Nicolette A Bugher, Boya Xiong, Runako I Gentles, Lukas D Glist, Helen G Siegel, Nicholaus P Johnson, Cassandra J Clark, Nicole C Deziel, James E Saiers, Desiree L Plata
Lack of water quality data for private drinking water sources prevents robust evaluation of exposure risk for communities co-located with historically contaminated sites and ongoing industrial activity. Areas of the Appalachian region of the United States (i.e., Pennsylvania, Ohio and West Virginia) contain extensive hydraulic fracturing activity, as well as other extractive and industrial technologies, in close proximity to communities reliant on private drinking water sources, creating concern over potential groundwater contamination. In this study, we characterized volatile organic compound (VOC) occurrence at 307 private groundwater well sites within Pennsylvania, Ohio, and West Virginia. The majority (97%) of water samples contained at least one VOC, while the average number of VOCs detected at a given site was 5 ± 3. The majority of individual VOC concentrations fell below applicable U.S. Environmental Protection Agency (EPA) Maximum Contamination Levels (MCLs), except for chloroform (MCL of 80 μg L-1; n = 1 at 98 μg L-1), 1,2-dibromoethane (MCL of 0.05 μg L-1; n = 3 ranging from 0.05 to 0.35 μg L-1), and 1,2-dibromo-3-chloropropane (MCL of 0.2 μg L-1; n = 7 ranging from 0.20 to 0.58 μg L-1). To evaluate well susceptibility to VOCs from industrial activity, distance to hydraulic fracturing site was used to assess correlations with contaminant occurrences. Proximity to closest hydraulic fracturing well-site revealed no statistically significant linear relationships with either individual VOC concentrations, or frequency of VOC detections. Evaluation of other known industrial contamination sites (e.g., US EPA Superfund sites) revealed elevated levels of three VOCs (chloroform, toluene, benzene) in groundwaters within 10 km of those Superfund sites in West Virginia and Ohio, illuminating possible point source influence. Lack of correlation between VOC concentrations and proximity to specific point sources indicates complex geochemical processes governing trace VOC contamination of private drinking water sources. While individual concentrations of VOCs fell well below recommended human health levels, the low dose exposure to multiple VOCs occurring in drinking supplies for Appalachian communities was noted, highlighting the importance of groundwater well monitoring.
{"title":"Domestic groundwater wells in Appalachia show evidence of low-dose, complex mixtures of legacy pollutants.","authors":"Nicolette A Bugher, Boya Xiong, Runako I Gentles, Lukas D Glist, Helen G Siegel, Nicholaus P Johnson, Cassandra J Clark, Nicole C Deziel, James E Saiers, Desiree L Plata","doi":"10.1039/d4em00364k","DOIUrl":"https://doi.org/10.1039/d4em00364k","url":null,"abstract":"<p><p>Lack of water quality data for private drinking water sources prevents robust evaluation of exposure risk for communities co-located with historically contaminated sites and ongoing industrial activity. Areas of the Appalachian region of the United States (<i>i.e.</i>, Pennsylvania, Ohio and West Virginia) contain extensive hydraulic fracturing activity, as well as other extractive and industrial technologies, in close proximity to communities reliant on private drinking water sources, creating concern over potential groundwater contamination. In this study, we characterized volatile organic compound (VOC) occurrence at 307 private groundwater well sites within Pennsylvania, Ohio, and West Virginia. The majority (97%) of water samples contained at least one VOC, while the average number of VOCs detected at a given site was 5 ± 3. The majority of individual VOC concentrations fell below applicable U.S. Environmental Protection Agency (EPA) Maximum Contamination Levels (MCLs), except for chloroform (MCL of 80 μg L<sup>-1</sup>; <i>n</i> = 1 at 98 μg L<sup>-1</sup>), 1,2-dibromoethane (MCL of 0.05 μg L<sup>-1</sup>; <i>n</i> = 3 ranging from 0.05 to 0.35 μg L<sup>-1</sup>), and 1,2-dibromo-3-chloropropane (MCL of 0.2 μg L<sup>-1</sup>; <i>n</i> = 7 ranging from 0.20 to 0.58 μg L<sup>-1</sup>). To evaluate well susceptibility to VOCs from industrial activity, distance to hydraulic fracturing site was used to assess correlations with contaminant occurrences. Proximity to closest hydraulic fracturing well-site revealed no statistically significant linear relationships with either individual VOC concentrations, or frequency of VOC detections. Evaluation of other known industrial contamination sites (<i>e.g.</i>, US EPA Superfund sites) revealed elevated levels of three VOCs (chloroform, toluene, benzene) in groundwaters within 10 km of those Superfund sites in West Virginia and Ohio, illuminating possible point source influence. Lack of correlation between VOC concentrations and proximity to specific point sources indicates complex geochemical processes governing trace VOC contamination of private drinking water sources. While individual concentrations of VOCs fell well below recommended human health levels, the low dose exposure to multiple VOCs occurring in drinking supplies for Appalachian communities was noted, highlighting the importance of groundwater well monitoring.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581049","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Prashant Srivastava, Grant Douglas, Greg B Davis, Rai S Kookana, Canh Tien Trinh Nguyen, Mike Williams, Karl Bowles, Jason K Kirby
The historical use and storage of aqueous film-forming foams (AFFF) containing per- and poly-fluoroalkyl substances (PFAS) at a range of sites including airports, defence, and port facilities have resulted in a legacy of contaminated infrastructure such as concrete. Contaminated concrete constitutes an ongoing source of PFAS contamination requiring management to ensure the protection of human health and the environment. In this study, modified Leaching Environmental Assessment Framework (LEAF) and Australian Standard Leaching Procedure (ASLP) were used to examine the leachability of PFAS, specifically, perfluorooctanesulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS) and perfluorohexanoic acid (PFHxA) from AFFF-contaminated concrete collected from an Australian Defence Fire Training Area (FTA). In general, PFAS readily leached from intact contaminated concrete monoliths with the cumulative proportion (%) decreasing in the order: PFHxA (>95%) > PFOS (26-84%) ≈ PFHxS (14-78%) > PFOA (<1-54%). Higher leachability for PFHxA from concrete is consistent with previous findings for solids, however, inconsistent for PFOA with higher retention (lower leachability) in concrete as compared to PFOS. Duration of exposure to water (0.5-48 h) and temperature (25 °C and 50 °C) had little influence on the proportion of PFAS leachability from powdered concrete. A higher proportion of PFAS leached from a <2 mm concrete powder size fraction as compared to 2-20 mm and 20 mm size fractions. This behavior reflects an increase in surface area with decreasing concrete particle size. Reducing the particle size could enhance PFAS removal from waste concrete.
