Pub Date : 2023-01-06DOI: 10.3389/fenvc.2022.1060651
F. Thibon, L. Weppe, C. Churlaud, T. Lacoue-Labarthe, S. Gasparini, Y. Cherel, P. Bustamante, N. Vigier
Non-conventional stable isotopes have received increasing attention in the past decade to investigate multi-level ecological connections from individuals to ecosystems. More recently, isotopes from trace and non-nutrient elements, potentially toxic (i.e., Hg), have also been recognized of great significance to discriminate sources, transports, and bioaccumulation, as well as trophic transfers. In contrast, lithium (Li) concentrations and its isotope compositions (δ7Li) remain poorly documented in aquatic ecosystems, despite its possible accumulation in marine organisms, its increasing industrial production, and its demonstrated hazardous effects on biota. Here, we present the first Li isotope investigation of various soft tissues, organs or whole organisms, from marine plankton, bivalves, cephalopods, crustaceans, and fish of different biogeographical regions [North Mediterranean Sea, North Atlantic Ocean (Bay of Biscay), South East Pacific Ocean (New Caledonia), and Southern Indian Ocean (Kerguelen Islands)]. Independently of the considered organisms, δ7Li values range widely, from 4.6‰ (digestive gland of bivalves) to 32.0‰ (zooplankton). Compared to homogeneous seawater (δ7Li ∼ 31.2‰ ± .3‰), marine organisms mostly fractionate Li isotopes in favor of the light isotope (6Li). Within the same taxonomic group, significant differences are observed among organs, indicating a key role of physiology on Li concentrations and on the distribution of Li isotopes. Statistically, the trophic position is only slightly related to the average Li isotope composition of soft tissues of marine organisms, but this aspect deserves further investigation at the organ level. Other potential influences are the Li uptake by ingestion or gill ventilation. Overall, this work constitutes the first δ7Li extensive baseline in soft tissues of coastal organisms from different large geographic areas mostly preserved from significant anthropogenic Li contamination.
{"title":"Lithium isotopes in marine food webs: Effect of ecological and environmental parameters","authors":"F. Thibon, L. Weppe, C. Churlaud, T. Lacoue-Labarthe, S. Gasparini, Y. Cherel, P. Bustamante, N. Vigier","doi":"10.3389/fenvc.2022.1060651","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1060651","url":null,"abstract":"Non-conventional stable isotopes have received increasing attention in the past decade to investigate multi-level ecological connections from individuals to ecosystems. More recently, isotopes from trace and non-nutrient elements, potentially toxic (i.e., Hg), have also been recognized of great significance to discriminate sources, transports, and bioaccumulation, as well as trophic transfers. In contrast, lithium (Li) concentrations and its isotope compositions (δ7Li) remain poorly documented in aquatic ecosystems, despite its possible accumulation in marine organisms, its increasing industrial production, and its demonstrated hazardous effects on biota. Here, we present the first Li isotope investigation of various soft tissues, organs or whole organisms, from marine plankton, bivalves, cephalopods, crustaceans, and fish of different biogeographical regions [North Mediterranean Sea, North Atlantic Ocean (Bay of Biscay), South East Pacific Ocean (New Caledonia), and Southern Indian Ocean (Kerguelen Islands)]. Independently of the considered organisms, δ7Li values range widely, from 4.6‰ (digestive gland of bivalves) to 32.0‰ (zooplankton). Compared to homogeneous seawater (δ7Li ∼ 31.2‰ ± .3‰), marine organisms mostly fractionate Li isotopes in favor of the light isotope (6Li). Within the same taxonomic group, significant differences are observed among organs, indicating a key role of physiology on Li concentrations and on the distribution of Li isotopes. Statistically, the trophic position is only slightly related to the average Li isotope composition of soft tissues of marine organisms, but this aspect deserves further investigation at the organ level. Other potential influences are the Li uptake by ingestion or gill ventilation. Overall, this work constitutes the first δ7Li extensive baseline in soft tissues of coastal organisms from different large geographic areas mostly preserved from significant anthropogenic Li contamination.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2023-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48575083","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-01-01DOI: 10.3389/fenvc.2023.1096199
Chris S Eckley, Collin Eagles-Smith, Todd P Luxton, Joel Hoffman, Sarah Janssen
Ecosystems downstream of mercury (Hg) contaminated sites can be impacted by both localized releases as well as Hg deposited to the watershed from atmospheric transport. Identifying the source of Hg in water, sediment, and fish downstream of contaminated sites is important for determining the effectiveness of source-control remediation actions. This study uses measurements of Hg stable isotopes in soil, sediment, water, and fish to differentiate between Hg from an abandoned Hg mine from non-mine-related sources. The study site is located within the Willamette River watershed (Oregon, United States), which includes free-flowing river segments and a reservoir downstream of the mine. The concentrations of total-Hg (THg) in the reservoir fish were 4-fold higher than those further downstream (>90 km) from the mine site in free-flowing sections of the river. Mercury stable isotope fractionation analysis showed that the mine tailings (δ202Hg: -0.36‰ ± 0.03‰) had a distinctive isotopic composition compared to background soils (δ202Hg: -2.30‰ ± 0.25‰). Similar differences in isotopic composition were observed between stream water that flowed through the tailings (particulate bound δ202Hg: -0.58‰; dissolved: -0.91‰) versus a background stream (particle-bound δ202Hg: -2.36‰; dissolved: -2.09‰). Within the reservoir sediment, the Hg isotopic composition indicated that the proportion of the Hg related to mine-release increased with THg concentrations. However, in the fish samples the opposite trend was observed-the degree of mine-related Hg was lower in fish with the higher THg concentrations. While sediment concentrations clearly show the influence of the mine, the relationship in fish is more complicated due to differences in methylmercury (MeHg) formation and the foraging behavior of different fish species. The fish tissue δ13C and Δ199Hg values indicate that there is a higher influence of mine-sourced Hg in fish feeding in a more sediment-based food web and less so in planktonic and littoral-based food webs. Identifying the relative proportion of Hg from local contaminated site can help inform remediation decisions, especially when the relationship between total Hg concentrations and sources do not show similar covariation between abiotic and biotic media.
