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Assessing the chemical anthropocene – Development of the legacy pollution fingerprint in the North Sea during the last century
2022
Logemann, A. | Reininghaus, M. | Schmidt, M. | Ebeling, A. | Zimmermann, T. | Wolschke, H. | Friedrich, J. | Brockmeyer, B. | Pröfrock, D. | Witt, G.
The North Sea and its coastal zones are heavily impacted by anthropogenic activities, which has resulted in significant chemical pollution ever since the beginning of the industrialization in Europe during the 19th century. In order to assess the chemical Anthropocene, natural archives, such as sediment cores, can serve as a valuable data source to reconstruct historical emission trends and to verify the effectiveness of changing environmental legislation. In this study, we investigated 90 contaminants covering inorganic and organic pollutant groups analyzed in a set of sediment cores taken in the North Seas' main sedimentation area (Skagerrak). We thereby develop a chemical pollution fingerprint that records the constant input of pollutants over time and illustrates their continued great relevance for the present. Additionally, samples were radiometrically dated and PAH and PCB levels in porewater were determined using equilibrium passive sampling. Furthermore, we elucidated the origin of lead (Pb) contamination utilizing non-traditional stable isotopic analysis. Our results reveal three main findings: 1. for all organic contaminant groups covered (PAHs, OCPs, PCBs, PBDEs and PFASs) as well as the elements lead (Pb) and titanium (Ti), determined concentrations decreased towards more recent deposited sediment. These decreasing trends could be linked to the time of introductions of restrictions and bans and therefor our results confirm, amongst possible other factors, the effectiveness of environmental legislation by revealing a successive change in contamination levels over the decades. 2. concentration trends for ΣPAH and ΣPCB measured in porewater correspond well with the ones found in sediment which suggests that this method can be a useful expansion to traditional bulk sediment analysis to determine the biologically available pollutant fraction. 3. Arsenic (As) concentrations were higher in younger sediment layers, potentially caused by emissions of corroded warfare material disposed in the study area after WW II.
显示更多 [+] 显示较少 [-]Biological toxicity risk assessment of two potential neutral carbon diesel fuel substitutes
2022
Arias, Silvana | Estrada, Verónica | Ortiz, Isabel C. | Molina, Francisco J. | Agudelo, John R.
We investigated the biological response of soluble organic fraction (SOF) and water-soluble fraction (WSF) extracted from particulate matter (PM) emitted by an automotive diesel engine operating in a representative urban driving condition. The engine was fueled with ultra-low sulfur diesel (ULSD), and its binary blends by volume with 13% of butanol (Bu13), and with hydrotreated vegetable oil (HVO) at 13% (HVO13) and 20% (HVO20). Cytotoxicity, genotoxicity, oxidative DNA damage and ecotoxicity tests were carried out, and 16 polycyclic aromatic hydrocarbons (PAH) expressed as tbenzo(a)pyrene total toxicity equivalent (BaP-TEQ) were also analyzed. The Hepatocarcinoma epithelial cell line (HepG2) was exposed to SOF for 24 h and analyzed using comet assay, with the inclusion of formamidopyrimidine DNA glycosylase (FPG) and endonuclease III (Endo III) to recognize oxidized DNA bases. The WSF was evaluated through acute ecotoxicity tests with the aquatic microcrustacean Daphnia pulex (D. Pulex). Results showed that there was no cytotoxic activity for all tested SOF concentrations. Genotoxic responses by all the SOF samples were at same level, except for the HVO13 which was weaker in the absence of the enzymes. The addition of the FPG and Endo III enzymes resulted in a significant increase in the comet tail, indicating that the DNA damage from SOF for all tested fuel blends involves oxidative damage including a higher level of oxidized purines for ULSD and Bu13 in comparison with HVO blends, but the oxidized pyrimidines for HVO blends were slightly higher compared to Bu13. The WSF did not show acute ecotoxicity for any of the fuels. Unlike other samples, Bu13-derived particles significantly increase the BaP-TEQ. The contribution to the genotoxic activity and oxidative DNA from SOF was not correlated to BaP-TEQ, which means that the biological activity of PM might be affected also by other toxic compounds present in particulate phase.