{"title":"Leachability of per- and poly-fluoroalkyl substances from contaminated concrete.","authors":"Prashant Srivastava, Grant Douglas, Greg B Davis, Rai S Kookana, Canh Tien Trinh Nguyen, Mike Williams, Karl Bowles, Jason K Kirby","doi":"10.1039/d4em00482e","DOIUrl":"https://doi.org/10.1039/d4em00482e","url":null,"abstract":"<p><p>The historical use and storage of aqueous film-forming foams (AFFF) containing per- and poly-fluoroalkyl substances (PFAS) at a range of sites including airports, defence, and port facilities have resulted in a legacy of contaminated infrastructure such as concrete. Contaminated concrete constitutes an ongoing source of PFAS contamination requiring management to ensure the protection of human health and the environment. In this study, modified Leaching Environmental Assessment Framework (LEAF) and Australian Standard Leaching Procedure (ASLP) were used to examine the leachability of PFAS, specifically, perfluorooctanesulfonate (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonate (PFHxS) and perfluorohexanoic acid (PFHxA) from AFFF-contaminated concrete collected from an Australian Defence Fire Training Area (FTA). In general, PFAS readily leached from intact contaminated concrete monoliths with the cumulative proportion (%) decreasing in the order: PFHxA (>95%) > PFOS (26-84%) ≈ PFHxS (14-78%) > PFOA (<1-54%). Higher leachability for PFHxA from concrete is consistent with previous findings for solids, however, inconsistent for PFOA with higher retention (lower leachability) in concrete as compared to PFOS. Duration of exposure to water (0.5-48 h) and temperature (25 °C and 50 °C) had little influence on the proportion of PFAS leachability from powdered concrete. A higher proportion of PFAS leached from a <2 mm concrete powder size fraction as compared to 2-20 mm and 20 mm size fractions. This behavior reflects an increase in surface area with decreasing concrete particle size. Reducing the particle size could enhance PFAS removal from waste concrete.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581062","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Estefania Garcia, Pan Liu, Sharon E Bone, Yinghao Wen, Yuanzhi Tang
Millions of tons of coal fly ashes (CFAs) are produced annually during coal combustion in the U.S., which are commonly beneficially used in the concrete industry or disposed of in ash ponds. CFAs contain trace amounts of a range of toxic heavy metals including selenium (Se). Because the toxicity of Se is dependent on its speciation, investigating Se speciation in CFAs as affected by coal source and combustion conditions can help understand the related environmental and human health impacts during disposal or beneficial reuse. In this study, a set of representative CFA samples were characterized for Se speciation using synchrotron X-ray absorption spectroscopy (XAS) and micro-X-ray fluorescence spectromicroscopy (μ-XRF/XAS). Se-containing particles were highly heterogeneous, and individual particles might contain multiple oxidation states including Se(0), Se(IV), and Se(VI). Principal component analysis was performed for sample characteristics including Al2O3, SiO2, CaO, FeO, loss on ignition, average particle size, Se concentration, and Se oxidation state. Selective catalytic reduction (SCR), which is used to limit nitrogen oxide (NOx) emissions during coal combustion, was found to be associated with the presence of reduced Se oxidation states, with up to 90% Se(0) observed in samples with SCR. Alongside SCR, FeO content may also influence Se speciation.
