IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c06697

Craig R. Jensen, David P. Genereux, D. Kip Solomon, Detlef R. U. Knappe, Troy E. Gilmore

{"title":"Forecasting and Hindcasting PFAS Concentrations in Groundwater Discharging to Streams near a PFAS Production Facility","authors":"Craig R. Jensen, David P. Genereux, D. Kip Solomon, Detlef R. U. Knappe, Troy E. Gilmore","doi":"10.1021/acs.est.4c06697","DOIUrl":"https://doi.org/10.1021/acs.est.4c06697","url":null,"abstract":"Per- and polyfluoroalkyl substances (PFAS) are known to be highly persistent in groundwater, making it vital to develop new approaches to important practical questions such as the time scale for future persistence of PFAS in contaminated groundwater. In the approach presented here, groundwater from beneath streambeds was analyzed for PFAS and age-dated using SF6 and 3H/3He. The results were coupled with groundwater flux measurements in a convolution approach to estimate past and future PFAS concentrations in groundwater discharge to the streams. At our test site near the Cape Fear River (CFR) of North Carolina, PFAS were detected in groundwater up to 43 years old, suggesting that some PFAS entered groundwater immediately or shortly after fluorochemical production began at the nearby Fayetteville Works. Results are consistent with little to no retardation in groundwater for perfluoroethers such as hexafluoropropylene oxide-dimer acid (HFPO–DA) and perfluoro-2-methoxypropanoic acid (PMPA), the two most abundant PFAS, with mean concentrations of 229 and 498 ng/L, respectively. Future PFAS concentrations in groundwater discharge to streams were estimated to remain above current MCL or health advisory levels through at least 2050 or 2060 (using 3H/3He and SF6, respectively). Recent atmospheric deposition data suggest lower but non-negligible amounts of PFAS may continue to enter groundwater, likely further extending PFAS persistence in groundwater and the adjacent CFR. This approach shows promise for giving an overall perspective on persistence of PFAS in groundwater discharge from a broad contaminated area.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317209","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Transcriptome-Guided Characterization of the Environmental Toxicity of Metformin: Disruption of Energy Homeostasis and Inhibition of Embryonic Development of Zebrafish at Environmentally Relevant Concentrations 转录组引导下的二甲双胍环境毒性表征：在环境相关浓度下破坏斑马鱼的能量平衡并抑制其胚胎发育

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-25 DOI: 10.1021/acs.est.4c05052

Ziyu Zhang, Haochun Shi, Kun Zhang, Ruiqi An, Congcong Wang, Peng Wang, Shen-An Chan, Yue Song, Jiayin Dai, Yanbin Zhao

{"title":"Transcriptome-Guided Characterization of the Environmental Toxicity of Metformin: Disruption of Energy Homeostasis and Inhibition of Embryonic Development of Zebrafish at Environmentally Relevant Concentrations","authors":"Ziyu Zhang, Haochun Shi, Kun Zhang, Ruiqi An, Congcong Wang, Peng Wang, Shen-An Chan, Yue Song, Jiayin Dai, Yanbin Zhao","doi":"10.1021/acs.est.4c05052","DOIUrl":"https://doi.org/10.1021/acs.est.4c05052","url":null,"abstract":"Metformin has been widely detected in aquatic ecosystems, yet the knowledge of its impact on aquatic organisms, particularly at environmentally relevant concentrations, remains limited. In the present study, we characterized the developmental toxicity of metformin in zebrafish, utilizing a transcriptome-guided toxicological assessment framework. Transcriptomic analysis conducted at metformin concentrations within the μg/L range revealed significant disruptions in biological processes associated with nucleotide, hydrocarbon, and amino acid metabolism, suggesting a significant disturbance in energy homeostasis. This observation was corroborated by energy-targeted metabolomic analysis, wherein a considerable number of metabolites involved in purine metabolism, pyrimidine metabolism, and the citrate cycle displayed significant alterations. Notably, most intermediates in the citrate cycle such as acetyl-CoA exhibited remarkable decreases. Additionally, our study identified significant impediments in zebrafish embryonic development, including decreased yolk extension progress, spontaneous contraction and body length, and increased yolk sac area and yolk/while body lipid content ratio, at metformin concentrations as low as 0.12 μg/L. Furthermore, the disruption of energy homeostasis by metformin was observed to persist into adulthood even after a prolonged recovery period. The present findings highlighted the disruptive effects of metformin on energy homeostasis and embryonic development in teleost at environmentally relevant concentrations, thereby prompting a reevaluation of its environmental risk to nontarget aquatic organisms.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317171","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Regulation of Ocean Surface Currents and Seasonal Sea Ice Variations on the Occurrence and Transport of Organophosphate Esters in the Central Arctic Ocean. 海洋表层流和季节性海冰变化对北冰洋中部有机磷酸酯发生和迁移的调控。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c05620