{"title":"Using mercury stable isotope fractionation to identify the contribution of historical mercury mining sources present in downstream water, sediment and fish.","authors":"Chris S Eckley, Collin Eagles-Smith, Todd P Luxton, Joel Hoffman, Sarah Janssen","doi":"10.3389/fenvc.2023.1096199","DOIUrl":"https://doi.org/10.3389/fenvc.2023.1096199","url":null,"abstract":"<p><p>Ecosystems downstream of mercury (Hg) contaminated sites can be impacted by both localized releases as well as Hg deposited to the watershed from atmospheric transport. Identifying the source of Hg in water, sediment, and fish downstream of contaminated sites is important for determining the effectiveness of source-control remediation actions. This study uses measurements of Hg stable isotopes in soil, sediment, water, and fish to differentiate between Hg from an abandoned Hg mine from non-mine-related sources. The study site is located within the Willamette River watershed (Oregon, United States), which includes free-flowing river segments and a reservoir downstream of the mine. The concentrations of total-Hg (THg) in the reservoir fish were 4-fold higher than those further downstream (>90 km) from the mine site in free-flowing sections of the river. Mercury stable isotope fractionation analysis showed that the mine tailings (δ<sup>202</sup>Hg: -0.36‰ ± 0.03‰) had a distinctive isotopic composition compared to background soils (δ<sup>202</sup>Hg: -2.30‰ ± 0.25‰). Similar differences in isotopic composition were observed between stream water that flowed through the tailings (particulate bound δ<sup>202</sup>Hg: -0.58‰; dissolved: -0.91‰) versus a background stream (particle-bound δ<sup>202</sup>Hg: -2.36‰; dissolved: -2.09‰). Within the reservoir sediment, the Hg isotopic composition indicated that the proportion of the Hg related to mine-release increased with THg concentrations. However, in the fish samples the opposite trend was observed-the degree of mine-related Hg was lower in fish with the higher THg concentrations. While sediment concentrations clearly show the influence of the mine, the relationship in fish is more complicated due to differences in methylmercury (MeHg) formation and the foraging behavior of different fish species. The fish tissue δ<sup>13</sup>C and Δ<sup>199</sup>Hg values indicate that there is a higher influence of mine-sourced Hg in fish feeding in a more sediment-based food web and less so in planktonic and littoral-based food webs. Identifying the relative proportion of Hg from local contaminated site can help inform remediation decisions, especially when the relationship between total Hg concentrations and sources do not show similar covariation between abiotic and biotic media.</p>","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":"4 ","pages":"1096199"},"PeriodicalIF":0.0,"publicationDate":"2023-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10269370/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10042332","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-12-20DOI: 10.3389/fenvc.2022.1058890
L. Schwab, Florian M. Rothe, D. McLagan, Alexandra Alten, S. Kraemer, H. Biester, J. Wiederhold
Mercury (Hg) release from contaminated legacy sites is a large contributor to riverine ecosystems and can represent a significant local and regional environmental issue even long after the initial site contamination. Understanding processes of in-stream species transformation is therefore important to assess the fate and bioavailability of the released Hg. In this study, we investigated in-stream Hg transformation processes with analyses of Hg binding forms and Hg stable isotopes. Stream sediments were collected downstream of a former kyanization facility (Black Forest, SW Germany), where highly soluble Hg(II)-chloride (HgCl2) was used as an anti-fouling agent to treat timber. Exfiltration of partly anoxic, contaminated groundwater with Hg concentrations of up to 700 μg L−1 into the adjacent Gutach stream is the main source of Hg to sediments. Total Hg concentrations in the stream bottom sediments (<2 mm) ranged from background values of 6.3 µg kg−1 upstream of the contaminated site to 77 mg kg−1 near the location of exfiltration of contaminated groundwater. A five-step sequential extraction procedure and Hg pyrolytic thermal desorption (PTD) analyses indicated changes in Hg binding forms in the sediments along the flow path towards a higher proportion of organically bound Hg. A large shift towards negative δ202Hg values was observed downstream of the contaminated site (change of ≈2‰) along with a minor offset in mass-independent fractionation. Binary mixing models based on Hg isotope ratios using one industrial and different natural background endmembers were tested to estimate their respective contribution of Hg to the sediments but failed to produce plausible allocations. Based on the observed changes in isotopic composition, total Hg concentrations and Hg binding forms, we propose that the large extent of fractionation observed in downstream sediments is the result of a combination of kinetic isotope effects during sorption, redistribution of Hg within the sediment and the preferential transport of Hg associated with the sediment fine fraction. These results highlight the importance of transformation processes when assessing the sources and fate of Hg in environmental systems and show limitations of using simple mixing models based on Hg stable isotopes.