美国每年在燃煤过程中会产生数百万吨煤飞灰(CFA),这些煤飞灰通常被用于混凝土行业或在灰池中进行处置。煤飞灰中含有微量的有毒重金属,包括硒(Se)。由于硒的毒性取决于其种类,因此调查 CFAs 中受煤源和燃烧条件影响的硒种类有助于了解在处置或有益再利用过程中对环境和人类健康的相关影响。本研究利用同步辐射 X 射线吸收光谱(XAS)和显微 X 射线荧光光谱(μ-XRF/XAS)对一组具有代表性的 CFA 样品进行了硒的标示。含Se颗粒具有高度异质性,单个颗粒可能含有多种氧化态,包括Se(0)、Se(IV)和Se(VI)。对样品特征进行了主成分分析,包括 Al2O3、SiO2、CaO、FeO、着火损耗、平均粒度、Se 浓度和 Se 氧化态。研究发现,选择性催化还原(SCR)用于限制煤炭燃烧过程中氮氧化物(NOx)的排放,与硒氧化态降低有关,在采用 SCR 的样品中,硒(0)的含量高达 90%。除 SCR 外,氧化铁含量也可能影响硒的标示。
{"title":"Systematic characterization of selenium speciation in coal fly ash.","authors":"Estefania Garcia, Pan Liu, Sharon E Bone, Yinghao Wen, Yuanzhi Tang","doi":"10.1039/d4em00398e","DOIUrl":"https://doi.org/10.1039/d4em00398e","url":null,"abstract":"<p><p>Millions of tons of coal fly ashes (CFAs) are produced annually during coal combustion in the U.S., which are commonly beneficially used in the concrete industry or disposed of in ash ponds. CFAs contain trace amounts of a range of toxic heavy metals including selenium (Se). Because the toxicity of Se is dependent on its speciation, investigating Se speciation in CFAs as affected by coal source and combustion conditions can help understand the related environmental and human health impacts during disposal or beneficial reuse. In this study, a set of representative CFA samples were characterized for Se speciation using synchrotron X-ray absorption spectroscopy (XAS) and micro-X-ray fluorescence spectromicroscopy (μ-XRF/XAS). Se-containing particles were highly heterogeneous, and individual particles might contain multiple oxidation states including Se(0), Se(IV), and Se(VI). Principal component analysis was performed for sample characteristics including Al<sub>2</sub>O<sub>3</sub>, SiO<sub>2</sub>, CaO, FeO, loss on ignition, average particle size, Se concentration, and Se oxidation state. Selective catalytic reduction (SCR), which is used to limit nitrogen oxide (NO<sub><i>x</i></sub>) emissions during coal combustion, was found to be associated with the presence of reduced Se oxidation states, with up to 90% Se(0) observed in samples with SCR. Alongside SCR, FeO content may also influence Se speciation.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142581064","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kendra Z Hess, Kyle R Forsythe, Xuewen Wang, Andrea Arredondo-Navarro, Gwen Tipling, Jesse Jones, Melissa Mata, Victoria Hughes, Christine Martin, John Doyle, Justin Scott, Matteo Minghetti, Andrea Jilling, José M Cerrato, Eliane El Hayek, Jorge Gonzalez-Estrella
Open dumping and burning of solid waste are widely practiced in underserved communities lacking access to solid waste management facilities; however, the generation of microplastics from these sites has been overlooked. We report elevated concentrations of microplastics (MPs) in soil of three solid waste open dump and burn sites: a single-family site in Tuttle, Oklahoma, USA, and two community-wide sites in Crow Agency and Lodge Grass, Montana, USA. We extracted, quantified, and characterized MPs from two soil depths (0-9 cm and 9-18 cm). The average of abundance of particles found at community-wide sites three sites (18, 460 particles kg-1 soil) equals or exceeds reported concentrations from currently understood sources of MPs including biosolids application and other agricultural practices. Attenuated total reflectance Fourier transformed infrared (ATR-FTIR) identified polyethylene as the dominant polymer across all sites (46.2-84.8%). We also detected rayon (≤11.5%), polystyrene (up to 11.5%), polyethylene terephthalate (≤5.1), polyvinyl chloride (≤4.4%), polyester (≤3.1), and acrylic (≤2.2%). Burned MPs accounted for 76.3 to 96.9% of the MPs found in both community wide dumping sites. These results indicate that solid waste dumping and burning activities are a major source of thermally oxidized MPs for the surrounding terrestrial environment with potential to negatively affect underserved communities.