Jinghua Zhang, Yuxin Ma, Peigen Lin, Minghong Cai

{"title":"Regulation of Ocean Surface Currents and Seasonal Sea Ice Variations on the Occurrence and Transport of Organophosphate Esters in the Central Arctic Ocean.","authors":"Jinghua Zhang, Yuxin Ma, Peigen Lin, Minghong Cai","doi":"10.1021/acs.est.4c05620","DOIUrl":"https://doi.org/10.1021/acs.est.4c05620","url":null,"abstract":"Organophosphate esters (OPEs) have been observed in the remote Arctic Ocean, yet the influence of hydrodynamics and seasonal sea ice variations on the occurrence and transport of waterborne OPEs remains unclear. This study comprehensively examines OPEs in surface seawater of the central Arctic Ocean during the summer of 2020, integrating surface ocean current and sea ice concentration data. The results confirm significant spatiotemporal variations of the OPEs, with the total concentration of seven major OPEs averaging 780 ± 970 pg/L. Chlorinated OPEs, particularly tris(1-chloro-2-propyl) phosphate (TCPP), were dominant. The significant impact of hydrodynamics on the OPE transport is demonstrated by higher OPE concentrations in regions with strong surface currents, especially at the edge of the Beaufort Gyre and the confluence of the Beaufort Gyre and the Transpolar Drift. Furthermore, OPE levels were generally higher in drifting-ice-covered regions compared to ice-free regions, attributed to the volatilization of dissolved OPEs formerly trapped below the sea ice or newly released from melting snow and sea ice. Notably, TCPP decreased by only 19% in the ice-free area, while the more volatile triphenyl phosphate decreased by 63% compared with the partial ice region.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306565","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Impact of Biotransformation on Internal Concentrations and Specificity Classification of Organic Chemicals in the Zebrafish Embryo (Danio rerio). 生物转化对斑马鱼胚胎（Danio rerio）中有机化学品内部浓度和特异性分类的影响。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c04156

Nico Grasse, Riccardo Massei, Bettina Seiwert, Stefan Scholz, Beate I Escher, Thorsten Reemtsma, Qiuguo Fu

{"title":"Impact of Biotransformation on Internal Concentrations and Specificity Classification of Organic Chemicals in the Zebrafish Embryo (Danio rerio).","authors":"Nico Grasse, Riccardo Massei, Bettina Seiwert, Stefan Scholz, Beate I Escher, Thorsten Reemtsma, Qiuguo Fu","doi":"10.1021/acs.est.4c04156","DOIUrl":"https://doi.org/10.1021/acs.est.4c04156","url":null,"abstract":"Internal concentrations (ICs) are crucial for linking exposure to effects in the development of New Approach Methodologies. ICs of chemicals in aquatic organisms are primarily driven by hydrophobicity and modulated by biotransformation and efflux. Comparing the predicted baseline to observed toxicity enables the estimation of effect specificity, but biological processes can lead to overestimating ICs and bias the specificity assessment. To evaluate the prediction of a mass balance model (MBM) and the impact of biotransformation on ICs, experimental ICs of 63 chemicals in zebrafish embryos were compared to predictions with physicochemical properties as input parameters. Experimental ICs of 79% (50 of 63) of the chemicals deviated less than 10-fold from predictions, and the remaining 13 deviated up to a factor of 90. Using experimental ICs changed the classification for 19 chemicals, with ICs 5 to 90 times lower than predicted, showing the bias of specificity classification. Uptake kinetics of pirinixic acid, genistein, dexamethasone, ethoprophos, atorvastatin, and niflumic acid were studied over a 96 h exposure period, and transformation products (TPs) were elucidated using suspect- and nontarget screening with UPLC-HRMS. 35 TPs (5 to 8 TPs per compound) were tentatively identified and semiquantified based on peak areas, suggesting that biotransformation may partly account for the overpredictions of ICs.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306563","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Integrating Transcriptome and Metabolome Analyses Revealed Salinity Induces Arsenobetaine Biosynthesis in Marine Medaka (Oryzias melastigma) 整合转录组和代谢组分析揭示盐度诱导海青蛙（Oryzias melastigma）砷甜菜碱的生物合成

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c07382

Le Zhang, Liping Huang, Zijun Ye, Ke Pan, Zhu Xiong, Jian-You Long, Gaosheng Zhang, Yunxue Guo, Wei Zhang