显示更多 [+] 显示较少 [-]Organic fertilizer activates soil beneficial microorganisms to promote strawberry growth and soil health after fumigation
2022
Li, Qingjie | Zhang, Daqi | Song, Zhaoxin | Ren, Lirui | Jin, Xi | Fang, Wensheng | Yan, Dongdong | Li, Yuan | Wang, Qiuxia | Cao, Aocheng
Soil fumigants aim to control soil-borne diseases below levels that affect economic crop production, but their use also reduces the abundance of beneficial microorganisms. Previous studies have shown that adding various types of fertilizers to soil after fumigation can reshape the soil microbial community and regulate crop growth. We fumigated soil with dazomet (DZ) that had been cropped continuously for more than 20 years. After fumigation we applied silicon fertilizer, potassium humate organic fertilizer, Bacillus microbial fertilizer or a mixture of the last two. We studied the effects of different fertilizers treatments on the soil's physicochemical properties, enzyme activities, key soil pathogens and beneficial microbes. We found that fertilizers applied after fumigation promoted soil beneficial microorganisms (such as Fimicutes, Chloroflexi, Bacillus and Actinomadura) restoration; increased Fusarium and Phytophthora pathogen mortality, the content of ammonium nitrogen, sucrase enzyme activity; and increased strawberry fruit yield. A significant increase in strawberry yield was positively correlated with increases in beneficial microorganisms such as Gemmatimonadota, Firmicutes, Bacillus and Flavisolibacter. We concluded that organic fertilizer applied after fumigation significantly increased the number of beneficial microorganisms, improved the physicochemical properties of the soil, increased soil enzyme activities, inhibited the growth of soil pathogens to increase strawberry fruit yield. In summary, organic fertilizer activated soil beneficial microorganisms after soil fumigation, promoted soil health, and increased strawberry fruit yield.
显示更多 [+] 显示较少 [-]Status and prospects of atmospheric microplastics: A review of methods, occurrence, composition, source and health risks
2022
Xu, An | Shi, Mingming | Xing, Xinli | Su, Yewang | Li, Xingyu | Liu, Weijie | Mao, Yao | Hu, Tianpeng | Qi, Shihua
The global pollution of microplastics (MPs) has attracted widespread attention, and the atmosphere was an indispensable media for the global transmission of MPs. With the growing awareness of MPs, atmospheric microplastics (AMPs) have been proposed as a new topic in recent years. Compared with the extensive studies on MPs in Marine and terrestrial environments, the studies of AMPs remain limited. In this study, sampling and analysis methods, occurrence, source analysis and health risk of AMPs were summarized and discussed. According to the different sampling methods, AMPs can be divided into suspension microplastics (SAMPs) and deposition microplastics (DAMPs). Previous studies have shown that SAMPs and DAMPs differ in composition and abundance, with SAMPs generally having a higher fraction of fragments. The mechanism of the migration of AMPs between different media was not clear yet. We further collated global data on the composition characteristics of MPs in soil and fresh water, which showed that the fragment MPs in soil and fresh water was higher than that in the atmosphere. Polymers in soil and fresh water were mainly PP and PE, while AMPs in the atmosphere were mainly PET. The shape composition of the MPs in both atmospheric and freshwater systems suggests that there may be the same dominant factor. The transport of AMPs and source apportionment were the important issues of current research, but both of them were at the initial stage. Therefore, AMPs needs to be further studied, especially for the source and fate, which would be conducive to understand the global distribution of AMPs. Furthermore, a standardized manual on sampling and processing of AMPs was also necessary to facilitate the comparative analysis of data between different studies and the construction of global models.
显示更多 [+] 显示较少 [-]Sediment records of global and regional Hg emissions to the atmosphere in North China over the last three centuries
2022
Wan, Dejun | Yang, Handong | Song, Lei | Jin, Zhangdong | Mao, Xin | Yang, Jinsong
Reconstructing the long-term Hg history in major emission countries is important for understanding the global Hg cycle and controlling Hg pollution. In this study, the atmospheric Hg history was reconstructed over the last three centuries based on three lacustrine sediment records from southeastern Inner Mongolia in North China, and its relationship with global and regional Hg emissions was revealed. These records show little Hg pollution in the 18th and 19th centuries. This implies a limited influence of Hg emitted from Europe and North America in this region, which is confirmed by their different Hg trends during the two World Wars and the post-1970s. Atmospheric Hg in the region had increased gradually since the 1900s, primarily contributed by emissions from the former Soviet Union in Lake Dalihu (DLH) and Lake Zhagesitai (ZGST) and from the Beijing-Tianjin-Hebei region in Lake Kulunnao (KLN). In the last century, two decreases in Hg fluxes occurred in the KLN core due to the economic recession in the 1960s–1970s and reduced energy consumption and industrial production in the 1990s. In the DLH and ZGST cores, only one decrease occurred, corresponded with the dissolution of the Soviet Union in the 1990s. Although atmospheric Hg emissions in China had stabilized or even decreased in the last decade, atmospheric Hg continued to increase, particularly in KLN, because of emissions from small cities in the region. This study can help understand Hg sources and control Hg pollution in North China and supplement the understanding of the global Hg cycling.
