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During the COVID-19 pandemic, one of Australia's biggest cities, Melbourne, experienced three major isolation ("lockdown") periods in 2020 (160 days) and in 2021 (111 days) which makes it one of the most locked down cities world-wide. This study assessed how the pandemic affected temporal trends in methamphetamine, MDMA and cocaine consumption using wastewater-based epidemiology. Daily samples were collected for most of 2020 and 2021 (n = 660 days). Concentrations were measured using direct-injection LC-MS/MS and back-calculated to consumption estimates. Results indicate that methamphetamine use was increasing before the first lockdown and decreased after the end of the first lockdown in 2020. Methamphetamine trends appeared to have remained steady throughout the second lockdown period before increasing steeply after it ended. For most of 2020, cocaine use remained steady, with an increase after the second lockdown. MDMA use decreased after the start of the first lockdown and remained steady throughout most of 2020 and 2021. In comparison to 2020, trends in 2021 were less variable and stimulant use did not appear to be as associated with COVID-19 restrictions. Overall, this study was able to show the impact of lockdown periods and the related social restrictions on illicit stimulant use. ENVIRONMENTAL IMPLICATION: Illicit drugs are hazardous chemicals, of concern both to humans and the environment. While studies have been undertaken to understand their temporal trends, this work utilizes wastewater-based epidemiology and daily sampling to provide a comprehensive understanding of the impact of the COVID-19 pandemic on the use of methamphetamine, MDMA and cocaine on one of the most locked-down cities in the world. Understanding the consequences of this significant intervention on illicit drug use could provide valuable insights into its potential environmental impact.
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COVID-19 , Cocaína , Metanfetamina , Aguas Residuales , COVID-19/epidemiología , Humanos , Cocaína/análisis , Metanfetamina/análisis , Australia/epidemiología , N-Metil-3,4-metilenodioxianfetamina/análisis , Trastornos Relacionados con Sustancias/epidemiología , Contaminantes Químicos del Agua/análisis , Monitoreo Epidemiológico Basado en Aguas Residuales , Detección de Abuso de Sustancias/métodos , Ciudades , Drogas Ilícitas/análisis , SARS-CoV-2RESUMEN
BACKGROUND: The chemical space is comprised of a vast number of possible structures, of which an unknown portion comprises the human and environmental exposome. Such samples are frequently analyzed using non-targeted analysis via liquid chromatography (LC) coupled to high-resolution mass spectrometry often employing a reversed phase (RP) column. However, prior to analysis, the contents of these samples are unknown and could be comprised of thousands of known and unknown chemical constituents. Moreover, it is unknown which part of the chemical space is sufficiently retained and eluted using RPLC. RESULTS: We present a generic framework that uses a data driven approach to predict whether molecules fall 'inside', 'maybe' inside, or 'outside' of the RPLC subspace. Firstly, three retention index random forest (RF) regression models were constructed that showed that molecular fingerprints are able to predict RPLC retention behavior. Secondly, these models were used to set up the dataset for building an RPLC RF classification model. The RPLC classification model was able to correctly predict whether a chemical belonged to the RPLC subspace with an accuracy of 92% for the testing set. Finally, applying this model to the 91 737 small molecules (i.e., ≤1 000 Da) in NORMAN SusDat showed that 19.1% fall 'outside' of the RPLC subspace. SIGNIFICANCE AND NOVELTY: The RPLC chemical space model provides a major step towards mapping the chemical space and is able to assess whether chemicals can potentially be measured with an RPLC method (i.e., not every RPLC method) or if a different selectivity should be considered. Moreover, knowing which chemicals are outside of the RPLC subspace can assist in reducing potential candidates for library searching and avoid screening for chemicals that will not be present in RPLC data.