汞(Hg)从受污染的遗址释放是河流生态系统的一个重要贡献者,即使在最初的地点污染很久之后,也可能代表一个重要的地方和区域环境问题。因此,了解河流物种转化过程对于评估汞释放的命运和生物利用度至关重要。在本研究中,我们通过分析汞的结合形式和汞的稳定同位素来研究河流中汞的转化过程。在德国西南部的黑森林(Black Forest),一个原氰化工厂的下游收集了河流沉积物,在那里,高可溶性汞(II)-氯化物(HgCl2)被用作防污剂来处理木材。部分缺氧、汞浓度高达700 μg L−1的污染地下水渗漏到邻近的Gutach河是汞进入沉积物的主要来源。河底沉积物(< 2mm)的总汞浓度范围从污染地点上游的6.3µg kg - 1的背景值到污染地下水渗漏位置附近的77 mg kg - 1。五步序萃取和汞热解热解吸(PTD)分析表明,沿流动路径的沉积物中汞的结合形式发生了变化,有机结合汞的比例更高。污染地点下游的δ202Hg值向负方向转变较大(≈2‰),与质量无关的分馏有轻微偏移。基于汞同位素比值的二元混合模型使用一个工业和不同的自然背景端元进行了测试,以估计它们各自对沉积物的汞贡献,但未能产生合理的分配。根据观测到的同位素组成、总汞浓度和汞结合形式的变化,我们认为下游沉积物中汞的大量分馏是吸附过程中的动力学同位素效应、汞在沉积物中的再分配以及与沉积物细组分相关的汞优先输运的综合结果。这些结果强调了在评估环境系统中汞的来源和去向时转化过程的重要性,并显示了使用基于汞稳定同位素的简单混合模型的局限性。
{"title":"Large extent of mercury stable isotope fractionation in contaminated stream sediments induced by changes of mercury binding forms","authors":"L. Schwab, Florian M. Rothe, D. McLagan, Alexandra Alten, S. Kraemer, H. Biester, J. Wiederhold","doi":"10.3389/fenvc.2022.1058890","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1058890","url":null,"abstract":"Mercury (Hg) release from contaminated legacy sites is a large contributor to riverine ecosystems and can represent a significant local and regional environmental issue even long after the initial site contamination. Understanding processes of in-stream species transformation is therefore important to assess the fate and bioavailability of the released Hg. In this study, we investigated in-stream Hg transformation processes with analyses of Hg binding forms and Hg stable isotopes. Stream sediments were collected downstream of a former kyanization facility (Black Forest, SW Germany), where highly soluble Hg(II)-chloride (HgCl2) was used as an anti-fouling agent to treat timber. Exfiltration of partly anoxic, contaminated groundwater with Hg concentrations of up to 700 μg L−1 into the adjacent Gutach stream is the main source of Hg to sediments. Total Hg concentrations in the stream bottom sediments (<2 mm) ranged from background values of 6.3 µg kg−1 upstream of the contaminated site to 77 mg kg−1 near the location of exfiltration of contaminated groundwater. A five-step sequential extraction procedure and Hg pyrolytic thermal desorption (PTD) analyses indicated changes in Hg binding forms in the sediments along the flow path towards a higher proportion of organically bound Hg. A large shift towards negative δ202Hg values was observed downstream of the contaminated site (change of ≈2‰) along with a minor offset in mass-independent fractionation. Binary mixing models based on Hg isotope ratios using one industrial and different natural background endmembers were tested to estimate their respective contribution of Hg to the sediments but failed to produce plausible allocations. Based on the observed changes in isotopic composition, total Hg concentrations and Hg binding forms, we propose that the large extent of fractionation observed in downstream sediments is the result of a combination of kinetic isotope effects during sorption, redistribution of Hg within the sediment and the preferential transport of Hg associated with the sediment fine fraction. These results highlight the importance of transformation processes when assessing the sources and fate of Hg in environmental systems and show limitations of using simple mixing models based on Hg stable isotopes.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"42823137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-11-14DOI: 10.3389/fenvc.2022.1029708
Marc-Simon Bahr, M. Wolff
Photoacoustic spectroscopy (PAS) is typically used for the detection of trace gases. In this way, mixtures of short-chain hydrocarbons such as methane, ethane or propane can be analyzed with detection limits in the range of parts per million (ppm) or parts per billion (ppb) or even below. However, there are a number of applications where highly concentrated mixtures need to be analyzed. In some cases even the isotopologic composition of certain hydrocarbons needs to be determined. Examples can be found in natural gas production and planetary research. We present PAS-based isotopologic analyses of two digit percentage-level methane concentrations in nitrogen. The investigation allows conclusions to be drawn about the extent to which PAS is suitable for an isotopologic analysis of undiluted natural gas-like mixtures.
