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Mechanism of uranium release from uranium mill tailings under long-term exposure to simulated acid rain: Geochemical evidence and environmental implication
2019
Yin, Meiling | Sun, Jing | Chen, Yongheng | Wang, Jin | Shang, Jianying | Belshaw, Nick | Shen, ChuanChou | Liu, Juan | Li, Huosheng | Linghu, Wensheng | Xiao, Tangfu | Dong, Xinjiao | Song, Gang | Xiao, Enzong | Chen, Diyun
To date, there is not sufficient knowledge to fully understand the occurrence, transport and fate of residual uranium (U) from uranium mill tailings (UMT). Herein this study investigated different U release behaviors from natural UMT (without grinding) under four simulated acid rain (pH = 2.0–5.0) compared with controlled scenario (pH = 6.0) for 25 weeks. The results showed that the most notable U release was observed from UMTₚH₂.₀, followed by UMTₚH₃.₀ whereas a nonlinear relationship between pH and U release was observed from UMTₚH₄.₀–₆.₀. The divergence of U release behaviors was attributed to the presence of minerals such as calcite and clinochlore. Autunite, a secondary mineral formed after leaching, might regulate U release in UMTₚH₃.₀–₆.₀. Fick theory model revealed the shift of U release mechanism from surface dissolution to diffusion transport for UMTₚH₂.₀, UMTₚH₃.₀ and UMTₚH₅.₀ at varied stage, whereas UMTₚH₄.₀ and UMTₚH₆.₀ displayed univocal dissolution and diffusion mechanism, respectively. This study highlights the necessity of performing long-term leaching tests to detect the “shift event” of leaching kinetics and to better understand the mechanism of U release influenced by mineralogy of the natural UMT under simulated acid rain conditions, which is conducive to developing UMT management strategies to minimize the risk of U release and exposure.
Show more [+] Less [-]Bibliometric study of the toxicology of nanoescale zero valent iron used in soil remediation
2019
Vanzetto, Guilherme Victor | Thomé, Antonio
The application of nanoscale zero-valent iron is one of the most widely used remediation technologies; however, the potential environmental risks of this technology are largely unknown. In order to broaden the knowledge on this subject, the present work consists of a bibliometric study of all of publications related to the toxicity of zero-valent iron nanoparticles used in soil remediation available from the Scopus (Elsevier) and Web of Science (Thompson Reuters) databases. This study presents a temporal distribution of the publications, the most cited articles, the authors who have made the greatest contribution to the theme, and the institutions, countries, and scientific journals that have published the most on this subject. The use of bibliometrics has allowed for the visualization of a panorama of the publications, providing an appropriate analysis to guide new research towards an effective contribution to science by filling the existing gaps. In particular, the lack of studies in several countries reveals a promising area for the development of further research on this topic.
Show more [+] Less [-]Oxidation of benzoic acid from biomass burning in atmospheric waters
2019
Santos, Patrícia S.M. | Cardoso, Helena B. | Rocha-Santos, Teresa A.P. | Duarte, Armando C.
This work evaluates the degradation of benzoic acid, a tracer from biomass burning, by different oxidation agents (Fe (III); H₂O₂; sunlight; and combinations of the previous ones) in model solutions and in real atmospheric waters. The extent of reactions was assessed by Ultraviolet–Visible and molecular fluorescence spectroscopies. The oxidation of benzoic acid occurred with the chemical oxidants Fe (III), H₂O₂, Fe (III) and H₂O₂ simultaneously in the presence of sunlight, and with Fe (III) and H₂O₂ simultaneously in the absence of light. The decrease of the pH value from neutral to acid for atmospheric waters generally increased the extent of oxidation. Sunlight was an important oxidation agent, and its combination with chemical oxidants increased the oxidation rate of benzoic acid, possibly due to the photogeneration of hydroxyl radicals. The results also suggested the occurrence of direct and indirect photolysis of benzoic acid in atmospheric waters. Moreover, the oxidation of benzoic acid produced new and more complex chromophoric compounds, which were then degraded. In addition, the nocturnal period is not sufficient for the full degradation of benzoic acid and of the intermediates formed by Fenton-like oxidation. The diurnal period may be enough for their full degradation through photo-Fenton-like oxidation, but this depends on the composition of the atmospheric waters, namely of the chromophoric content. Thus, this study highlights that benzoic acid from biomass burning, and its derivatives, may persist in atmospheric waters for periods of longer than one day, becoming available for other reactions, and may also affect the terrestrial and aquatic ecosystems through the wet depositions.