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Tobacco-specific alkaloids and nitrosamines are important biomarkers for the estimation of tobacco use and human exposure to tobacco-specific nitrosamines that can be monitored by wastewater analysis. Thus far their analysis has used solid phase extraction, which is costly and time-consuming. In this study, we developed a direct injection liquid chromatography-tandem mass spectrometry method for the quantification of two tobacco-specific alkaloids and five nitrosamines in wastewater. The method achieved excellent linearity (R2 > 0.99) for all analytes, with calibration ranging from 0.10 to 800 ng/L. Method limits of detection and quantification were 0.17 ng/L (N-nitrosonornicotine, NNN) and 1.0 ng/L (N-nitrosoanatabine (NAT) and NNN), with acceptable accuracy (100 % ± 20 %) and precision (± 15 %). Analyte loss during filtration was < 15 %, and the relative matrix effect was < 10 %. The method was applied to 43 pooled wastewater samples collected from three wastewater treatment plants in Australia between 2017 and 2021. Anabasine and anatabine were detected in all samples at concentrations of 5.0 - 33 ng/L and 12 - 41 ng/L, respectively. Three of the five tobacco-specific nitrosamines (NAT, NNN, and (4-(methylnitrosamino)-1-(3-pyridyl)-1-butanol) (NNAL)) were detected, in < 50 % of the wastewater samples, with concentrations nearly ten times lower than the tobacco alkaloids (< 1.0 - 6.2 ng/L). In-sewer stability of the nitrosamines was also assessed in this study, with four (NAT, NNAL, NNN, and N-nitrosoanabasine (NAB)) being stable (i.e. < 20 % transformation over 12 h in both control reactor (CR) and rising main reactor (RM) and 4-(methylnitrosamino)-1-(3-pyridyl)-1-butanone (NNK) being moderately stable (< 40 % loss over 12 h in RM). This direct injection method provides a high-throughput approach in simultaneous investigation of tobacco use and assessment of public exposure to tobacco-specific nitrosamines.
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Alcaloides , Nicotiana , Nitrosaminas , Espectrometría de Masas en Tándem , Aguas Residuales , Nitrosaminas/análisis , Nicotiana/química , Aguas Residuales/análisis , Aguas Residuales/química , Alcaloides/análisis , Espectrometría de Masas en Tándem/métodos , Límite de Detección , Contaminantes Químicos del Agua/análisis , Cromatografía Liquida/métodos , Ensayos Analíticos de Alto Rendimiento/métodosRESUMEN
BACKGROUND: Wastewater analysis provides a complementary measure of alcohol use in whole communities. We assessed absolute differences and temporal trends in alcohol consumption by degree of remoteness and socioeconomics indicators in Australia from 2016 to 2023. METHODS: Alcohol consumption estimates from 50 wastewater treatment plants (WWTP) in the Australian National Wastewater Drug Monitoring Program were used. Trends were analysed based on 1) site remoteness: Major Cities, Inner Regional and a combined remoteness category of Outer Regional and Remote, and 2) using two socioeconomic indexes from the Australian Bureau of Statistics (ABS) relating to advantage and disadvantage for Income, education, occupation, and housing. RESULTS: Consumption estimates were similar for Major Cities and Inner Regional areas (14.3 and 14.4L/day/1000 people), but significantly higher in Outer Regional and Remote sites (18.6L/day/1000 people). Consumption was decreasing in Major cities by 4.5% annually, Inner Regional by 2.4%, and 3.5% in the combined Outer Regional and Remote category. Consumption estimates were higher in socioeconomically advantaged quartiles than those of lower advantage (0%-25% mean = 13.0, 75%-100% mean = 17.4). Consumption in all quartiles decreased significantly over the 7 year period with annual rates of decrease of 0.9%, 3.7%, 3.6%, and 3.0% for the lowest to highest quartile, respectively. CONCLUSIONS: Declines in Australian alcohol consumption have been steeper in large urban areas than regional and remote areas. There were smaller annual decreases in the most socioeconomically disadvantaged areas. If continued, these trends may increase Australian health inequalities. Policy and prevention work should be appropriately targeted to produce more equitable long-term outcomes.
