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Change in diagnostic ratios in expelled oils and residual extracts during semi-open pyrolysis experiments of an organic-rich shale
2022
Li, Zhongxuan | Huang, Haiping | Wang, Qianru | Zheng, Lunju
In order to investigate the effectiveness of diagnostic ratios in polycyclic aromatic hydrocarbon (PAH) source discrimination, semi-open pyrolysis experiments have been performed on an organic-rich, immature shale from the Winnipegosis Formation in southeastern Saskatchewan, Western Canada Sedimentary Basin. The concentrations and distributions of PAHs in expelled oils and residual extracts change drastically with increasing pyrolysis temperatures. The difficulty and inconsistency commonly encountered by using diagnostic ratios for PAH source identification in environmental samples seem to be rooted in the great variation of the diagnostic ratios themselves under different formation temperatures. No single diagnostic ratio allows a simple segregation of PAHs into petrogenic or pyrogenic sources. Some diagnostic ratios such as anthracene/phenanthrene and benz[a]anthracene/chrysene compound pairs are mostly effective for low-temperature pyrolysis, whereas indeno[1,2,3-cd]pyrene/benzo[ghi]perylene, aromatic hydrocarbon ring number distribution and degree of alkylation are mainly valid for high-temperature pyrolysis. The diagnostic ratios based on fluoranthene/pyrene, benzo[bk]fluoranthene/benz[a]pyrene compound pairs enjoy limited validity over a narrow pyrolysis range, whereas parameters derived from aromatic hydrocarbon ring number distribution, degree of alkylation and 1,7-/(2,6- + 1,7-dimentylphenanthrene) may be undistinguishable between petrogenesis and low-temperature pyrolysis. The apparent temperature-related variability must be taken into account when using the diagnostic ratios for source identification purposes. Multiple molecular markers need to be carefully selected to confirm the results obtained with PAH diagnostic ratios. Mechanical use of diagnostic ratios most likely leads to misinterpretation of environmental samples.
Afficher plus [+] Moins [-]Effects of forest management on mercury bioaccumulation and biomagnification along the river continuum
2022
Negrazis, Lauren | Kidd, Karen A. | Erdozain, Maitane | Emilson, Erik J.S. | Mitchell, Carl P.J. | Gray, Michelle A.
Forest management can alter the mobilization of mercury (Hg) into headwater streams and its conversion to methylmercury (MeHg), the form that bioaccumulates in aquatic biota and biomagnifies through food webs. As headwater streams are important sources of organic materials and nutrients to larger systems, this connectivity may also increase MeHg in downstream biota through direct or indirect effects of forestry on water quality or food web structure. In this study, we collected water, seston, food sources (biofilm, leaves, organic matter), five macroinvertebrate taxa and fish (slimy sculpin; Cottus cognata) at 6 sites representing different stream orders (1–5) within three river basins with different total disturbances from forestry (both harvesting and silviculture). Methylmercury levels were highest in water and some food sources from the basin with moderate disturbance (greater clearcutting but less silviculture). Water, leaves, stoneflies and fish increased in MeHg or total Hg along the river continuum in the least disturbed basin, and there were some dissipative effects of forest management on these spatial patterns. Trophic level (δ¹⁵N) was a significant predictor of MeHg (and total Hg in fish) within food webs across all 18 sites, and biomagnification slopes were significantly lower in the basin with moderate total disturbance but not different in the other two basins. The elevated MeHg in lower trophic levels but its reduced trophic transfer in the basin with moderate disturbance was likely due to greater inputs of sediments and of dissolved organic carbon that is more humic, as these factors are known to both increase transport of Hg to streams and its uptake in primary producers but to also decrease MeHg bioaccumulation in consumers. Overall, these results suggest that the type of disturbance from forestry affects MeHg bioaccumulation and trophic transfer in stream food webs and some longitudinal patterns along a river continuum.