{"title":"Integrating Transcriptome and Metabolome Analyses Revealed Salinity Induces Arsenobetaine Biosynthesis in Marine Medaka (Oryzias melastigma)","authors":"Le Zhang, Liping Huang, Zijun Ye, Ke Pan, Zhu Xiong, Jian-You Long, Gaosheng Zhang, Yunxue Guo, Wei Zhang","doi":"10.1021/acs.est.4c07382","DOIUrl":"https://doi.org/10.1021/acs.est.4c07382","url":null,"abstract":"Marine fish exhibit elevated levels of arsenobetaine (AsB), while the impact and underlying mechanism of salinity on AsB biosynthesis remain inadequately explored. In this study, marine medaka (Oryzias melastigma), typically inhabiting 30‰ high salinity, were gradually acclimated to low salinities of 20, 10, and 0‰. Following acclimation, the fish were exposed to arsenate (As(V)) in their diet for 30 days. Results showed a significant accumulation of total arsenic (As) and AsB concentrations in the muscle and head tissues of the exposed fish, with these accumulations exhibiting a positive correlation with water salinity. Transcriptome analyses revealed that exposure to As(V) at low salinity may disrupt membrane components and induce cytoskeletal injuries, while at high salinity, it triggered oxidoreductase activity and transmembrane transport. Metabolome analyses indicated that low salinity induced osmotic stress, resulting in an increased requirement for amino acids to upload intracellular osmotic equilibrium in O. melastigma. Furthermore, the key organic osmolytes and amino acids, including taurine, l-methionine, guanidinoethyl sulfonate, and N-acetyl-l-aspartic acid, exhibited a negative correlation with the AsB concentration. These findings indicated that salinity can regulate osmotic balance by influencing amino acid synthesis under low salinity and stimulating AsB synthesis under high salinity conditions in O. melastigma. This study provides insights into the impact of high salinity on AsB biosynthesis, the underlying regulatory mechanisms, and implications for managing As(V) risk.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142314022","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Facilitating Intracellular Electron Bifurcation by Mediating Flavin-Based Extracellular and Transmembrane Electron Transfer: A Novel Role of Pyrogenic Carbon in Dark Fermentation for Hydrogen Production. 通过介导基于黄素的胞外和跨膜电子传递促进细胞内电子分叉：热原碳在黑暗发酵制氢中的新作用。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c05994

Wenjing Tian, Yanfei Tang, Thomas F Ducey, Eakalak Khan, Daniel C W Tsang

{"title":"Facilitating Intracellular Electron Bifurcation by Mediating Flavin-Based Extracellular and Transmembrane Electron Transfer: A Novel Role of Pyrogenic Carbon in Dark Fermentation for Hydrogen Production.","authors":"Wenjing Tian, Yanfei Tang, Thomas F Ducey, Eakalak Khan, Daniel C W Tsang","doi":"10.1021/acs.est.4c05994","DOIUrl":"https://doi.org/10.1021/acs.est.4c05994","url":null,"abstract":"Pyrogenic carbon is considered an enhancer to H2-yielding dark fermentation (DF), but little is known about how it regulates extracellular electron transfer (EET) and influences transmembrane respiratory chains and intracellular metabolisms. This study addressed these knowledge gaps and demonstrated that wood waste pyrogenic carbon (biochar) could significantly improve the DF performance; e.g., addition of pyrogenic carbon produced by pyrolysis at 800 °C (PC800) increased H2 yield by 369.7%. Biochemical quantification, electrochemical analysis, and electron respiratory chain inhibition tests revealed that PC800 promoted the extracellular flavin-based electron transfer process and further activated the acceleration of the transmembrane electron transfer. Comparative metagenome/metatranscriptome analyses indicated that the flavin-containing Rnf complex was the potential transmembrane respiratory enzyme associated with PC800-mediated EET. Based on NADH/NAD+ circulation, the promoted Rnf complex could stimulate the functions of the electron bifurcating Etf/Bcd complex and startup of glycolysis. The promoted Etf/Bcd could further contribute to balance the NADH/NAD+ level for glycolytic reactions and meanwhile provide reduced ferredoxin for group A1 [FeFe]-hydrogenases. This proton-energy-linked mechanism could achieve coupling production of ATP and H2. This study verified the important roles of pyrogenic carbon in mediating EET and transmembrane/intracellular pathways and revealed the crucial roles of electron bifurcation in DF for hydrogen production.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306560","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Identification of Primary Organophosphate Esters Contributing to Enhanced Risk of Gestational Diabetes Mellitus Based on a Case-Control Study. 基于病例对照研究，确定导致妊娠糖尿病风险增加的主要有机磷酯类化合物。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c04180