{"title":"PAS-based isotopologic analysis of highly concentrated methane","authors":"Marc-Simon Bahr, M. Wolff","doi":"10.3389/fenvc.2022.1029708","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1029708","url":null,"abstract":"Photoacoustic spectroscopy (PAS) is typically used for the detection of trace gases. In this way, mixtures of short-chain hydrocarbons such as methane, ethane or propane can be analyzed with detection limits in the range of parts per million (ppm) or parts per billion (ppb) or even below. However, there are a number of applications where highly concentrated mixtures need to be analyzed. In some cases even the isotopologic composition of certain hydrocarbons needs to be determined. Examples can be found in natural gas production and planetary research. We present PAS-based isotopologic analyses of two digit percentage-level methane concentrations in nitrogen. The investigation allows conclusions to be drawn about the extent to which PAS is suitable for an isotopologic analysis of undiluted natural gas-like mixtures.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47720717","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-11-10DOI: 10.3389/fenvc.2022.961369
J. Olomukoro, Nwamaka Ogochukwu Obi-Obueze, Rukeme Eko-Imirianye, O. Anani, V. Obot
The preliminary consequence of pollutants in water is to reduce the quality of water although this may not be immediately noticeable because of the self-purifying ability of some water bodies. The study on the physicochemical characteristics, bacteriological, and macrobenthic invertebrates was carried out in the Orogodo River. All the examined physicochemical characteristics of the water showed no significant difference (p > 0.05) across the stations. For the heavy metals, it was in decreasing order as follows: station 2 > station 3 > station 1. All the heavy metals except nickel had high values upstream (station 1). Bacteriological examination of the water revealed the presence of mesophilic bacteria across the stations at p < 0.01 (a highly significant difference). E. coli varied significantly (p < 0.01) across the stations. However, a further evaluation using the DMR test revealed that the population recorded at station 3 was significantly higher than that recorded at stations 1 and 2. A total of 787 macrobenthic invertebrates comprising 44 macroinvertebrates’ taxa were recorded. Most of the macrobenthic faunas observed were distributed across the three stations except the chironomids, the rat-tailed maggot (Eristalis tenax), and the family Hirudinea whose occurrence was almost restricted to station 2. This revealed an ecological impact because this species is a basic indicator of an ecosystem sentinel. Sorenson’s quotient of faunal similarity showed that macrobenthic fauna at these three stations was similar. The similarity was the highest between stations 1 and 3 (75.0%) and the lowest between stations 1 and 2 (50.0%). The biological monitoring working party (BMWP) score system showed that station 2 was moderately polluted, while stations 1 and 3 were only slightly affected. At stations 1, 2, and 3, the arithmetic WQI (water quality) values were 900.99, 1010.10, and 951.20, respectively. The high values of WQI obtained across the stations were attributable to the concentrations of Fe, Cu, Cr, Cd, Ni, Pb, V, and THC, thus reiterating the conclusion drawn from the physicochemical parameter analysis. Boiling the water before consumption is highly recommended to avoid possible human health problems, especially effects from microbial pathogens like coliforms and E. coli.