显示更多 [+] 显示较少 [-]Gestational phthalate exposure and lung function during childhood: A prospective population-based study
2022
Bosch de Basea, Magda | Carsin, Anne-Elie | Abellan, Alicia | Cobo, Inés | Lertxundi, Aitana | Marin, Natalia | Soler-Blasco, Raquel | Ibarluzea, Jesús | Vrijheid, Martine | Sunyer, Jordi | Casas, Maribel | Garcia-Aymerich, Judith
The potential effect of gestational exposure to phthalates on the lung function levels during childhood is unclear. Therefore, we examined this association at different ages (from 4 to 11 years) and over the whole childhood. Specifically, we measured 9 phthalate metabolites (MEP, MiBP, MnBP, MCMHP, MBzP, MEHHP, MEOHP, MECPP, MEHP) in the urine of 641 gestating women from the INMA study (Spain) and the forced vital capacity (FVC), forced expiratory volume in 1 s (FEV₁) and FEV₁/FVC in their offspring at ages 4, 7, 9 and 11. We used linear regression and mixed linear regression with a random intercept for subject to assess the association between phthalates and lung function at each study visit and for the overall childhood, respectively. We also assessed the phthalate metabolites mixture effect on lung function using a Weighted Quantile Sum (WQS) regression. We observed that the phthalate metabolites gestational levels were consistently associated with lower FVC and FEV₁ at all ages, both when assessed individually and jointly as a mixture, although most associations were not statistically significant. Of note, a 10% increase in MiBP was related to lower FVC (−0.02 (−0.04, 0)) and FEV₁ z-scores (−0.02 (−0.04, −0.01) at age 4. Similar significant reductions in FVC were observed at ages 4 and 7 associated with an increase in MEP and MnBP, respectively, and for FEV₁ at age 4 associated with an increase in MBzP. WQS regression consistently identified MBzP as an important contributor to the phthalate mixture effect. We can conclude that the gestational exposure to phthalates was associated with children's lower FVC and FEV₁, especially in early childhood, and in a statistically significant manner for MEP, MiBP, MBzP and MnBP. Given the ubiquity of phthalate exposure and its established endocrine disrupting effects in children, our findings support current regulations that limit phthalate exposure.
显示更多 [+] 显示较少 [-]Comprehensive chemical characterization of gaseous I/SVOC emissions from heavy-duty diesel vehicles using two-dimensional gas chromatography time-of-flight mass spectrometry
2022
He, Xiao | Zheng, Xuan | You, Yan | Zhang, Shaojun | Zhao, Bin | Wang, Xuan | Huang, Guanghan | Chen, Ting | Cao, Yihuan | He, Liqiang | Chang, Xing | Wang, Shuxiao | Wu, Ye
Intermediate-volatility and semi-volatile organic compounds (I/SVOCs) are key precursors of secondary organic aerosol (SOA). However, the comprehensive characterization of I/SVOCs has long been an analytical challenge. Here, we develop a novel method of speciating and quantifying I/SVOCs using two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC-ToF-MS) by constructing class-screening programs based on their characteristic fragments and mass spectrum patterns. Using this new approach, we then present a comprehensive analysis of gaseous I/SVOC emissions from heavy-duty diesel vehicles (HDDVs). Over three-thousand compounds are identified and classified into twenty-one categories. The dominant compound groups of I/SVCOs emitted by HDDVs are alkanes (including normal and branched alkanes, 37–66%), benzylic alcohols (7–20%), alkenes (3–11%), cycloalkanes (3–9%), and benzylic ketones (1–4%). Oxygenated I/SVOCs (O–I/SVOCs, e.g., benzylic alcohols and ketones) are first quantified and account for >20% of the total I/SVOC mass. Advanced aftertreatment devices largely reduce the total I/SVOC emissions but increase the proportion of O–I/SVOCs. With the speciation data, we successfully map the I/SVOCs into the two-dimensional volatility basis set space, which facilitates a better estimation of SOA. As aging time goes by, approximate 45% difference between the two scenarios after seven-day aging is observed, which confirms the significant impact of speciated I/SVOC emission data on SOA prediction.