Afficher plus [+] Moins [-]Vehicle exhausts contribute high near-UV absorption through carbonaceous aerosol during winter in a fast-growing city of Sichuan Basin, China
2022
Liu, Song | Luo, Tianzhi | Zhou, Li | Song, Tianli | Wang, Ning | Luo, Qiong | Huang, Gang | Jiang, Xia | Zhou, Shuhua | Qiu, Yang | Yang, Fumo
Carbonaceous aerosols pose significant climatic impact, however, their sources and respective contribution to light absorption vary and remain poorly understood. In this work, filter-based PM₂.₅ samples were collected in winter of 2021 at three urban sites in Yibin, a fast-growing city in the south of Sichuan Basin, China. The composition characteristics of PM₂.₅, light absorption and source of carbonaceous aerosol were analyzed. The city-wide average concentration of PM₂.₅ was 87.4 ± 31.0 μg/m³ in winter. Carbonaceous aerosol was the most abundant species, accounting for 42.5% of the total PM₂.₅. Source apportionment results showed that vehicular emission was the main source of PM₂.₅ during winter, contributing 34.6% to PM₂.₅. The light absorption of black carbon (BC) and brown carbon (BrC) were derived from a simplified two-component model. We apportioned the light absorption of carbonaceous aerosols to BC and BrC using the Least Squares Linear Regression with optimal angstrom absorption exponent of BC (AAEBC). The average absorption of BC and BrC at 405 nm were 51.6 ± 21.5 Mm⁻¹ and 17.7 ± 8.0 Mm⁻¹, respectively, with mean AAEBC = 0.82 ± 0.02. The contribution of BrC to the absorption of carbonaceous reached 26.1% at 405 nm. Based on the PM₂.₅ source apportionment and the mass absorption cross-section (MAC) value of BrC at 405 nm, vehicle emission was found to be the dominant source of BrC in winter, contributing up to 56.4%. Therefore, vehicle emissions mitigation should be the primary and an effective way to improve atmospheric visibility in this fast-developing city.
Afficher plus [+] Moins [-]Separating emissions and meteorological impacts on peak ozone concentrations in Southern California using generalized additive modeling
2022
Gao, Ziqi | Ivey, Cesunica E. | Blanchard, Charles L. | Do, Khanh | Lee, Sang-Mi | Russell, Armistead G.
Ozone levels have been declining in the Los Angeles, CA, USA area for the last four decades, but there was a recent uptick in the 4th highest daily maximum 8-h (MDA8) ozone concentrations from 2014 to 2018 despite continued reductions in the estimated precursor emissions. In this study, we assess the emissions and meteorological impacts on the 4th highest MDA8 ozone concentrations to better understand the factors affecting the observed MDA8 ozone using a two-step generalized additive model (GAM)/least squares approach applied to the South Coast Air Basin (SoCAB) for the 1990 to 2019 period. The GAM model includes emissions, meteorological factors, large-scale climate variables, date, and the interactions between meteorology and emissions. A least squares method was applied to the GAM output to better capture the 4th highest MDA8 ozone. The resulting two-step model had an R² of 0.98 and a slope of 1 between the observed and predicted 4th highest MDA8 ozone. Emissions and the interactions between the maximum temperature and emissions explain most of the variation in the peak MDA8 ozone concentrations. Declining emissions have lowered the 4th highest MDA8 ozone concentration. Meteorology explains the higher than expected 4th-high, ozone levels observed in 2014–2018, indicating that meteorology was a stronger forcer than the continued reductions in emissions during that time period. The model was applied to estimate future ozone levels. Meteorology developed from climate modeling of the representative concentration pathway (RCP) scenarios, and two sets of emissions were used in the application. The modeling results indicated climate trends will push ozone levels slightly higher if no further emissions reductions are realized and that of two emissions trajectories modeled, the more stringent is required to reliably meet the federal ozone standard given annual meteorological variability.
Afficher plus [+] Moins [-]Features of the accumulation of macroplastic on the river bottom in the Mekong delta and the impact on fish and decapods
2022
Karpova, Evgeniia | Abliazov, Ernes | Statkevich, Svetlana | Dinh, Cu Nguyen
For the first time, a quantitative assessment of this pollutant was made at the bottom of the rivers of the Mekong basin, and the features of its accumulation and dynamics in bottom sediments and relationship with abundance of fish and decapods were investigated. Sampling of materials for the research was carried out by bottom trawls in the Mekong delta in Vietnam. The amount of macroplastic caught by the trawl from the bottom averaged 33.4 g/100 m². The maximum values of the waste content (up to 923.2 g/100 m²) were confined to the districts of large cities. The distribution of macroplastic was characterized by high spatio-temporal variability. Its amount was significantly (p < 0.05) higher in branches with low monthly flow, in shallow-water areas, as well as in the low-water period. During the flood period, which usually lasts from July to November, the amount of macroplastic at the bottom decreased by an average of 2.5 times. In this study a significant relationship between the number of animals and the mass of macroplastics was statistically proven for most species of fish and decapods. The substrate, containing a significant amount of plastic fragments, attracted aquatic organisms. All in all, we present results for poorly understood processes of transport, deposition and influence of plastic debris in large rivers in regions of monsoon subequatorial climate and show that more efforts should be dedicated to further unravel potentially complex pathways of the plastic exposure to water ecosystems.