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Consumo de Bebidas Alcohólicas , Factores Socioeconómicos , Aguas Residuales , Humanos , Australia/epidemiología , Consumo de Bebidas Alcohólicas/epidemiología , Consumo de Bebidas Alcohólicas/tendencias , MasculinoRESUMEN
Wastewater treatment plants (WWTPs) have been recognized as secondary sources of per- and polyfluoroalkyl substances (PFAS) released into the environment. In this study, PFAS concentrations were measured in effluent and biosolids samples collected from 75 WWTPs across Australia during the 2016 Census period, which covers more than half of the Australian population. Twelve PFAS compounds, including six C5-C10 perfluoroalkyl carboxylic acids (PFCAs), four perfluoro sulfonic acids (PFSAs) such as perfluorobutane sulfonate (PFBS), perfuorohexane sulfonic (PFHxS), perfluorooctane sulfonic acid (PFOS), and perfluorodecane sulfonic acid (PFDS), and one fluorotelomer sulfonic acid (6:2 FTS), were detected in the effluent, with concentrations up to 504 ng/L (PFHxS). Among these, perfluorooctanoic acid (PFOA), perfluorohexanoic acid (PFHxA), and perfluoropentanic acid (PFPeA) exhibited the highest median concentrations. In the biosolids, a total of 21 PFAS compounds were detected, encompassing ten C4-C14 PFCAs, four PFSAs, two FTS (6:2 and 8:2 FTS), perfluorooctane sulfonamide (PFOSA), two perfluorooctane sulfonamido acetic acid (NMethyl FOSAA and NEthyl FOSAA), and two perfluorooctane sulfonamido ethanol (FOSE), with dry weight (dw) concentrations approaching 235 ng/g (PFOS). The highest median and mean concentrations were observed for perfluorodecanoic acid (PFDA) and PFOS. An annual discharge of approximately 250 kg of the total 21 PFAS compounds was estimated through the effluent and biosolids of the participating WWTPs. Notably, PFOS and 6:2 FTS constituted the largest proportion of total PFAS in the WWTPs' output. While PFCAs were higher in effluent concentrations compared to influent levels across most WWTPs (92% of WWTPs for ∑8PFCAs), the concentrations of PFSAs either decreased or remained relatively stable (in 80% of WWTPs for ∑4PFSAs) throughout the wastewater treatment process.
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Fluorocarburos , Eliminación de Residuos Líquidos , Aguas Residuales , Contaminantes Químicos del Agua , Australia , Fluorocarburos/análisis , Contaminantes Químicos del Agua/análisis , Aguas Residuales/química , Monitoreo del Ambiente , Aguas del Alcantarillado/análisis , Ácidos Alcanesulfónicos/análisisRESUMEN
The complexity around the dynamic markets for new psychoactive substances (NPS) forces researchers to develop and apply innovative analytical strategies to detect and identify them in influent urban wastewater. In this work a comprehensive suspect screening workflow following liquid chromatography - high resolution mass spectrometry analysis was established utilising the open-source InSpectra data processing platform and the HighResNPS library. In total, 278 urban influent wastewater samples from 47 sites in 16 countries were collected to investigate the presence of NPS and other drugs of abuse. A total of 50 compounds were detected in samples from at least one site. Most compounds found were prescription drugs such as gabapentin (detection frequency 79%), codeine (40%) and pregabalin (15%). However, cocaine was the most found illicit drug (83%), in all countries where samples were collected apart from the Republic of Korea and China. Eight NPS were also identified with this protocol: 3-methylmethcathinone 11%), eutylone (6%), etizolam (2%), 3-chloromethcathinone (4%), mitragynine (6%), phenibut (2%), 25I-NBOH (2%) and trimethoxyamphetamine (2%). The latter three have not previously been reported in municipal wastewater samples. The workflow employed allowed the prioritisation of features to be further investigated, reducing processing time and gaining in confidence in their identification.
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Drogas Ilícitas , Contaminantes Químicos del Agua , Aguas Residuales , Flujo de Trabajo , Psicotrópicos , China , Contaminantes Químicos del Agua/análisisRESUMEN
Wastewater-based epidemiology (WBE) is proposed as a cost-effective approach to objectively monitor the antidepressant use but it requires more accurate correction factors (CF) than what had been used in previous studies. Amitriptyline is a popular prescription medicine for treating depression and nerve pain, which could be prone to misuse and need monitoring. The CF of amitriptyline employed in previous WBE studies varied from 10 to 100, leading to substantial disparities between WBE estimates and expected mass of antidepressants in wastewater. Hence, this study aimed to take amitriptyline as a case study and refine the CF by correlating mass loads measured in wastewater from 12.2 million inhabitants collected during the 2016 Census with corresponding annual sales data. The triangulation of WBE data and sales data resulted in a newly-derived CF of 7, which is significantly different from the CF values used in previous studies. The newly derived CF was applied to a secondary, multi-year (2017 to 2020) WBE dataset for validation against sales data in the same period, demonstrating the estimated amitriptyline use (380 ± 320 mg/day/1000 inhabitants) is consistent with sales data (450 ± 190 mg/day/1000 inhabitants). When we applied the new CF to previous studies, the wastewater consumption loads matched better to prescription data than previous WBE estimations. The refined CF of amitriptyline can be used in future WBE studies to improve the accuracy of the consumption estimates.