显示更多 [+] 显示较少 [-]Generation of novel n-p-n (CeO2-PPy-ZnO) heterojunction for photocatalytic degradation of micro-organic pollutants
2022
Rajendran, Saravanan | Hoang, Tuan K.A. | Trudeau, Michel L. | Jalil, A.A. | Naushad, Mu | Awual, Md Rabiul
Recently, hetero junction materials (p-n-p and n-p-n) have been developed for uplifting the visible light activity to destroy the harmful pollutants in wastewater. This manuscript presents a vivid description of novel n-p-n junction materials namely CeO₂-PPy-ZnO. This novel n-p-n junction was applied as the photocatalyst in drifting the mobility of charge carriers and hence obtaining the better photocatalytic activity when compared with p-n and pure system. Such catalyst's syntheses were successful via the copolymerization method. The structural, morphological and optical characterization techniques were applied to identify the physio-chemical properties of the prepared materials. Additionally, the superior performance of this n-p-n nanostructured material was demonstrated in the destruction of micro organic (chlorophenol) toxic wastes under visible light. The accomplished ability of the prepared catalysts (up to 92% degradation of chlorophenol after 180 min of irradiation) and their profound degradation mechanism was explained in detail.
显示更多 [+] 显示较少 [-]Inventory of riverine dissolved organic carbon in the Bohai Rim
2022
Sun, Cece | Liu, Jun | Li, Menglu | Zang, Jiaye | Wang, Lu | Wu, Wentao | Zhang, Aijun | Wang, Junjie | Ran, Xiangbin
Riverine carbon (C) composition and export are closely related to changes in the coastal environment and climate. Excessive C inputs from rivers to seas and their subsequent decomposition could result in harmful algal blooms and ecosystem degradation in the coastal sea. In this study, we explored the C transportation and composition in the 24 major rivers of the Bohai Sea (BS) Rim based on the investigation of dissolved organic carbon (DOC), carbon stable isotopes (δ¹³CDOC) and chromophoric dissolved organic matter (CDOM). The results showed that the riverine DOC concentrations were high (10.6 ± 6.04 mg/L) in the BS Rim compared with the DOC levels in the main rivers in Eastern China (4.98 ± 2.45 mg/L). The δ¹³CDOC ranged from −28.29‰ to −25.32‰ in the rivers of the BS Rim, suggesting that the DOC mainly originated from riverine plankton, soil organic matter mainly induced by C3 plants, and sewage. The excitation-emission matrix fluorescence spectroscopy of the CDOM indicated that a soluble, microbial by product-like material accounted for the largest proportion (approximately 40%) of CDOM in these rivers and that CDOM mainly originated from autochthonous riverine sources with high protein-like components. The rivers in the BS Rim transported approximately 0.55 Tg C of DOC to the BS each year, with more than 70% of reactive C based on the CDOM composition. The DOC yields in terms of unit drainage area transported from the small rivers to the BS were higher compared to those of the larger rivers in the world, which indicated that the small rivers in the Bohai Rim could be an important source of the C in the BS. This study would enrich our understanding of environmental evolution in coastal areas with numerous small rivers.
显示更多 [+] 显示较少 [-]Cadmium, lead, and mercury mixtures interact with non-alcoholic fatty liver diseases
2022
Nguyen, Hai Duc | Kim, Min-Sun
There is a scarcity of studies on the interactions between heavy metals and non-alcoholic fatty liver disease (NAFLD). Using a variety of statistical approaches, we investigated the impact of three common heavy metals on liver enzymes and NAFLD markers in a Korean adult population. We observed that cadmium, mercury, and lead all demonstrated positive correlations with liver enzymes and NAFLD indices. Our findings were mostly robust in secondary analysis, which included three novel mixture modeling approaches (WQS, qgcomp, and BKMR) as well as in silico investigation of molecular mechanisms (genes, miRNAs, biological processes, pathways, and illnesses). The 16 genes interacted with a mixture of heavy metals, which was linked to the development of NAFLD. Co-expression was discovered in nearly half of the interactions between the 18 NAFLD-linked genes. Key molecular pathways implicated in the pathogenesis of NAFLD generated by the heavy metal combination include activated oxidative stress, altered lipid metabolism, and increased cytokines and inflammatory response. Heavy metal exposure levels were related to liver enzymes and NAFLD indices, and cutoff criteria were revealed. More studies are needed to validate our findings and gain knowledge about the effects of chronic combined heavy metal exposure on adult and child liver function and the likelihood of developing NAFLD. To reduce the occurrence of NAFLD, early preventative and regulatory actions (half-yearly screening of workers at high-risk facilities; water filtration; avoiding excessive amounts of seafood, etc.) should be taken.
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