{"title":"Water quality evaluation using physicochemical and biological indices to characterize the integrity of the Orogodo River in sub-Saharan Africa","authors":"J. Olomukoro, Nwamaka Ogochukwu Obi-Obueze, Rukeme Eko-Imirianye, O. Anani, V. Obot","doi":"10.3389/fenvc.2022.961369","DOIUrl":"https://doi.org/10.3389/fenvc.2022.961369","url":null,"abstract":"The preliminary consequence of pollutants in water is to reduce the quality of water although this may not be immediately noticeable because of the self-purifying ability of some water bodies. The study on the physicochemical characteristics, bacteriological, and macrobenthic invertebrates was carried out in the Orogodo River. All the examined physicochemical characteristics of the water showed no significant difference (p > 0.05) across the stations. For the heavy metals, it was in decreasing order as follows: station 2 > station 3 > station 1. All the heavy metals except nickel had high values upstream (station 1). Bacteriological examination of the water revealed the presence of mesophilic bacteria across the stations at p < 0.01 (a highly significant difference). E. coli varied significantly (p < 0.01) across the stations. However, a further evaluation using the DMR test revealed that the population recorded at station 3 was significantly higher than that recorded at stations 1 and 2. A total of 787 macrobenthic invertebrates comprising 44 macroinvertebrates’ taxa were recorded. Most of the macrobenthic faunas observed were distributed across the three stations except the chironomids, the rat-tailed maggot (Eristalis tenax), and the family Hirudinea whose occurrence was almost restricted to station 2. This revealed an ecological impact because this species is a basic indicator of an ecosystem sentinel. Sorenson’s quotient of faunal similarity showed that macrobenthic fauna at these three stations was similar. The similarity was the highest between stations 1 and 3 (75.0%) and the lowest between stations 1 and 2 (50.0%). The biological monitoring working party (BMWP) score system showed that station 2 was moderately polluted, while stations 1 and 3 were only slightly affected. At stations 1, 2, and 3, the arithmetic WQI (water quality) values were 900.99, 1010.10, and 951.20, respectively. The high values of WQI obtained across the stations were attributable to the concentrations of Fe, Cu, Cr, Cd, Ni, Pb, V, and THC, thus reiterating the conclusion drawn from the physicochemical parameter analysis. Boiling the water before consumption is highly recommended to avoid possible human health problems, especially effects from microbial pathogens like coliforms and E. coli.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-11-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47323374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-10-19DOI: 10.3389/fenvc.2022.1002301
Jinxiang Wang, Jianmin Ma, Panliang Liu
Ambient non-methane hydrocarbons (NMHCs) were investigated at Shenhua coal chemical industrial park (SH), and Baofeng coal chemical industrial park (BF) in Ningdong Energy and Chemical Industrial Base (NECIB) in China’s Energy Golden Triangle (EGT). Ambient air samples were collected using pre-evacuated 2-L electro-polished stainless steel canisters at SH and BF from 9:00 a.m. to 9:30 a.m. (UTC+8) from 22 to 31 December 2016. Fifty-seven NMHCs were analyzed using gas chromatography-mass selective detector/flame ionization detector. The average NMHCs mixing ratios were 49.05 ± 44.37 ppbv in SH, and 39.31 ± 18.77 ppbv in BF. Overall, alkanes took up the largest proportion (>60%), followed by alkenes, acetylene, and aromatics. The propylene-equivalent (Prop-Equiv) concentration and the ozone formation potential (OFP) of NMHCs were calculated to estimate their chemical reactivities. Alkenes played a predominant role in NMHCs reactivity, among which propylene and ethylene were the largest contributors. OFP values show that alkenes and acetylene were the largest contributors (60%) to measured total NMHCs. Ethylene, propylene, m/p-xylene, n-butane, 1-butene, propane and acetylene were the major precursors in ground-level ozone formation in this region, which accounted for 66% and 62% of the total ozone formed by NMHCs at BF and SH, respectively. This study identified that industrial activities were the primary sources of NMHCs, confirmed by the high ratios of benzene to toluene (B/T = 2.23). Therefore, these organic pollutants should be monitored further based on their high toxicities.
{"title":"Ambient non-methane hydrocarbons and their contribution to ozone formation potential in a super coal chemical industry in China’s Energy Golden Triangle","authors":"Jinxiang Wang, Jianmin Ma, Panliang Liu","doi":"10.3389/fenvc.2022.1002301","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1002301","url":null,"abstract":"Ambient non-methane hydrocarbons (NMHCs) were investigated at Shenhua coal chemical industrial park (SH), and Baofeng coal chemical industrial park (BF) in Ningdong Energy and Chemical Industrial Base (NECIB) in China’s Energy Golden Triangle (EGT). Ambient air samples were collected using pre-evacuated 2-L electro-polished stainless steel canisters at SH and BF from 9:00 a.m. to 9:30 a.m. (UTC+8) from 22 to 31 December 2016. Fifty-seven NMHCs were analyzed using gas chromatography-mass selective detector/flame ionization detector. The average NMHCs mixing ratios were 49.05 ± 44.37 ppbv in SH, and 39.31 ± 18.77 ppbv in BF. Overall, alkanes took up the largest proportion (>60%), followed by alkenes, acetylene, and aromatics. The propylene-equivalent (Prop-Equiv) concentration and the ozone formation potential (OFP) of NMHCs were calculated to estimate their chemical reactivities. Alkenes played a predominant role in NMHCs reactivity, among which propylene and ethylene were the largest contributors. OFP values show that alkenes and acetylene were the largest contributors (60%) to measured total NMHCs. Ethylene, propylene, m/p-xylene, n-butane, 1-butene, propane and acetylene were the major precursors in ground-level ozone formation in this region, which accounted for 66% and 62% of the total ozone formed by NMHCs at BF and SH, respectively. This study identified that industrial activities were the primary sources of NMHCs, confirmed by the high ratios of benzene to toluene (B/T = 2.23). Therefore, these organic pollutants should be monitored further based on their high toxicities.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-10-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"44419061","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-10-10DOI: 10.3389/fenvc.2022.1046468