{"title":"Emerging investigator series: open dumping and burning: an overlooked source of terrestrial microplastics in underserved communities.","authors":"Kendra Z Hess, Kyle R Forsythe, Xuewen Wang, Andrea Arredondo-Navarro, Gwen Tipling, Jesse Jones, Melissa Mata, Victoria Hughes, Christine Martin, John Doyle, Justin Scott, Matteo Minghetti, Andrea Jilling, José M Cerrato, Eliane El Hayek, Jorge Gonzalez-Estrella","doi":"10.1039/d4em00439f","DOIUrl":"10.1039/d4em00439f","url":null,"abstract":"<p><p>Open dumping and burning of solid waste are widely practiced in underserved communities lacking access to solid waste management facilities; however, the generation of microplastics from these sites has been overlooked. We report elevated concentrations of microplastics (MPs) in soil of three solid waste open dump and burn sites: a single-family site in Tuttle, Oklahoma, USA, and two community-wide sites in Crow Agency and Lodge Grass, Montana, USA. We extracted, quantified, and characterized MPs from two soil depths (0-9 cm and 9-18 cm). The average of abundance of particles found at community-wide sites three sites (18, 460 particles kg<sup>-1</sup> soil) equals or exceeds reported concentrations from currently understood sources of MPs including biosolids application and other agricultural practices. Attenuated total reflectance Fourier transformed infrared (ATR-FTIR) identified polyethylene as the dominant polymer across all sites (46.2-84.8%). We also detected rayon (≤11.5%), polystyrene (up to 11.5%), polyethylene terephthalate (≤5.1), polyvinyl chloride (≤4.4%), polyester (≤3.1), and acrylic (≤2.2%). Burned MPs accounted for 76.3 to 96.9% of the MPs found in both community wide dumping sites. These results indicate that solid waste dumping and burning activities are a major source of thermally oxidized MPs for the surrounding terrestrial environment with potential to negatively affect underserved communities.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11533025/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142566396","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ecosystem services play an essential role as intermediaries, linking natural ecosystem resources to socio-economic demands. Understanding their impact on ecological well-being is pivotal for ensuring regional environmental security and promoting sustainable societal and economic development. However, there is insufficient research on the relationship between the two. Accordingly, this study explores the evolutionary relationship between ecological health and ecosystem services by constructing an evaluation system. Regression analysis is used to explore the spatial relationship between ecosystem services and ecological health, providing a reference for maintaining the balance between ecological supply and ecological health. The results show that from 1980 to 2020, an overall improvement was observed in the eco-health index of the Yangtze River Economic Belt's. This improvement was notably marked by substantial growth in the eco-vitality index alongside consistent maintenance of the spatial distribution within the eco-organization index. With regard to distributions of specific ecosystem services, dispersed occurrences characterized areas with high water production and crop yield levels; however, within forested regions, attributes for habitat quality preservation, water purification, soil retention and carbon sequestration were predominant. In the impact of ecosystem services on ecological health, food production held sway over less-developed areas, while soil conservation, water supply and habitat quality exerted greater influence over more-developed regions. This study regards ecosystem services as a bridge connecting humans and the environment not only providing a material basis for society but also reflecting the status of ecological health.
{"title":"How do ecosystem service functions affect ecological health? Evidence from the Yangtze River Economic Belt in China.","authors":"Wei Wang, Jun Yang, Guishan Yang, Chao Wu, Jie Yu","doi":"10.1039/d4em00296b","DOIUrl":"https://doi.org/10.1039/d4em00296b","url":null,"abstract":"<p><p>Ecosystem services play an essential role as intermediaries, linking natural ecosystem resources to socio-economic demands. Understanding their impact on ecological well-being is pivotal for ensuring regional environmental security and promoting sustainable societal and economic development. However, there is insufficient research on the relationship between the two. Accordingly, this study explores the evolutionary relationship between ecological health and ecosystem services by constructing an evaluation system. Regression analysis is used to explore the spatial relationship between ecosystem services and ecological health, providing a reference for maintaining the balance between ecological supply and ecological health. The results show that from 1980 to 2020, an overall improvement was observed in the eco-health index of the Yangtze River Economic Belt's. This improvement was notably marked by substantial growth in the eco-vitality index alongside consistent maintenance of the spatial distribution within the eco-organization index. With regard to distributions of specific ecosystem services, dispersed occurrences characterized areas with high water production and crop yield levels; however, within forested regions, attributes for habitat quality preservation, water purification, soil retention and carbon sequestration were predominant. In the impact of ecosystem services on ecological health, food production held sway over less-developed areas, while soil conservation, water supply and habitat quality exerted greater influence over more-developed regions. This study regards ecosystem services as a bridge connecting humans and the environment not only providing a material basis for society but also reflecting the status of ecological health.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556588","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The Bioconcentration Factor (BCF) is used to evaluate the bioaccumulation potential of chemical substances in reference organisms, and it directly correlates with ecotoxicity. Traditional in vivo BCF estimation methods are costly, time-consuming, and involve animal sacrifice. Many in silico technologies are used to avoid the problems associated with in vivo testing. This study aims to develop a quantitative read across structure-property relationship (q-RASPR) model using a structurally diverse dataset consisting of 1303 compounds by combining quantitative structure-property relationship (QSPR) and read-across (RA) algorithms. The model incorporates simple, interpretable, and reproducible 2D molecular descriptors along with RASAR descriptors. The PLS-based q-RASPR model demonstrated robust performance with internal validation metrics (R2 = 0.727 and Q2(LOO) = 0.723) and external validation metrics (Q2F1 = 0.739, Q2F2 = 0.739, and CCC = 0.858). These results indicate that the q-RASPR model is statistically superior to the corresponding QSPR model. Furthermore, screening of 1694 compounds from the Pesticide Properties Database (PPDB) was performed using the PLS-based q-RASPR model for assessing the eco-toxicological bioaccumulative potential of various compounds, ensuring the external predictability of the developed model and confirming the real-world application of the developed model. This model offers a reliable tool for predicting the BCF of new or untested compounds, thereby helping to develop safe and environment-friendly chemicals.