Yun Deng, Shujun Yi, Wenya Liu, Liping Yang, Lingyan Zhu, Qiang Zhang, Hangbiao Jin, Rongyan Yang, Rouyi Wang, Nai-Jun Tang

{"title":"Identification of Primary Organophosphate Esters Contributing to Enhanced Risk of Gestational Diabetes Mellitus Based on a Case-Control Study.","authors":"Yun Deng, Shujun Yi, Wenya Liu, Liping Yang, Lingyan Zhu, Qiang Zhang, Hangbiao Jin, Rongyan Yang, Rouyi Wang, Nai-Jun Tang","doi":"10.1021/acs.est.4c04180","DOIUrl":"https://doi.org/10.1021/acs.est.4c04180","url":null,"abstract":"Epidemiological studies on associations of organophosphate ester (OPE) exposure and gestational diabetes mellitus (GDM) risk, which remain rare and inconclusive, were carried out with a case-control population comprising 287 GDM and 313 non-GDM pregnant women recruited from Tianjin. The GDM group suffered distinctly higher serum concentrations of tri-n-butyl phosphate (TNBP), tri(2-butoxyethyl) phosphate (TBOEP), triphenyl phosphate (TPHP), tri-iso-propyl phosphate (TIPP), and tri(1-chloro-2-propyl) phosphate (TCIPP) than the healthy control group (p < 0.001). Traditional analysis methods employed for either individual or mixture effects found positive correlations (p < 0.05) between the concentrations of five OPEs (i.e., TNBP, TBOEP, TPHP, TIPP, and TCIPP) and the incidence of GDM, while 2-ethylhexyl diphenyl phosphate, tri(1-chloro-2-propyl) phosphate, and bis(2-ethylhexyl) phosphate exhibited opposite effects. Three machine learning methods considering the concurrence of OPE mixture exposure and population characteristics were applied to clarify their relative importance to GDM risk, among which random forest performed the best. Several OPEs, particularly TNBP and TBOEP ranking at the top, made greater contributions than some demographical characteristics, such as prepregnancy body mass index and family history of diabetes, to the occurrence of GDM. This was further validated by another independent case-control population obtained from Hangzhou.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Bioaccumulation of Atmospherically Deposited Cadmium in Soybean: Three-Year Field Experiment Combined with Cadmium Isotopes 大气沉积镉在大豆中的生物累积：结合镉同位素的三年田间试验

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c07961

Hailong Liu, Xiuting Rong, Huan Zhao, Ruizhi Xia, Min Li, Haotian Wang, Hongbiao Cui, Xiaozhi Wang, Jun Zhou

{"title":"Bioaccumulation of Atmospherically Deposited Cadmium in Soybean: Three-Year Field Experiment Combined with Cadmium Isotopes","authors":"Hailong Liu, Xiuting Rong, Huan Zhao, Ruizhi Xia, Min Li, Haotian Wang, Hongbiao Cui, Xiaozhi Wang, Jun Zhou","doi":"10.1021/acs.est.4c07961","DOIUrl":"https://doi.org/10.1021/acs.est.4c07961","url":null,"abstract":"Atmospheric deposition plays a significant role in introducing cadmium (Cd) into agroecological systems; however, accurately determining its accumulation in crops through foliar and root uptake presents challenges. This study investigated the bioaccumulation of atmospherically deposited Cd in soybean using a three-year fully factorial atmospheric exposure experiment incorporating Cd isotope analysis. Results shown that atmospheric deposition accounted for 1–13% of soil Cd pools, yet contributed 11–72% of Cd to soybean tissues during the growing seasons. Over the course of soil exposure to atmospheric deposition ranging from 1 to 3 years, no notable variations were observed in Cd concentrations in soil solutions and soybean tissues, nor in isotope ratios. Newly deposited Cd was a major source in soybean plants, and the bioavailability of deposited Cd rapidly aged in soils. Atmospheric Cd enriched in lighter isotopes induced negative isotope shifts in soybean plants. By employing an optimized isotope mixing model in conjunction with a mass balance approach, foliar Cd uptake contributed 13–51%, 16–45%, and 21–56% to stem, leaf, and seed, respectively. This study highlights substantial contribution of foliar uptake of atmospheric deposition to Cd levels in soybean and controlling foliar uptake as a potential strategy in agroecological systems experiencing high atmospheric Cd deposition.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142317212","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Chemical Exposomics in Human Plasma by Lipid Removal and Large-Volume Injection Gas Chromatography–High-Resolution Mass Spectrometry 通过脂质去除和大容量进样气相色谱-高分辨质谱法研究人体血浆中的化学物质暴露情况