D. Amouroux, N. Vigier
The isotopic composition of trace metals and elements can be used to characterize their sources of emission and to trace the physicochemical or biological processes that these elements undergo. Precise measurements of trace metals and their isotopic compositions are pre-required for such research issues. Regarding the processes leading to fractionation between isotopes and thereby to a modification of the isotopic composition, the main mechanisms of isotopic fractionations result from physicochemical reactions such as redox transformations, the dissolution or precipitation of minerals and/or neoformed phases (eg. oxy-hydroxides). Added to this are the effects associated with living organisms that, for their development, can integrate metals into their metabolism and be also the cause of strong isotopic fractionations. The development of multi-collector inductively coupled plasma instruments (MC-ICP-MS) has made it possible to accurately and repeatably measure the isotopic composition of trace metals and elements whose (small) variations in isotopic abundance obey the laws of mass dependent fractionation. In addition, few nontraditional elements, such as Hg, have been identified to exhibit specific isotopic fractionation that do not follow such basic rules (i.e. mass independent isotopic fractionation). This Research Topic aimed to promote specific studies on stable and meta-stable isotopes of metals and trace elements that have been recently developed and integrated into environmental sciences and pollution research. Isotopic composition of trace metals OPEN ACCESS
{"title":"Editorial: Advances in metals and trace elements isotopes measurements, experiments and application in environmental sciences","authors":"D. Amouroux, N. Vigier","doi":"10.3389/fenvc.2022.1046468","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1046468","url":null,"abstract":"The isotopic composition of trace metals and elements can be used to characterize their sources of emission and to trace the physicochemical or biological processes that these elements undergo. Precise measurements of trace metals and their isotopic compositions are pre-required for such research issues. Regarding the processes leading to fractionation between isotopes and thereby to a modification of the isotopic composition, the main mechanisms of isotopic fractionations result from physicochemical reactions such as redox transformations, the dissolution or precipitation of minerals and/or neoformed phases (eg. oxy-hydroxides). Added to this are the effects associated with living organisms that, for their development, can integrate metals into their metabolism and be also the cause of strong isotopic fractionations. The development of multi-collector inductively coupled plasma instruments (MC-ICP-MS) has made it possible to accurately and repeatably measure the isotopic composition of trace metals and elements whose (small) variations in isotopic abundance obey the laws of mass dependent fractionation. In addition, few nontraditional elements, such as Hg, have been identified to exhibit specific isotopic fractionation that do not follow such basic rules (i.e. mass independent isotopic fractionation). This Research Topic aimed to promote specific studies on stable and meta-stable isotopes of metals and trace elements that have been recently developed and integrated into environmental sciences and pollution research. Isotopic composition of trace metals OPEN ACCESS","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"48055637","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-10-10DOI: 10.3389/fenvc.2022.1018576
R. Rather, S. Ara, Sanjeev Sharma, S. A. Padder, F. Lone, S. Mir, Z. Baba, I. Ayoub, I. A. Mir, Tariq A Bhat, T. R. Baba
Trace elements are a major pollutant in the river water and these pollutants are present in all components of the ecological system. Since time immemorial, the River Veshaw has been one of the important sources of water and has shaped the cultural and social values in the Kashmir Valley. This study was conducted in rural parts of South Kashmir in the Western Himalaya from February to January 2020–2022. The river Veshaw provides various ecosystem services to the local communities as well as in the upper and lower stream regions in the form of many direct and indirect ecosystem services. The river is polluted by human waste from both rural and urban communities, as well as by agricultural runoff and effluent discharges from a variety of industrial activities due to its proximity. Effluent that makes it to the river contains a variety of pollutants, some of which are trace elements that accumulate in the local ecosystem, killing off plants and animals and reducing biodiversity. Trace element levels in water and sediment were found to follow the trend as: Sangam > Khudwani > Kulgam > Nihama > Aharbal > Kingwattan. The dominance pattern of heavy metals in water was Pb > As > Cd. The overall trend showed a downward trend of heavy metals, indicating the effect of land area drainage and anthropogenic activities on the stream water. The dominance pattern of heavy metals in water was Pb > As > Cd. Heavy metals were not detected in the middle and upstream sites. The average levels of heavy metals were highest at Downstream (Sangam), with values of Cd, Pd ad As 0.0054, 0.038 and 0.038 mgL-1. This shows that land drainage and human activities have an effect on the water in the stream.