{"title":"Quantitative read-across structure-property relationship (q-RASPR): a novel approach to estimate the bioaccumulative potential for diverse classes of industrial chemicals in aquatic organisms.","authors":"Prodipta Bhattacharyya, Pabitra Samanta, Ankur Kumar, Shubha Das, Probir Kumar Ojha","doi":"10.1039/d4em00374h","DOIUrl":"https://doi.org/10.1039/d4em00374h","url":null,"abstract":"<p><p>The Bioconcentration Factor (BCF) is used to evaluate the bioaccumulation potential of chemical substances in reference organisms, and it directly correlates with ecotoxicity. Traditional <i>in vivo</i> BCF estimation methods are costly, time-consuming, and involve animal sacrifice. Many <i>in silico</i> technologies are used to avoid the problems associated with <i>in vivo</i> testing. This study aims to develop a quantitative read across structure-property relationship (q-RASPR) model using a structurally diverse dataset consisting of 1303 compounds by combining quantitative structure-property relationship (QSPR) and read-across (RA) algorithms. The model incorporates simple, interpretable, and reproducible 2D molecular descriptors along with RASAR descriptors. The PLS-based q-RASPR model demonstrated robust performance with internal validation metrics (<i>R</i><sup>2</sup> = 0.727 and <i>Q</i><sup>2</sup><sub>(LOO)</sub> = 0.723) and external validation metrics (<i>Q</i><sup>2</sup><sub>F1</sub> = 0.739, <i>Q</i><sup>2</sup><sub>F2</sub> = 0.739, and CCC = 0.858). These results indicate that the q-RASPR model is statistically superior to the corresponding QSPR model. Furthermore, screening of 1694 compounds from the Pesticide Properties Database (PPDB) was performed using the PLS-based q-RASPR model for assessing the eco-toxicological bioaccumulative potential of various compounds, ensuring the external predictability of the developed model and confirming the real-world application of the developed model. This model offers a reliable tool for predicting the BCF of new or untested compounds, thereby helping to develop safe and environment-friendly chemicals.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556590","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The escalating presence of microplastic pollution poses a significant environmental threat, with far-reaching implications for both ecosystems and human health. This study investigated the toxicological impact of polyethylene microplastics (PE MPs) using Drosophila melanogaster, fruit flies, as a model organism. Drosophila were exposed to PE MPs orally at concentrations of 1 mg ml-1 and 10 mg ml-1 agar food. The study assessed behavioural parameters and biochemical markers including reactive oxygen species (ROS), superoxide dismutase (SOD), and glutathione-S-transferase (GST) activity. The expression levels of key genes (Hsp70Bc, rpr, and p53) were also analysed using the RT-qPCR technique. Results indicated a significant decline in climbing activity among adult flies and crawling behaviour in larvae, indicating potential disruption of motor function. Biochemical analysis revealed elevated ROS levels, indicative of oxidative stress, in both larval and fly stages. Moreover, the antioxidant defence system exhibited decreased SOD activity and a concentration-dependent increase in GST activity indicating the functioning of a quick xenobiotic clearance mechanism. Gene expression analysis demonstrated upregulation of rpr, p53, and Hsp70Bc genes, suggesting activation of cell death pathways and stress response mechanisms. Overall, these findings underline the adverse effects of PE MPs on Drosophila, including behavioural impairment, oxidative stress, and activation of stress response pathways.
{"title":"Polyethylene microplastics affect behavioural, oxidative stress, and molecular responses in the <i>Drosophila</i> model.","authors":"Himanshu Ranjan, Swetha Senthil Kumar, Sharine Priscilla, Subhashini Swaminathan, Masakazu Umezawa, Sahabudeen Sheik Mohideen","doi":"10.1039/d4em00537f","DOIUrl":"https://doi.org/10.1039/d4em00537f","url":null,"abstract":"<p><p>The escalating presence of microplastic pollution poses a significant environmental threat, with far-reaching implications for both ecosystems and human health. This study investigated the toxicological impact of polyethylene microplastics (PE MPs) using <i>Drosophila melanogaster</i>, fruit flies, as a model organism. <i>Drosophila</i> were exposed to PE MPs orally at concentrations of 1 mg ml<sup>-1</sup> and 10 mg ml<sup>-1</sup> agar food. The study assessed behavioural parameters and biochemical markers including reactive oxygen species (ROS), superoxide dismutase (SOD), and glutathione-<i>S</i>-transferase (GST) activity. The expression levels of key genes (<i>Hsp70Bc</i>, <i>rpr</i>, and <i>p53</i>) were also analysed using the RT-qPCR technique. Results indicated a significant decline in climbing activity among adult flies and crawling behaviour in larvae, indicating potential disruption of motor function. Biochemical analysis revealed elevated ROS levels, indicative of oxidative stress, in both larval and fly stages. Moreover, the antioxidant defence system exhibited decreased SOD activity and a concentration-dependent increase in GST activity indicating the functioning of a quick xenobiotic clearance mechanism. Gene expression analysis demonstrated upregulation of <i>rpr</i>, <i>p53</i>, and <i>Hsp70Bc</i> genes, suggesting activation of cell death pathways and stress response mechanisms. Overall, these findings underline the adverse effects of PE MPs on <i>Drosophila</i>, including behavioural impairment, oxidative stress, and activation of stress response pathways.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Leigh R Crilley, Jenna C Ditto, Melodie Lao, Zilin Zhou, Jonathan P D Abbatt, Arthur W H Chan, Trevor C VandenBoer