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Amitriptilina , Aguas Residuales , Monitoreo Epidemiológico Basado en Aguas Residuales , Antidepresivos/uso terapéuticoRESUMEN
BACKGROUND: In the context of drug prohibition, potential adulteration and variable purity pose additional health risks for people who use drugs, with these risks often compounded by the outdoor music festival environment. Ahead of the imminent implementation of drug checking services in Queensland, Australia, this study aims to characterise this problem using triangulated survey and wastewater data to understand self-reported and detected drug use among attendees of a multi-day Queensland-based music festival in 2021 and 2022. METHODS: We administered an in-situ survey focusing on drug use at the festival to two convenience samples of 136 and 140 festival attendees in 2021 and 2022 respectively. We compared survey findings to wastewater collected concurrently from the festival's site-specific wastewater treatment plant, which was analysed using Liquid Chromatography Tandem Mass Spectrometry. RESULTS: Most survey respondents (82 % in 2021, 92 % in 2022) reported using or intending to use an illicit drug at the festival. Some respondents reported potentially risky drug use practices such as using drugs found on the ground (2 % in 2021, 4 % in 2022). Substances detected in wastewater but not surveys include MDEA, mephedrone, methylone, 3-MMC, alpha-D2PV, etizolam, eutylone, and N,N-dimethylpentylone. CONCLUSION: Many substances detected in wastewater but not self-reported in surveys likely represent substitutions or adulterants. These findings highlight the benefits of drug checking services to prevent harms from adulterants and provide education on safer drug use practices. These findings also provide useful information on socio-demographic characteristics and drug use patterns of potential users of Queensland's future drug checking service.
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Música , Trastornos Relacionados con Sustancias , Humanos , Autoinforme , Aguas Residuales , Australia , Vacaciones y Feriados , Trastornos Relacionados con Sustancias/epidemiologíaRESUMEN
One of the primary criteria for a suitable drug biomarker for wastewater-based epidemiology (WBE) is having a unique source representing human metabolism. For WBE studies, this means it is important to identify and monitor metabolites rather than parent drugs, to capture consumption of drugs and not fractions that could be directly disposed. In this study, a high-throughput workflow based on a human liver S9 fraction in vitro metabolism assay was developed to identify human transformation products of new chemicals, using α-pyrrolidino-2-phenylacetophenone (α-D2PV) as a case study. Analysis by liquid chromatography coupled to high resolution mass spectrometry identified four metabolites. Subsequently, a targeted liquid chromatography - tandem mass spectrometry method was developed for their analysis in wastewater samples collected from a music festival in Australia. The successful application of this workflow opens the door for future work to better understand the metabolism of chemicals and their detection and application for wastewater-based epidemiology.
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Monitoreo Epidemiológico Basado en Aguas Residuales , Aguas Residuales , Humanos , Espectrometría de Masas , Cromatografía Liquida/métodos , AustraliaRESUMEN
Users of novel psychoactive substances (NPS) are at risk, due to limited information about the toxicity and unpredictable effects of these compounds. Wastewater-based epidemiology (WBE) has been used as a tool to provide insight into NPS use at the population level. To understand the preferences and trends of NPS use in Australia, this study involved liquid chromatography mass spectrometry analysis of wastewater collected from Australian states and territories from February 2022 to February 2023. In total, 59 different NPS were included across two complementary analytical methods and covered up to 57 wastewater catchments over the study. The NPS detected in wastewater were 25-B-NBOMe, buphedrone, 1-benzylpiperazine (BZP), 3-chloromethcathinone, N,N-dimethylpentylone (N,N-DMP), N-ethylheptedrone, N-ethylpentylone, eutylone, 4F-phenibut, 2-fluoro deschloroketamine, hydroxetamine, mephedrone, methoxetamine, methylone, mitragynine, pentylone, phenibut, para-methoxyamphetamine (PMA), alpha-pyrrolidinovalerophenone (α-PVP) and valeryl fentanyl. The detection frequency for these NPS ranged from 3 % to 100 % of the sites analysed. A noticeable decreasing trend in eutylone detection frequency and mass loads was observed whilst simultaneously N,N-DMP and pentylone increased over the study period. The emergence of some NPS in wastewater pre-dates other sources of monitoring and provides further evidence that WBE can be used as an additional early warning system for alerting potential NPS use.