{"title":"Seasonal changes and determination of heavy metal concentrations in Veshaw river of the Indian western Himalaya","authors":"R. Rather, S. Ara, Sanjeev Sharma, S. A. Padder, F. Lone, S. Mir, Z. Baba, I. Ayoub, I. A. Mir, Tariq A Bhat, T. R. Baba","doi":"10.3389/fenvc.2022.1018576","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1018576","url":null,"abstract":"Trace elements are a major pollutant in the river water and these pollutants are present in all components of the ecological system. Since time immemorial, the River Veshaw has been one of the important sources of water and has shaped the cultural and social values in the Kashmir Valley. This study was conducted in rural parts of South Kashmir in the Western Himalaya from February to January 2020–2022. The river Veshaw provides various ecosystem services to the local communities as well as in the upper and lower stream regions in the form of many direct and indirect ecosystem services. The river is polluted by human waste from both rural and urban communities, as well as by agricultural runoff and effluent discharges from a variety of industrial activities due to its proximity. Effluent that makes it to the river contains a variety of pollutants, some of which are trace elements that accumulate in the local ecosystem, killing off plants and animals and reducing biodiversity. Trace element levels in water and sediment were found to follow the trend as: Sangam > Khudwani > Kulgam > Nihama > Aharbal > Kingwattan. The dominance pattern of heavy metals in water was Pb > As > Cd. The overall trend showed a downward trend of heavy metals, indicating the effect of land area drainage and anthropogenic activities on the stream water. The dominance pattern of heavy metals in water was Pb > As > Cd. Heavy metals were not detected in the middle and upstream sites. The average levels of heavy metals were highest at Downstream (Sangam), with values of Cd, Pd ad As 0.0054, 0.038 and 0.038 mgL-1. This shows that land drainage and human activities have an effect on the water in the stream.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-10-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"47641403","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-09-28DOI: 10.3389/fenvc.2022.1018162
Luise Henneberger, Julia Huchthausen, M. König, Alina Menge, Niklas Wojtysiak, B. Escher
Cell-based bioassays are useful tools for the effect assessment of complex mixtures, but so far exposure assessment has not been performed for mixtures of chemicals. In the present study, cytotoxicity and activation of oxidative stress response were measured for three designed chemical mixtures with up to twelve components. The measurements of biological responses were complemented by concentration measurements using solid-phase microextraction to derive the freely dissolved concentrations of the mixtures (C free,mix). The tested mixtures showed slightly higher cytotoxic effects than predicted by the concentration addition model. Nominal and freely dissolved effect concentrations of the mixtures were very similar (within a factor of 1.5), but nominal concentrations (C nom) and C free of the individual mixture components were only similar for the hydrophilic chemicals (e.g., caffeine, coumarin, lamotrigine). For hydrophobic (e.g., fluoranthene) and acidic chemicals (e.g., diclofenac, naproxen) C free was up to 648 times lower than C nom. Chemicals were dosed in equipotent nominal concentration ratios and therefore contributed equally to the detected effects. Hydrophilic chemicals with low potency dominated C nom,mix (up to 95%) and C free,mix (up to 99%). Several mixture components (e.g., diclofenac, ibuprofen, naproxen and warfarin) showed increasing free fractions with increasing C nom,mix and therefore also a concentration-dependent contribution to C free,mix. Based on the findings of this study, we concluded that C nom,mix will be sufficient for evaluating the toxicity of mixtures that contain chemicals with diverse physicochemical properties at low concentration levels. In contrast, for risk assessment purposes and quantitative in vitro to in vivo extrapolations, C free,mix is a better parameter because the in vitro responses can be related to freely dissolved concentrations in human plasma.
{"title":"Experimental exposure assessment of designed chemical mixtures in cell-based in vitro bioassays","authors":"Luise Henneberger, Julia Huchthausen, M. König, Alina Menge, Niklas Wojtysiak, B. Escher","doi":"10.3389/fenvc.2022.1018162","DOIUrl":"https://doi.org/10.3389/fenvc.2022.1018162","url":null,"abstract":"Cell-based bioassays are useful tools for the effect assessment of complex mixtures, but so far exposure assessment has not been performed for mixtures of chemicals. In the present study, cytotoxicity and activation of oxidative stress response were measured for three designed chemical mixtures with up to twelve components. The measurements of biological responses were complemented by concentration measurements using solid-phase microextraction to derive the freely dissolved concentrations of the mixtures (C free,mix). The tested mixtures showed slightly higher cytotoxic effects than predicted by the concentration addition model. Nominal and freely dissolved effect concentrations of the mixtures were very similar (within a factor of 1.5), but nominal concentrations (C nom) and C free of the individual mixture components were only similar for the hydrophilic chemicals (e.g., caffeine, coumarin, lamotrigine). For hydrophobic (e.g., fluoranthene) and acidic chemicals (e.g., diclofenac, naproxen) C free was