Gas-phase reactive nitrogen species (Nr) are important drivers of indoor air quality. Cooking and cleaning are significant direct sources indoors, whose emissions will vary depending on activity and materials used. Commercial kitchens experience regular high volumes of both cooking and cleaning, making them ideal study locations for exploring emission factors from these sources. Here, we present a total Nr (tNr) budget and contributions of key species NO, NO2, acidic Nr (primarily HONO) and basic Nr (primarily NH3) using novel instrumentation in a commercial kitchen over a two-week period. In general, highest tNr was observed in the morning and driven compositionally by NO, indicative of cooking events in the kitchen. The observed HONO and basic Nr levels were unexpectedly stable throughout the day, despite the dynamic and high air change rate in the kitchen. After summing the measured NOx, HONO and Nr,base fractions, there was on average 5 ppbv of Nr unaccounted for, expected to be dominated by neutral Nr species. Using co-located measurements from a proton transfer reaction mass spectrometer (PTR-MS), we propose the identities for these major Nr species from cooking and cleaning that contributed to Nr,base and the neutral fraction of tNr. When focused specifically on cooking events in the kitchen, a vast array of N-containing species was observed by the PTR-MS. Reproducibly, oxygenated N-containing class ions (C1-12H3-24O1-4N1-3), consistent with the known formulae of amides, were observed during meat cooking and may be good cooking tracers. During cleaning, an unexpectedly high level of chloramines was observed, with monochloramine dominating the profile, as emitted directly from HOCl based cleaners or through surface reactions with reduced-N species. For many species within the tNr budget, including HONO, acetonitrile and basic Nr species, we observed stable levels day and night despite the high air change rate during the day (>27 h-1). The stable levels for these species point to large surface reservoirs which act as a significant indoor source, that will be transported outdoors with ventilation.
气相活性氮物种(Nr)是影响室内空气质量的重要因素。烹饪和清洁是室内的重要直接来源,其排放量会因活动和使用的材料而异。商业厨房经常会有大量的烹饪和清洁活动,因此是探索这些来源的排放因子的理想研究场所。在此,我们使用新型仪器对商业厨房进行了为期两周的检测,得出了总氮氧化物(tNr)预算以及主要物种一氧化氮(NO)、二氧化氮(NO2)、酸性氮氧化物(主要是 HONO)和碱性氮氧化物(主要是 NH3)的贡献。一般来说,在上午观测到的 tNr 最高,由氮氧化物(NO)驱动,表明厨房里有烹饪活动。尽管厨房内的空气变化率很高,但全天观测到的 HONO 和基本 Nr 水平却出乎意料地稳定。将测量到的 NOx、HONO 和 Nr、碱组分相加后,平均有 5 ppbv 的 Nr 未被计算在内,预计主要是中性 Nr 物种。利用质子转移反应质谱仪(PTR-MS)的同位测量,我们提出了烹饪和清洁过程中产生的这些主要 Nr 物种的特性,这些 Nr 物种对 Nr 碱和 tNr 的中性部分有贡献。当特别关注厨房中的烹饪活动时,PTR-MS 观察到了大量含氮物质。在肉类烹饪过程中,可重复观察到含氧 N 类离子(C1-12H3-24O1-4N1-3),与已知的酰胺分子式一致,可能是很好的烹饪示踪剂。在清洁过程中,观察到氯胺的含量出乎意料地高,其中一氯胺占主导地位,它直接从基于 HOCl 的清洁剂中释放出来,或通过与还原 N 物种的表面反应释放出来。对于 tNr 预算中的许多物种,包括 HONO、乙腈和碱性 Nr 物种,尽管白天的换气率很高(>27 h-1),但我们还是观测到了日夜稳定的水平。这些物种的稳定水平表明,有大量的地表储层是重要的室内源,它们会随着通风被带到室外。
{"title":"Commercial kitchen operations produce a diverse range of gas-phase reactive nitrogen species.","authors":"Leigh R Crilley, Jenna C Ditto, Melodie Lao, Zilin Zhou, Jonathan P D Abbatt, Arthur W H Chan, Trevor C VandenBoer","doi":"10.1039/d4em00491d","DOIUrl":"https://doi.org/10.1039/d4em00491d","url":null,"abstract":"<p><p>Gas-phase reactive nitrogen species (N<sub>r</sub>) are important drivers of indoor air quality. Cooking and cleaning are significant direct sources indoors, whose emissions will vary depending on activity and materials used. Commercial kitchens experience regular high volumes of both cooking and cleaning, making them ideal study locations for exploring emission factors from these sources. Here, we present a total N<sub>r</sub> (tN<sub>r</sub>) budget and contributions of key species NO, NO<sub>2</sub>, acidic N<sub>r</sub> (primarily HONO) and basic N<sub>r</sub> (primarily NH<sub>3</sub>) using novel instrumentation in a commercial kitchen over a two-week period. In general, highest tN<sub>r</sub> was observed in the morning and driven compositionally by NO, indicative of cooking events in the kitchen. The observed HONO and basic N<sub>r</sub> levels were unexpectedly stable throughout the day, despite the dynamic and high air change rate in the kitchen. After summing the measured NO<sub><i>x</i></sub>, HONO and N<sub>r,base</sub> fractions, there was on average 5 ppbv of N<sub>r</sub> unaccounted for, expected to be dominated by neutral N<sub>r</sub> species. Using co-located measurements from a proton transfer reaction mass spectrometer (PTR-MS), we propose the identities for these major N<sub>r</sub> species from cooking and cleaning that contributed to N<sub>r,base</sub> and the neutral fraction of tN<sub>r</sub>. When focused specifically on cooking events in the kitchen, a vast array of N-containing species was observed by the PTR-MS. Reproducibly, oxygenated N-containing class ions (C<sub>1-12</sub>H<sub>3-24</sub>O<sub>1-4</sub>N<sub>1-3</sub>), consistent with the known formulae of amides, were observed during meat cooking and may be good cooking tracers. During cleaning, an unexpectedly high level of chloramines was observed, with monochloramine dominating the profile, as emitted directly from HOCl based cleaners or through surface reactions with reduced-N species. For many species within the tN<sub>r</sub> budget, including HONO, acetonitrile and basic N<sub>r</sub> species, we observed stable levels day and night despite the high air change rate during the day (>27 h<sup>-1</sup>). The stable levels for these species point to large surface reservoirs which act as a significant indoor source, that will be transported outdoors with ventilation.