IF 9.028 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c05942

Hongyu Xie, Kalliroi Sdougkou, Bénilde Bonnefille, Stefano Papazian, Ingvar A. Bergdahl, Panu Rantakokko, Jonathan W. Martin

{"title":"Chemical Exposomics in Human Plasma by Lipid Removal and Large-Volume Injection Gas Chromatography–High-Resolution Mass Spectrometry","authors":"Hongyu Xie, Kalliroi Sdougkou, Bénilde Bonnefille, Stefano Papazian, Ingvar A. Bergdahl, Panu Rantakokko, Jonathan W. Martin","doi":"10.1021/acs.est.4c05942","DOIUrl":"https://doi.org/10.1021/acs.est.4c05942","url":null,"abstract":"For comprehensive chemical exposomics in blood, analytical workflows are evolving through advances in sample preparation and instrumental methods. We hypothesized that gas chromatography–high-resolution mass spectrometry (GC-HRMS) workflows could be enhanced by minimizing lipid coextractives, thereby enabling larger injection volumes and lower matrix interference for improved target sensitivity and nontarget molecular discovery. A simple protocol was developed for small plasma volumes (100–200 μL) by using isohexane (H) to extract supernatants of acetonitrile-plasma (A-P). The HA-P method was quantitative for a wide range of hydrophobic multiclass target analytes (i.e., log Kow > 3.0), and the extracts were free of major lipids, thereby enabling robust large-volume injections (LVIs; 25 μL) in long sequences (60–70 h, 70–80 injections) to a GC-Orbitrap HRMS. Without lipid removal, LVI was counterproductive because method sensitivity suffered from the abundant matrix signal, resulting in low ion injection times to the Orbitrap. The median method quantification limit was 0.09 ng/mL (range 0.005–4.83 ng/mL), and good accuracy was shown for a certified reference serum. Applying the method to plasma from a Swedish cohort (n = 32; 100 μL), 51 of 103 target analytes were detected. Simultaneous nontarget analysis resulted in 112 structural annotations (12.8% annotation rate), and Level 1 identification was achieved for 7 of 8 substances in follow-up confirmations. The HA-P method is potentially scalable for application in cohort studies and is also compatible with many liquid-chromatography-based exposomics workflows.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":9.028,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142314021","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

Arsenic Reduces Methane Emissions from Paddy Soils: Insights from Continental Investigation and Laboratory Incubations. 砷可减少稻田土壤的甲烷排放：大陆调查和实验室培育的启示。

IF 10.8 1区环境科学与生态学

环境科学与技术 Pub Date : 2024-09-24 DOI: 10.1021/acs.est.4c06809

Ou-Yuan Jiang, Si-Yu Zhang, Xin-Di Zhao, Zi-Teng Liu, Andreas Kappler, Jian-Ming Xu, Xian-Jin Tang

{"title":"Arsenic Reduces Methane Emissions from Paddy Soils: Insights from Continental Investigation and Laboratory Incubations.","authors":"Ou-Yuan Jiang, Si-Yu Zhang, Xin-Di Zhao, Zi-Teng Liu, Andreas Kappler, Jian-Ming Xu, Xian-Jin Tang","doi":"10.1021/acs.est.4c06809","DOIUrl":"https://doi.org/10.1021/acs.est.4c06809","url":null,"abstract":"Arsenic (As) contamination and methane (CH4) emissions co-occur in rice paddies. However, how As impacts CH4 production, oxidation, and emission dynamics is unknown. Here, we investigated the abundances and activities of CH4-cycling microbes from 132 paddy soils with different As concentrations across continental China using metagenomics and the reverse transcription polymerase chain reaction. Our results revealed that As was a crucial factor affecting the abundance and distribution patterns of the mcrA gene, which is responsible for CH4 production and anaerobic CH4 oxidation. Laboratory incubation experiments showed that adding 30 mg kg-1 arsenate increased 13CO2 production by 10-fold, ultimately decreasing CH4 emissions by 68.5%. The inhibition of CH4 emissions by As was induced through three aspects: (1) the toxicity of As decreased the abundance and activity of the methanogens; (2) the adaptability and response of methanotrophs to As is beneficial for CH4 oxidation under As stress; and (3) the more robust arsenate reduction would anaerobically consume more CH4 in paddies. Additionally, significant positive correlations were observed between arsC and pmoA gene abundance in both the observational study and incubation experiment. These findings enhance our understanding of the mechanisms underlying the interactions between As and CH4 cycling in soils.","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":null,"pages":null},"PeriodicalIF":10.8,"publicationDate":"2024-09-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142306559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}

引用次数: 0

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