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Anfetaminas , Drogas Ilícitas , Monitoreo Epidemiológico Basado en Aguas Residuales , Ácido gamma-Aminobutírico/análogos & derivados , Australia , Aguas Residuales , Drogas Ilícitas/análisis , Psicotrópicos/análisisRESUMEN
Monitoring urinary markers of dietary, disease, and stress by wastewater-based epidemiology (WBE) is a promising tool to better understand population health and wellbeing. However, common urinary biomarkers are subject to degradation in sewer systems and their fates have to be assessed before they can be used in WBE. This study investigated the stability of 31 urinary biomarkers (12 food biomarkers, 8 vitamins, 9 oxidative stress biomarkers, and 1 histamine biomarker) in a laboratory sewer sediment reactor and evaluated their suitability for WBE, considering their detectability in real wastewater and in-sewer stability. These biomarkers showed various transformation patterns, among which 16 compounds had half-lives <2 h while other 15 compounds presented moderate to high stability (2 to >500 h). Thirteen biomarkers showed potential for WBE because of their consistently measurable concentrations in untreated wastewater and sufficient in-sewer stability. Eighteen biomarkers were unsuitable due to their rapid in-sewer degradation and/or undetectable concentration levels in untreated wastewater using previous methods. Transformation rates of these biomarkers showed generally weak relationships with molecular properties but relatively higher correlations with biological activities in sewers. Overall, this study determined in-sewer stability of 31 health-related biomarkers through laboratory experiments, providing new findings to WBE for population health assessment.
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Aguas Residuales , Contaminantes Químicos del Agua , Humanos , Monitoreo Epidemiológico Basado en Aguas Residuales , Contaminantes Químicos del Agua/análisis , Biomarcadores , Alimentos , Aguas del AlcantarilladoRESUMEN
Previous wastewater-based epidemiology (WBE) studies have reported decreasing trends of nicotine and tobacco use in Australia before 2017, but there is concern that increasing illicit use of nicotine in vaping products and illicit tobacco could reverse this progress. This study aimed to assess temporal trends of nicotine consumption and specifically tobacco consumption via wastewater analysis in a population in Australia between 2013 and 2021. One week of daily wastewater samples were analyzed every two months from February 2013 to December 2021 in a regional city serving â¼100,000 people. A total of 340 daily samples were analyzed for anabasine (tobacco specific biomarker) and nicotine metabolites, cotinine and hydroxycotinine, using direct injection method by liquid chromatography with tandem mass spectrometry. Daily consumption estimates were calculated from daily flow data, population estimates and previously reported excretion factors. Linear spline regression was performed to identify periods when significant change of slopes occurred and to evaluate the temporal trends. Tobacco use monitored using anabasine as a biomarker, showed a decreasing trend over the whole period with a higher rate of decrease during the first two years (2013-2014, 21 % decrease) compared to the later 7 years (2015-2021, 10 % decrease). Nicotine use, monitored using cotinine and hydroxycotinine, showed a downward trend between 2013 and 2018 (2013-2014: 18 % decrease, p < 0.05; 2015-2016: 6 % increase, p = 0.48; Feb-Dec 2017: 15 % decrease, p = 0.39) followed by a significant increase from 2018 to 2021 (40 % increase, p < 0.001). This finding suggests the increasing use of non-tobacco nicotine-based products. Additionally, the tobacco use estimate by wastewater analysis was higher than the tobacco sales data, which suggests the use of illicit tobacco in the catchment.