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-11-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142556587","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Fragrant personal care products are a subset of volatile chemical products (VCPs), an emerging source of outdoor pollutants capable of impacting air quality. Fragrant molecules, such as musks, are used in perfumes and have been found in aquatic organisms, water bodies, indoor air, and urban environments. Considering the distribution of musk-smelling compounds, there is a need to constrain their atmospheric fate indoors and outdoors. Here, we used a Vocus proton-transfer-reaction time-of-flight mass spectrometer to quantify the atmospheric oxidative fate of cashmeran, a bicyclic musk compound, detected in a commercial perfume alongside galaxolide, astratone and rosamusk. Cashmeran concentrations rose up to 0.35 ppbv representing a mass yield of 0.33 ± 0.04% of the perfume. We determined the second order rate constant of the cyclo-addition of O3 with cashmeran to be (2.78 ± 0.31) × 10-19 cm3 molec-1 s-1 at 293 ± 1 K in N2. This rate constant corresponds to an 85 day lifetime against 20 ppbv of O3. Then, we repeated the ozonolysis experiments in air with 20% O2 and measured significant secondary OH concentrations up to 5.1 × 105 molec cm-3. Consequently, the lifetime of cashmeran in our experiment was shortened to 5 h. Thus, the oxidation of fragrant molecules, like cashmeran, could alter the oxidative capacity of indoor air via the production of secondary OH radicals. Furthermore, our results show that cashmeran is long-lived and could serve as a VCP tracer in urban air.
{"title":"The gas phase ozonolysis and secondary OH production of cashmeran, a musk compound from fragrant volatile chemical products.","authors":"Ayomide A Akande, Nadine Borduas-Dedekind","doi":"10.1039/d4em00452c","DOIUrl":"https://doi.org/10.1039/d4em00452c","url":null,"abstract":"<p><p>Fragrant personal care products are a subset of volatile chemical products (VCPs), an emerging source of outdoor pollutants capable of impacting air quality. Fragrant molecules, such as musks, are used in perfumes and have been found in aquatic organisms, water bodies, indoor air, and urban environments. Considering the distribution of musk-smelling compounds, there is a need to constrain their atmospheric fate indoors and outdoors. Here, we used a Vocus proton-transfer-reaction time-of-flight mass spectrometer to quantify the atmospheric oxidative fate of cashmeran, a bicyclic musk compound, detected in a commercial perfume alongside galaxolide, astratone and rosamusk. Cashmeran concentrations rose up to 0.35 ppbv representing a mass yield of 0.33 ± 0.04% of the perfume. We determined the second order rate constant of the cyclo-addition of O<sub>3</sub> with cashmeran to be (2.78 ± 0.31) × 10<sup>-19</sup> cm<sup>3</sup> molec<sup>-1</sup> s<sup>-1</sup> at 293 ± 1 K in N<sub>2</sub>. This rate constant corresponds to an 85 day lifetime against 20 ppbv of O<sub>3</sub>. Then, we repeated the ozonolysis experiments in air with 20% O<sub>2</sub> and measured significant secondary OH concentrations up to 5.1 × 10<sup>5</sup> molec cm<sup>-3</sup>. Consequently, the lifetime of cashmeran in our experiment was shortened to 5 h. Thus, the oxidation of fragrant molecules, like cashmeran, could alter the oxidative capacity of indoor air <i>via</i> the production of secondary OH radicals. Furthermore, our results show that cashmeran is long-lived and could serve as a VCP tracer in urban air.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-10-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142542945","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Guijuan Li, Yan Cheng, Mengyao Jing, Dan Zhang, Yufei Ma, Shengke Yang
This study thoroughly investigated the degradation of norfloxacin (NOR) under the influence of micro-nanobubbles (MNBs) and sodium hypochlorite (NaClO), focusing on their synergistic effects. The impact of various environmental factors, including NaClO concentration, pH, inorganic anions, and surfactants, on NOR degradation efficiency within the MNBs/NaClO system was systematically assessed. The basic properties of the MNBs/NaClO system and the degradation kinetics of NOR were explored. The degradation products and pathways of NOR were explored to reveal the degradation mechanism of antibiotics in the MNBs/NaClO system by employing density functional theory (DFT) and high-performance liquid chromatography-mass spectrometry (HPLC-MS). The redox potential of the MNBs/NaClO system exhibited significantly superior properties than the single system, with bubble sizes predominantly in the nanoscale. The degradation kinetics of NOR adhered to a pseudo-first-order reaction model, with optimal degradation occurring at a 0.025% NaClO volume concentration. Acidic conditions promoted the degradation of NOR, and alkaline conditions inhibited the degradation of NOR. Inorganic anions PO43-, HCO3-, and CO32- in the water matrix led to strong inhibition of NOR degradation. Cationic surfactants accelerated the degradation process of NOR, while anionic and nonionic surfactants had a consistent inhibitory effect on the degradation of NOR. Based on the degradation behavior, three potential pathways for NOR degradation were proposed: quinolone group transformation, defluorination reaction, piperazine ring cracking and quinolone ring decomposition. This research contributes a novel technical approach for addressing antibiotic pollution and offers a theoretical framework for understanding the fate of antibiotics in the environment.