Afficher plus [+] Moins [-]Spatial patterning of chlorophyll a and water-quality measurements for determining environmental thresholds for local eutrophication in the Nakdong River basin
2021
Kim, Hyo Gyeom | Hong, Sungwon | Chon, Tae Soo | Joo, Gea-Jae
Management of water-quality in a river ecosystem needs to be focused on susceptible regions to eutrophication based on proper measurements. The stress–response relationships between nutrients and primary productivity of phytoplankton allow the derivation of ecologically acceptable thresholds of stressors under field conditions. However, spatio-temporal variations in heterogeneous environmental conditions have hindered the development of locally applicable criteria. To address these issues, we utilized a combination of a geographically specialized artificial neural network (Geo-SOM, geo-self-organizing map) and linear mixed-effect models (LMMs). The model was applied to a 24-month dataset of 54 stations that spanned a wide spatial gradient in the Nakdong River basin. The Geo-SOM classified 1286 observations in the basin into 13 clusters that were regionally and seasonally distinct. Inclusion of the random effects of Geo-SOM clustering improved the performance of each LMM, which suggests that there were significant spatio-temporal variations in the Chla–stressor relationships. These variations arise owing to differences in background seasonality and the effects of local pollutant variables and land-use patterns. Among the 16 environmental variables, the major stressors for Chla were total phosphate (TP) as a nutrient and biological oxygen demand (BOD) as a non-nutrient according to the results of both Geo-SOM and LMM analyses. Based on LMMs with the random effect of the Geo-SOM clusters on the intercept and the slope, we can propose recommended thresholds for TP (18.5 μg L⁻¹) and BOD (1.6 mg L⁻¹) in the Nakdong River. The combined method of LMM and Geo-SOM will be useful in guiding appropriate local water-quality-management strategies and in the global development of large-scale nutrient criteria.
Afficher plus [+] Moins [-]Agricultural activities compromise ecosystem health and functioning of rivers: Insights from multivariate and multimetric analyses of macroinvertebrate assemblages
2021
Zhang, You | Leung, Jonathan Y.S. | Zhang, Ying | Cai, Yongjiu | Zhang, Zhiming | Li, Kuanyi
Agricultural activities often lead to nutrient enrichment and habitat modification in rivers, possibly altering macroinvertebrate assemblages and hence ecosystem functioning. For the sake of environmental management and conservation, therefore, assessing the impacts of agricultural activities becomes indispensable, especially when these activities are predicted to be intensified in the future. In this study, the plain river network in the Lake Chaohu Basin was chosen to examine how agricultural activities influence the functioning of rivers by assessing land use, water quality, habitat condition and macroinvertebrate assemblages, followed by calculating the macroinvertebrate-based multimetric index (MMI) to indicate overall ecosystem health of the rivers. We found that agricultural activities lowered the diversity of macroinvertebrates (e.g. total number of taxa and Simpson index) primarily due to elevated ammonium concentrations in water and reduced microhabitat types, thereby impairing the habitat integrity and nutrient cycling of rivers. The macroinvertebrate-based MMI was positively correlated with increasing habitat quality but negatively with increasing nutrient concentrations, suggesting its high reliability for indicating the impacts of agricultural activities, which was further substantiated by classification and regression tree (CART) analysis. We recommend analyzing macroinvertebrate assemblages using both multivariate and multimetric approaches to offer a more comprehensive evaluation of the impacts of agricultural activities on ecosystem health. Some environmental (CODMₙ, NH₄⁺-N and PO₄³⁻-P) and biological parameters (total number of taxa), however, can be used as good proxies for MMI, when time and resources for gathering information to develop MMI are limited.
Afficher plus [+] Moins [-]Microplastic pollution in the Yangtze River Basin: Heterogeneity of abundances and characteristics in different environments
2021
Zhang, Zeqian | Deng, Chenning | Dong, Li | Liu, Lusan | Li, Haisheng | Wu, Jia | Ye, Chenlei
Microplastic pollution in the Yangtze River Basin has become a major concern; however, the variations in different environmental compartments are unknown. Here, we compiled published information including detection methods, occurrence, and characterization of microplastics from 624 sampling sites in river water, river sediment, lake and reservoir water, and lake and reservoir sediment in the Yangtze River Basin. The spatial distribution of sampling sites shows fractal pattern and was uniformly concentrated around the main stream of the Yangtze River and the lake geographical zone. Collection, pretreatment, identification, and quantification processes varied among different studies. Non-parametric tests were performed to compare the different microplastic indices. A Pearson correlation analysis was used to study the relationship between microplastic pollution and local socioeconomic conditions. We found that the microplastic size and abundance distribution in river water and lake and reservoir water showed different patterns for different sampling methods, indicating that different methods influenced the results. Population density and urbanization rate are suggested to be important factors influencing the spatial heterogeneity of microplastic abundances in water, rather than in sediment. The microplastic abundances in lake and reservoir water were higher than that in river water in bulk samples. However, microplastic abundances among different sediment environments shows no significant difference. For bulk water samples and sediment samples overall, the proportion of small microplastics (<1 mm, i.e. SMP), fibers, transparent debris, and polypropylene (PP) were 65.1%, 67.8%, 31.8%, and 29.7%, respectively. The microplastic characteristics of lake and reservoir water and sediment were similar, differing from those of river water and sediment. This study provides the first basin scale insight into microplastic occurrence and characteristics in different environments in the Yangtze River Basin.