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Cotinina , Nicotina , Humanos , Nicotina/análisis , Cotinina/análisis , Aguas Residuales , Anabasina/análisis , Queensland/epidemiología , Australia/epidemiología , BiomarcadoresRESUMEN
Non-targeted analysis (NTA) has emerged as a valuable approach for the comprehensive monitoring of chemicals of emerging concern (CECs) in the exposome. The NTA approach can theoretically identify compounds with diverse physicochemical properties and sources. Even though they are generic and have a wide scope, non-targeted analysis methods have been shown to have limitations in terms of their coverage of the chemical space, as the number of identified chemicals in each sample is very low (e.g., ≤5%). Investigating the chemical space that is covered by each NTA assay is crucial for understanding the limitations and challenges associated with the workflow, from the experimental methods to the data acquisition and data processing techniques. In this review, we examined recent NTA studies published between 2017 and 2023 that employed liquid chromatography-high-resolution mass spectrometry. The parameters used in each study were documented, and the reported chemicals at confidence levels 1 and 2 were retrieved. The chosen experimental setups and the quality of the reporting were critically evaluated and discussed. Our findings reveal that only around 2% of the estimated chemical space was covered by the NTA studies investigated for this review. Little to no trend was found between the experimental setup and the observed coverage due to the generic and wide scope of the NTA studies. The limited coverage of the chemical space by the reviewed NTA studies highlights the necessity for a more comprehensive approach in the experimental and data processing setups in order to enable the exploration of a broader range of chemical space, with the ultimate goal of protecting human and environmental health. Recommendations for further exploring a wider range of the chemical space are given.
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Bioensayo , Salud Ambiental , Humanos , Cromatografía Liquida , Espectrometría de MasasRESUMEN
Campylobacter spp. is one of the four leading causes of diarrhoeal diseases worldwide, which are generally mild but can be fatal in children, the elderly, and immunosuppressed persons. The existing disease surveillance for Campylobacter infections is usually based on untimely clinical reports. Wastewater surveillance or wastewater-based epidemiology (WBE) has been developed for the early warning of disease outbreaks and the detection of the emerging new variants of human pathogens, especially after the global pandemic of COVID-19. However, the WBE monitoring of Campylobacter infections in communities is rare due to a few large data gaps. This study is a meta-analysis and systematic review of the prevalence of Campylobacter spp. in various wastewater samples, primarily the influent of wastewater treatment plants. The results showed that the overall prevalence of Campylobacter spp. was 53.26 % in influent wastewater and 52.97 % in all types of wastewater samples. The mean concentration in the influent was 3.31 ± 0.39 log10 gene copies or most probable number (MPN) per 100 mL. The detection method combining culture and PCR yielded the highest positive rate of 90.86 %, while RT-qPCR and qPCR were the two most frequently used quantification methods. In addition, the Campylobacter concentration in influent wastewater showed a seasonal fluctuation, with the highest concentration in the autumn at 3.46 ± 0.41 log10 gene copies or MPN per 100 mL. Based on the isolates of all positive samples, Campylobacter jejuni (62.34 %) was identified as the most prevalent species in wastewater, followed by Campylobacter coli (30.85 %) and Campylobacter lari (4.4 %). These findings provided significant data to further develop and optimize the wastewater surveillance of Campylobacter spp. infections. In addition, large data gaps were found in the decay of Campylobacter spp. in wastewater, indicating insufficient research on the persistence of Campylobacter spp. in wastewater.
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Drug consumption in prisons is a concern for the safety of incarcerated people and staff. Typically, drug use prevalence in prisons is estimated through urinalysis and intelligence operations, which can be intrusive and stressful. An alternative approach, wastewater-based epidemiology (WBE), was used in this study to estimate the consumption of licit and illicit drugs for the entire population of a prison in Australia. Wastewater samples were collected from March to December 2020, covering periods of no restrictions and periods when prison access was restricted to prevent the transmission of COVID-19. Target biomarkers were analysed by liquid chromatography coupled with tandem mass spectrometry (LC-MS/MS). The average consumption of common illicit drugs (MDMA, methamphetamine and cocaine) over the sampling period in the prison (0.5 - 4.5 mg/1000 people/day) was two to three orders of magnitude lower than in the community population (254 - 1000 mg/1000 people/day). Comparison of WBE estimates against pharmacy dispensing data suggested potential illicit buprenorphine consumption at the prison. Methamphetamine and buprenorphine use decreased when no visitors were allowed (18% - 72% decrease for methamphetamine; about half decrease for buprenorphine) and increased once these restrictions were eased (22% - 39% increase for methamphetamine; 44% - 67% increase for buprenorphine). The changes in drug use may be attributed in part to a reduction of drug trafficking into the prison from visitors or non-essential staffs and in part to the reduced contribution of urine from staff who used toilets within the prison. This study provided useful information on the scale of illicit drug use and extra-medical use of licit drugs in prison, and its changes under different security conditions.
