacts on the environment and human health. nAChRs are vital to proper brain organization during the prenatal period and play important roles in various motor, emotional, and cognitive functions. Little is known on children's contamination by NN. In a pilot study we tested the hypothesis that children's cerebro-spinal fluid (CSF) can be contaminated by NN. METHODS: NN were analysed in leftover CSF, blood, and urine samples from children treated for leukaemias and lymphomas and undergoing therapeutic lumbar punctions. We monitored all neonicotinoids approved on the global market and some of their most common metabolites by ultra-high performance liquid chromatography-tandem mass spectrometry. RESULTS: From August to December 2020, 14 children were consecutively included in the study. Median age was 8 years (range 3-18). All CSF and plasma samples were positive for at least one NN. Nine (64%) CSF samples and 13 (93%) plasma samples contained more than one NN. Thirteen (93%) CSF samples had N-desmethyl-acetamiprid (median concentration 0.0123, range 0.0024-0.1068 ng/mL), the major metabolite of acetamiprid. All but one urine samples were positive for ≥ one NN. A statistically significant linear relationship was found between plasma/urine and CSF N-desmethyl-acetamiprid concentrations. CONCLUSIONS: We have developed a reliable analytical method that revealed multiple NN and/or their metabolites in children's CSF, plasma, and urine. Our data suggest that contamination by multiple NN is not only an environmental hazard for non-target insects such as bees but also potentially for children.

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Animal studies have revealed that exposure to neonicotinoid insecticides (NNIs) could compromise male reproductive function; however, related data on the occurrence of NNIs and their specific metabolites in human seminal plasma are scarce. To explore the potential effects of NNI exposure on male semen quality, we determined the concentrations of NNIs and some of their metabolites (collectively defined as mNNIs) in seminal plasma samples collected from men (n = 191) who visited a fertility clinic in Shijiazhuang, North China from 2018 to 2019. Associations between the mNNI concentrations and semen quality parameters were assessed using linear regression models, adjusting for important covariates. In the seminal plasma samples, desmethyl-acetamiprid (DM-ACE, detection frequency: 98.4%), imidacloprid-olefin (IMI-olefin, detection frequency: 86.5%), and desmethyl-clothianidin (DM-CLO, detection frequency: 70.8%) were frequently detected at median concentrations of 0.052, 0.003, and 0.007 ng/mL, respectively; meanwhile other compounds were detected at less than the method detection limits. In the single-mNNI models, the IMI-olefin concentration was associated with decreased progressive motility [IMI-olefin concentration: percent change (%Δ) = -17.0; 95% confidence interval (CI) = -30.3, -0.92; the highest tertile compared with the lowest tertile: %Δ = -21.1; 95% CI = -37.5, -0.23]. Similar results were found in the multiple-mNNIs models. No other inverse associations were found between the other mNNI concentrations and semen quality parameters. This is the first study to identify the occurrence of mNNIs in the seminal plasma and the potential associations of their concentrations with human semen quality parameters. These findings imply an inverse association between the IMI-olefin concentration and semen quality.

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Neonicotinoid insecticides (NNIs) are the most widely used insecticides globally and ubiquitous in the environment, which has led to widespread human exposure. However, studies on internal exposure levels of NNIs and their metabolites in pregnant women are scarce. In this study, we measured nine parent NNIs and ten main metabolites in 1224 urine samples donated by 408 pregnant women at three trimesters. In the urine samples, the unadjusted vs. specific gravity (SG) adjusted median concentrations and detection frequencies (DFs) of desmethyl-acetamiprid (DM-ACE; 1.01 vs. 1.08 ng/mL; DF: 99.7%), 5-hydroxy-imidacloprid (5-hydroxy-IMI; 0.54 vs. 0.56 ng/mL; 98.5%), imidacloprid-olefin (IMI-olefin; 0.41 vs. 0.44 ng/mL; 99.3%), and desnitro-imidacloprid (DN-IMI; 0.12 vs. 0.12 ng/mL; 90.4%) were higher than their corresponding parent NNIs, acetamiprid (ACE; <0.01 vs. <0.01 ng/mL; 26.4%) and imidacloprid (IMI; 0.04 vs. 0.04 ng/mL; 69.9%). The unadjusted and SG-adjusted median concentrations of clothianidin (CLO), thiamethoxam (THM), and desmethyl-clothianidin (DM-CLO) were 0.05 vs. 0.07, 0.05 vs. 0.06, and 0.04 vs. 0.05 ng/mL, with the DFs of 61.0%, 57.5%, and 75.7%, respectively. The cumulative exposure level, imidacloprid-equivalent total NNIs (IMIeq), was generated by the relative potency factor approach considering the toxic effects of NNIs and their metabolites. The unadjusted IMIeq varied from 0.17 ng/mL (SG-adjusted: 0.20) to 1969 ng/mL (SG-adjusted: 1817) with a median of 14.1 ng/mL (SG-adjusted: 14.1). A decreased trend was observed in urinary NNIs and their metabolites throughout the three trimesters. Maternal age, educational level, and household income were related to the concentrations of NNIs and their metabolites. DM-ACE, 5-hydroxy-IMI, and IMI-olefin were significantly lower in winter than in autumn; DN-IMI, THM, CLO, and DM-CLO were significantly higher in both summer and autumn than in winter. The maximum estimated daily intake of IMIeq [34.8 µg/kg-body weight (bw)/d] was lower than the chronic reference dose of IMI (57 µg/kg-bw/d) currently recommended by the United States Environmental Protection Agency. Human health risk of exposure to NNIs and their main metabolites warranted further studies.

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Neonicotinoid insecticides (NNIs) are the most extensively used insecticides worldwide, threatening ecosystem and human health. However, nationwide studies of NNIs and their metabolites in drinking water are limited. In order to characterize the contamination status of NNIs in drinking water throughout China, we collected 884 drinking water samples including 789 tap water and 95 groundwater samples from 32 provinces (covering seven regions of mainland China: south, central, east, north, northeast, northwest, and southwest) and Hong Kong. Ten NNIs and six of their main metabolites were determined in the water samples. The relative potency factor method was used to assess the cumulative concentrations of NNIs and their metabolites (imidacloprid-equivalent total NNIs, IMIeq) based on the chronic reference doses (cRfDs) of the NNIs or the toxic effects of the mataboilites. The IMIeq varied among the studied regions, with a median concentration of 24.5 ng/L and a maximum concentration of 8,622 ng/L. The predominant NNIs in drinking water were acetamiprid (ACE) and imidacloprid (IMI). Compared with tap water derived from groundwater, much higher concentrations of IMIeq and NNIs were found in tap water derived from surface water. Different concentrations and patterns of NNIs in drinking water were observed in different regions, provinces, and capital cities, mainly due to regional and provincial differences in crop types and volumes of pesticide usage. The concentrations of NNIs in the drinking water of provincial capitals and small/medium cities were higher than the concentrations in rural areas. The estimated daily intake (EDI) of IMIeq was at least two orders of magnitude lower than the cRfD of IMI, while the NNIs in 16 drinking water samples exceeded the acceptable value (100 ng/L) recommended by the European Union. This study provided a nationwide profile of the occurrence of NNIs and their metabolites in the drinking water of China and the associated potential cumulative human health risks, taking into account of the toxicity differences between NNIs and their metabolites.

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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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