up to 648 times lower than C nom. Chemicals were dosed in equipotent nominal concentration ratios and therefore contributed equally to the detected effects. Hydrophilic chemicals with low potency dominated C nom,mix (up to 95%) and C free,mix (up to 99%). Several mixture components (e.g., diclofenac, ibuprofen, naproxen and warfarin) showed increasing free fractions with increasing C nom,mix and therefore also a concentration-dependent contribution to C free,mix. Based on the findings of this study, we concluded that C nom,mix will be sufficient for evaluating the toxicity of mixtures that contain chemicals with diverse physicochemical properties at low concentration levels. In contrast, for risk assessment purposes and quantitative in vitro to in vivo extrapolations, C free,mix is a better parameter because the in vitro responses can be related to freely dissolved concentrations in human plasma.","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"43433227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2022-09-02DOI: 10.3389/fenvc.2022.958607
Ignacio Martínez-Álvarez, K. Le Ménach, M. Devier, M. Cajaraville, A. Orbea, H. Budzinski
Microplastics (MPs) largely occur in aquatic ecosystems due to degradation of larger plastics or release from MP-containing products. Due to the hydrophobic nature and large specific surface of MPs, other contaminants, such as polycyclic aromatic hydrocarbons (PAHs), can potentially sorb onto MPs. Several studies have addressed the potential impact of MPs as vectors of PAHs for aquatic organisms. Therefore the role of MPs as sorbents of these compounds should be carefully investigated. The present study aimed to determine the sorption capacity of benzo(a)pyrene (B(a)P), as a model pyrolytic PAH, to polystyrene (PS) MPs of different sizes (4.5 and 0.5 μm). In addition, the sorption of PAHs present in the water accommodated fraction (WAF) of a naphthenic North Sea crude oil to 4.5 μm MPs was also studied as a model of a complex mixture of petrogenic PAHs that could appear in oil-polluted environments. The results indicated that 0.5 μm MPs showed higher maximum sorption capacity (Qmax) for B(a)P (145–242.89 μg/g) than 4.5 μm MPs (30.50–67.65 μg/g). From the WAF mixture, naphthalene was sorbed at a higher extent than the other PAHs to 4.5 μm MPs but with weak binding interactions (Kf = 69.25 L/g; 1/n = 0.46) according to the analysis of the aqueous phase, whereas phenanthrene showed stronger binding interactions (Kf = 0.24 L/g; 1/n = 0.98) based on the analysis of the solid phase. Sorption of PAHs of the complex WAF mixture to 4.5 μm MPs was relatively limited and driven by the hydrophobicity and initial concentration of each PAH. Overall, the results indicate that sorption estimations based solely on the analysis of the aqueous phase could overestimate the capacity of MPs to carry PAHs. Therefore, controlled laboratory assays assessing the “Trojan Horse effect” of MPs for aquatic organisms should consider these findings in order to design accurate and relevant experimental procedures. GRAPHICAL ABSTRACT
{"title":"Sorption of benzo(a)pyrene and of a complex mixture of petrogenic polycyclic aromatic hydrocarbons onto polystyrene microplastics","authors":"Ignacio Martínez-Álvarez, K. Le Ménach, M. Devier, M. Cajaraville, A. Orbea, H. Budzinski","doi":"10.3389/fenvc.2022.958607","DOIUrl":"https://doi.org/10.3389/fenvc.2022.958607","url":null,"abstract":"Microplastics (MPs) largely occur in aquatic ecosystems due to degradation of larger plastics or release from MP-containing products. Due to the hydrophobic nature and large specific surface of MPs, other contaminants, such as polycyclic aromatic hydrocarbons (PAHs), can potentially sorb onto MPs. Several studies have addressed the potential impact of MPs as vectors of PAHs for aquatic organisms. Therefore the role of MPs as sorbents of these compounds should be carefully investigated. The present study aimed to determine the sorption capacity of benzo(a)pyrene (B(a)P), as a model pyrolytic PAH, to polystyrene (PS) MPs of different sizes (4.5 and 0.5 μm). In addition, the sorption of PAHs present in the water accommodated fraction (WAF) of a naphthenic North Sea crude oil to 4.5 μm MPs was also studied as a model of a complex mixture of petrogenic PAHs that could appear in oil-polluted environments. The results indicated that 0.5 μm MPs showed higher maximum sorption capacity (Qmax) for B(a)P (145–242.89 μg/g) than 4.5 μm MPs (30.50–67.65 μg/g). From the WAF mixture, naphthalene was sorbed at a higher extent than the other PAHs to 4.5 μm MPs but with weak binding interactions (Kf = 69.25 L/g; 1/n = 0.46) according to the analysis of the aqueous phase, whereas phenanthrene showed stronger binding interactions (Kf = 0.24 L/g; 1/n = 0.98) based on the analysis of the solid phase. Sorption of PAHs of the complex WAF mixture to 4.5 μm MPs was relatively limited and driven by the hydrophobicity and initial concentration of each PAH. Overall, the results indicate that sorption estimations based solely on the analysis of the aqueous phase could overestimate the capacity of MPs to carry PAHs. Therefore, controlled laboratory assays assessing the “Trojan Horse effect” of MPs for aquatic organisms should consider these findings in order to design accurate and relevant experimental procedures. GRAPHICAL ABSTRACT","PeriodicalId":73082,"journal":{"name":"Frontiers in environmental chemistry","volume":" ","pages":""},"PeriodicalIF":0.0,"publicationDate":"2022-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41604307","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}