本研究深入研究了诺氟沙星(NOR)在微纳米气泡(MNBs)和次氯酸钠(NaClO)影响下的降解过程,重点关注它们之间的协同效应。系统评估了各种环境因素(包括 NaClO 浓度、pH 值、无机阴离子和表面活性剂)对 MNBs/NaClO 系统中 NOR 降解效率的影响。探讨了 MNBs/NaClO 系统的基本特性和 NOR 的降解动力学。利用密度泛函理论(DFT)和高效液相色谱-质谱联用技术(HPLC-MS),探索了 NOR 的降解产物和降解途径,从而揭示了抗生素在 MNBs/NaClO 体系中的降解机理。与单一体系相比,MNBs/NaClO 体系的氧化还原电位表现出明显的优越性,气泡尺寸主要在纳米级。NOR 的降解动力学遵循伪一阶反应模型,最佳降解发生在 NaClO 体积浓度为 0.025% 时。酸性条件促进 NOR 的降解,碱性条件抑制 NOR 的降解。水基质中的无机阴离子 PO43-、HCO3- 和 CO32- 强烈抑制了 NOR 的降解。阳离子表面活性剂加速了 NOR 的降解过程,而阴离子和非离子表面活性剂对 NOR 的降解具有一致的抑制作用。根据降解行为,提出了 NOR 降解的三种潜在途径:喹诺酮基团转化、脱氟反应、哌嗪环裂解和喹诺酮环分解。这项研究为解决抗生素污染问题提供了一种新的技术方法,并为了解抗生素在环境中的归宿提供了一个理论框架。
{"title":"Degradation of norfloxacin by the synergistic effect of micro-nano bubbles and sodium hypochlorite: kinetics, influencing factors and pathways.","authors":"Guijuan Li, Yan Cheng, Mengyao Jing, Dan Zhang, Yufei Ma, Shengke Yang","doi":"10.1039/d4em00490f","DOIUrl":"10.1039/d4em00490f","url":null,"abstract":"<p><p>This study thoroughly investigated the degradation of norfloxacin (NOR) under the influence of micro-nanobubbles (MNBs) and sodium hypochlorite (NaClO), focusing on their synergistic effects. The impact of various environmental factors, including NaClO concentration, pH, inorganic anions, and surfactants, on NOR degradation efficiency within the MNBs/NaClO system was systematically assessed. The basic properties of the MNBs/NaClO system and the degradation kinetics of NOR were explored. The degradation products and pathways of NOR were explored to reveal the degradation mechanism of antibiotics in the MNBs/NaClO system by employing density functional theory (DFT) and high-performance liquid chromatography-mass spectrometry (HPLC-MS). The redox potential of the MNBs/NaClO system exhibited significantly superior properties than the single system, with bubble sizes predominantly in the nanoscale. The degradation kinetics of NOR adhered to a pseudo-first-order reaction model, with optimal degradation occurring at a 0.025% NaClO volume concentration. Acidic conditions promoted the degradation of NOR, and alkaline conditions inhibited the degradation of NOR. Inorganic anions PO<sub>4</sub><sup>3-</sup>, HCO<sub>3</sub><sup>-</sup>, and CO<sub>3</sub><sup>2-</sup> in the water matrix led to strong inhibition of NOR degradation. Cationic surfactants accelerated the degradation process of NOR, while anionic and nonionic surfactants had a consistent inhibitory effect on the degradation of NOR. Based on the degradation behavior, three potential pathways for NOR degradation were proposed: quinolone group transformation, defluorination reaction, piperazine ring cracking and quinolone ring decomposition. This research contributes a novel technical approach for addressing antibiotic pollution and offers a theoretical framework for understanding the fate of antibiotics in the environment.</p>","PeriodicalId":74,"journal":{"name":"Environmental Science: Processes & Impacts","volume":null,"pages":null},"PeriodicalIF":4.3,"publicationDate":"2024-10-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142520365","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}