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Buprenorfina , COVID-19 , Drogas Ilícitas , Metanfetamina , Trastornos Relacionados con Sustancias , Contaminantes Químicos del Agua , Humanos , Drogas Ilícitas/análisis , Prisiones , Aguas Residuales , Cromatografía Liquida , Detección de Abuso de Sustancias/métodos , Espectrometría de Masas en Tándem , COVID-19/epidemiología , Trastornos Relacionados con Sustancias/epidemiología , Metanfetamina/análisis , Contaminantes Químicos del Agua/análisis , Buprenorfina/análisisRESUMEN
Clean high-resolution mass spectra (HRMS) are essential to a successful structural elucidation of an unknown feature during nontarget analysis (NTA) workflows. This is a crucial step, particularly for the spectra generated during data-independent acquisition or during direct infusion experiments. The most commonly available tools only take advantage of the time domain for spectral cleanup. Here, we present an algorithm that combines the time domain and mass domain information to perform spectral deconvolution. The algorithm employs a probability-based cumulative neutral loss (CNL) model for fragment deconvolution. The optimized model, with a mass tolerance of 0.005 Da and a scoreCNL threshold of 0.00, was able to achieve a true positive rate (TPr) of 95.0%, a false discovery rate (FDr) of 20.6%, and a reduction rate of 35.4%. Additionally, the CNL model was extensively tested on real samples containing predominantly pesticides at different concentration levels and with matrix effects. Overall, the model was able to obtain a TPr above 88.8% with FD rates between 33 and 79% and reduction rates between 9 and 45%. Finally, the CNL model was compared with the retention time difference method and peak shape correlation analysis, showing that a combination of correlation analysis and the CNL model was the most effective for fragment deconvolution, obtaining a TPr of 84.7%, an FDr of 54.4%, and a reduction rate of 51.0%.
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The leaching of per- and polyfluoroalkyl substances (PFASs) from Australian firefighting training grounds has resulted in extensive contamination of groundwater and nearby farmlands. Humans, farm animals, and wildlife in these areas may have been exposed to complex mixtures of PFASs from aqueous film-forming foams (AFFFs). This study aimed to identify PFAS classes in pooled whole blood (n = 4) and serum (n = 4) from cattle exposed to AFFF-impacted groundwater and potentially discover new PFASs in blood. Thirty PFASs were identified at various levels of confidence (levels 1a-5a), including three novel compounds: (i) perfluorohexanesulfonamido 2-hydroxypropanoic acid (FHxSA-HOPrA), (ii) methyl((perfluorohexyl)sulfonyl)sulfuramidous acid, and (iii) methyl((perfluorooctyl)sulfonyl)sulfuramidous acid, belonging to two different classes. Biotransformation intermediate, perfluorohexanesulfonamido propanoic acid (FHxSA-PrA), hitherto unreported in biological samples, was detected in both whole blood and serum. Furthermore, perfluoroalkyl sulfonamides, including perfluoropropane sulfonamide (FPrSA), perfluorobutane sulfonamide (FBSA), and perfluorohexane sulfonamide (FHxSA) were predominantly detected in whole blood, suggesting that these accumulate in the cell fraction of blood. The suspect screening revealed several fluoroalkyl chain-substituted PFAS. The results suggest that targeting only the major PFASs in the plasma or serum of AFFF-exposed mammals likely underestimates the toxicological risks associated with exposure. Future studies of AFFF-exposed populations should include whole-blood analysis with high-resolution mass spectrometry to understand the true extent of PFAS exposure.