Afficher plus [+] Moins [-]Ecological and health risk assessments and water quality criteria of heavy metals in the Haihe River
2021
Cui, Liang | Wang, Xiaonan | Li, Ji | Gao, Xiangyun | Zhang, Jiawen | Liu, Zhengtao
Heavy metal pollution is an issue of wide concern owing to the toxic and bioaccumulative properties of many heavy metals and their tendencies to persist in the environment. The Haihe River is an important river in the Beijing–Tianjin–Hebei region, and heavy metal pollution of the basin has attracted considerable attention. This study determined the concentrations of 14 heavy metals (As, Ba, Cd, Co, Cr, Cu, Hg, Mn, Ni, Pb, Sb, Se, Sn, and Zn) in water, sediments, and fish samples from the Haihe River basin. The results showed that the concentrations ranged from 0.08 μg L⁻¹ to 60.49 μg L⁻¹ in water, 0.11 mg kg⁻¹ to 229.20 mg kg⁻¹ in sediments, and 0.01 mg kg⁻¹ to 11.72 mg kg⁻¹ in fish. We derived the ambient water quality criteria (AWQC) value of each heavy metal with respect to human health, and then performed a comprehensive risk assessment according to the native parameters. The human health AWQC values for the assessed 14 heavy metals ranged from 0.16 μg L⁻¹ to 726.53 μg L⁻¹. The health risks posed by As, Cr, Hg, and Sb and the ecological risks associated with Ni, Cu, Cr, Zn, Cd, Co, Hg, and Sn were found to be issues of concern. The results of a sensitivity analysis revealed that the highest contributing parameter was i) the concentration in water (Cw) for Cd, Co, Mn, Sb, and Sn; ii) the intake rate of water (IRw) for As, Ba, Cr, Hg, Ni, Pb, and Se; and iii) the concentration in fish (Cf) for Cu and Zn. The results of this research could contribute to the information required for water quality assessments and the development of water quality standards.
Afficher plus [+] Moins [-]Deep winter intrusions of urban black carbon into a canyon near Santiago, Chile: A pathway towards Andean glaciers
2021
Huneeus, Nicolás | Lapere, Rémy | Mazzeo, Andrea | Ordóñez Morales, César Eduardo | Donoso, Nicolás | Munoz, Ricardo | Rutllant, José A.
Black carbon transport from the Santiago Metropolitan Area, Chile, up to the adjacent Andes Cordillera and its glaciers is of major concern. Its deposition accelerates the melting of the snowpack, which could lead to stress on water supply in addition to climate feedback. A proposed pathway for this transport is the channelling through the network of canyons that connect the urban basin to the elevated summits, as suggested by modelling studies, although no observations have validated this hypothesis so far. In this work, atmospheric measurements from a dedicated field campaign conducted in winter 2015, under severe urban pollution conditions, in Santiago and the Maipo canyon, southeast of Santiago, are analysed. Wind (speed and direction) and particulate matter concentrations measured at the surface and along vertical profiles, demonstrate intrusions of thick layers (up to 600 m above ground) of urban black carbon deep into the canyon on several occasions. Transport of PM down-valley occurs mostly through shallow layers at the surface except in connection with deep valley intrusions, when a secondary layer in altitude with return flow (down-valley) at night is observed. The transported particulate matter is mostly from the vicinity of the entrance to the canyon and uncorrelated to concentrations observed in downtown Santiago. Reanalyses data show that for 10% of the wintertime days, deep intrusions into the Maipo canyon are prevented by easterly winds advecting air pollutants away from the Andes. Also, in 23% of the cases, intrusions proceed towards a secondary north-eastward branch of the Maipo canyon, leaving 67% of the cases with favourable conditions for deep penetrations into the main Maipo canyon. Reanalyses show that the wind directions associated to the 33% anomalous cases are related to thick cloud cover and/or the development of coastal lows.
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