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Fluorocarburos , Agua Subterránea , Humanos , Animales , Bovinos , Australia , Animales Salvajes , Plasma , MamíferosRESUMEN
Environmental antimicrobial pollution and antimicrobial resistance pose a threat to environmental and human health. Wastewater analysis has been identified as a promising tool for antimicrobial monitoring and the back-estimation of antimicrobial consumption, but current pretreatment methods are tedious and complicated, limiting their scope for high-throughput analysis. A sensitive direct injection method for the quantification of 109 antimicrobials and their metabolites in wastewater samples was developed using liquid chromatography-tandem mass spectrometry (LC-MS/MS). The method was validated for both wastewater influent and effluent in terms of specificity, calibration range, matrix effect, filtration loss, accuracy, precision, limit of detection (LOD), and limit of quantification (LOQ). Most analytes achieved calibration of R2 > 0.99, and the calibration range was from 0.0002 to 150 µg L-1. Recoveries ranged consistently between ~50 % and ~100 % and losses were attributed to sample filtration. Method LOQs were determined as low as 0.0003 µg L-1, and acceptable accuracy (75 %-125 %) and precision (within 25 %) were achieved for >90 % of the analytes. The method was subsequently further assessed using wastewater of raw influent and treated effluent collected from 6 Australian wastewater treatment plants in 2021. In total, 37 analytes were detected in influent and 22 in effluent. Most of them could be quantified at concentrations ranging from 0.0053 to 160 µg L-1, with benzalkonium chloride-C12, amoxicilloic acid, and cephalexin detected at the highest concentrations. The current study provides a straightforward analytical method for antimicrobial monitoring in wastewater with a fast and simple pretreatment procedure.
Asunto(s)
Antiinfecciosos , Contaminantes Químicos del Agua , Humanos , Cromatografía Liquida , Aguas Residuales , Espectrometría de Masas en Tándem/métodos , Cromatografía Líquida de Alta Presión/métodos , Contaminantes Químicos del Agua/análisis , Australia , Extracción en Fase SólidaRESUMEN
Campylobacter spp. is one of the most frequent pathogens of bacterial gastroenteritis recorded worldwide. Campylobacter jejuni (C. jejuni) and Campylobacter coli (C. coli) are the two major disease-associated species, accounting for >95 % of infections, and thus have been selected for disease surveillance. Monitoring temporal variations in pathogen concentration and diversity excreted from community wastewater allows the early detection of outbreaks. Multiplex real-time/quantitative PCR (qPCR) enables multi-target quantification of pathogens in various types of samples including wastewater. Also, an internal amplification control (IAC) is required for each sample when adopting PCR-based methods for pathogen detection and quantification in wastewater to exclude the inhibition of the wastewater matrix. To achieve reliable quantification of C. jejuni and C. coli towards wastewater samples, this study developed and optimized a triplex qPCR assay by combining three qPCR primer-probe sets targeting Campylobacter jejuni subsp. jejuni, Campylobacter coli, and Campylobacter sputorum biovar sputorum (C. sputorum), respectively. This triplex qPCR assay not only can directly and simultaneously detect the concentration of C. jejuni and C. coli in wastewater but also can achieve the PCR inhibition control using C. sputorum primer-probe set. This is the first developed triplex qPCR assay with IAC for C. jejuni and C. coli, to be used in the wastewater-based epidemiology (WBE) applications. The optimized triplex qPCR assay enables the detection limit of the assay (ALOD100%) and wastewater (PLOD80%) as 10 gene copy/µL and 2 log10 cells/mL (2 gene copies/µL of extracted DNA), respectively. The application of this triplex qPCR to 52 real raw wastewater samples from 13 wastewater treatment plants demonstrated its potential as a high-throughput and economically viable tool for the long-term monitoring of C. jejuni and C. coli prevalence in communities and the surrounding environments. This study provided an accessible methodology and a solid foundation for WBE-based monitoring of Campylobacter spp. relevant diseases and paved the road for future WBE back-estimation of C. jejuni and C. coli prevalence.
Asunto(s)
Campylobacter coli , Campylobacter jejuni , Campylobacter , Campylobacter jejuni/genética , Campylobacter coli/genética , Aguas Residuales , Sensibilidad y Especificidad , ADN Bacteriano/análisisRESUMEN
Non-target analysis (NTA) employing high-resolution mass spectrometry (HRMS) coupled with liquid chromatography is increasingly being used to identify chemicals of biological relevance. HRMS datasets are large and complex making the identification of potentially relevant chemicals extremely challenging. As they are recorded in vendor-specific formats, interpreting them is often reliant on vendor-specific software that may not accommodate advancements in data processing. Here we present InSpectra, a vendor independent automated platform for the systematic detection of newly identified emerging chemical threats. InSpectra is web-based, open-source/access and modular providing highly flexible and extensible NTA and suspect screening workflows. As a cloud-based platform, InSpectra exploits parallel computing and big data archiving capabilities with a focus for sharing and community curation of HRMS data. InSpectra offers a reproducible and transparent approach for the identification, tracking and prioritisation of emerging chemical threats.