Show more [+] Less [-]Characterizing spatiotemporal dynamics of anthropogenic heat fluxes: A 20-year case study in Beijing–Tianjin–Hebei region in China
2019
Chen, Shanshan | Hu, Deyong | Wong, Ernest Man-Sing | Ren, Huazhong | Cao, Shisong | Yu, Chen | Ho, Hung Chak
Rapid urbanization, which is closely related to economic growth, human health, and micro-climate, has resulted in a considerable amount of anthropogenic heat emissions. The lack of estimation data on long-term anthropogenic heat emissions is a great concern in climate and urban flux research. This study estimated the annual average anthropogenic heat fluxes (AHFs) in Beijing–Tianjin–Hebei region in China between 1995 and 2015 on the basis of multisource remote sensing images and ancillary data. Anthropogenic heat emissions from different sources (e.g., industries, buildings, transportation, and human metabolism) were also estimated to analyze the composition of AHFs. The spatiotemporal dynamics of long-term AHFs with high spatial resolution (500 m) were estimated by using a refined AHF model and then analyzed using trend and standard deviation ellipse analyses. Results showed that values in the region increased significantly from 0.15 W· m−2 in 1995 to 1.46 W· m−2 in 2015. Heat emissions from industries, transportation, buildings, and human metabolism accounted for 64.1%, 17.0%, 15.5%, and 3.4% of the total anthropogenic heat emissions, respectively. Industrial energy consumption was the dominant contributor to the anthropogenic heat emissions in the region. During this period, industrial heat emissions presented an unstable variation but showed a growing trend overall. Heat emissions from buildings increased steadily. Spatial distribution was extended with an increasing tendency of the difference between the maximum and the minimum and was generally dominated by the northeast–southwest directional pattern. The spatiotemporal distribution patterns and trends of AHFs could provide vital support on management decision in city planning and environmental monitoring.
Show more [+] Less [-]First account of plastic pollution impacting freshwater fishes in the Amazon: Ingestion of plastic debris by piranhas and other serrasalmids with diverse feeding habits
2019
Andrade, Marcelo C. | Winemiller, Kirk O. | Barbosa, Priscilla S. | Fortunati, Alessia | Chelazzi, David | Cincinelli, Alessandra | Giarrizzo, Tommaso
Reported here is the first evidence of plastic ingestion by freshwater fishes in the Amazon. Plastic bags, bottles, fishing gear, and other products are entering Amazonian water bodies and degrade into meso- and micro-plastic particles that may be ingested, either directly or indirectly via food chains, by fishes. Examination of stomach contents from 172 specimens of 16 serrasalmid species from lower Xingu River Basin revealed consumption of plastic particles by fishes in each of three trophic guilds (herbivores, omnivores, carnivores). Overall, about one quarter of specimens and 80% of species analyzed had ingested plastic particles ranging from 1 to 15 mm in length. Fourier transform infrared spectroscopy indicated 12 polymer types, including 27% identified as polyethylene, 13% polyvinyl chloride, 13% polyamide, 13% polypropylene, 7% poly(methyl methacrylate), 7% rayon, 7% polyethylene terephtalate, and 13% a blend of polyamide and polyethylene terephtalate. Dimensions of ingested plastic particles varied among trophic guilds, even though the frequency and mass of ingested particles were not significantly different among fishes with different feeding habits.
Show more [+] Less [-]Atmospheric fate of peroxyacetyl nitrate in suburban Hong Kong and its impact on local ozone pollution
2019
Zeng, Lewei | Fan, Gang-Jie | Lyu, Xiaopu | Guo, Hai | Wang, Jia-Lin | Yao, Dawen
Peroxyacetyl nitrate (PAN) is an important reservoir of atmospheric nitrogen, modulating reactive nitrogen cycle and ozone (O3) formation. To understand the origins of PAN, a field measurement was conducted at Tung Chung site (TC) in suburban Hong Kong from October to November 2016. The average level of PAN was 0.63 ± 0.05 ppbv, with a maximum of 7.30 ppbv. Higher PAN/O3 ratio (0.043–0.058) was captured on episodes, i.e. when hourly maximum O3 exceeded 80 ppbv, than on non-episodes (0.01), since O3 production was less efficient than PAN when there was an elevation of precursors (i.e. volatile organic compounds (VOCs) and nitrogen oxide (NOx)). Model simulations revealed that oxidations of acetaldehyde (65.3 ± 2.3%), methylglyoxal (MGLY, 12.7 ± 1.2%) and other oxygenated VOCs (OVOCs) (8.0 ± 0.6%), and radical cycling (12.2 ± 0.8%) were the major production pathways of peroxyacetyl (PA) radical, while local PAN formation was controlled by both VOCs and nitrogen dioxide (NO2). Among all VOC species, carbonyls made the highest contribution (59%) to PAN formation, followed by aromatics (26%) and biogenic VOCs (BVOCs) (10%) through direct oxidation/decomposition. Besides, active VOCs (i.e. carbonyls, aromatics, BVOCs and alkenes/alkynes) could stimulate hydroxyl (OH) production, thus indirectly facilitating the PAN formation. Apart from primary emissions, carbonyls were also generated from oxidation of first-generation precursors, i.e., hydrocarbons, of which xylenes contributed the most to PAN production. Furthermore, PAN formation suppressed local O3 formation at a rate of 2.84 ppbv/ppbv, when NO2, OH and hydroperoxy (HO2) levels decreased and nitrogen monoxide (NO) value enhanced. Namely, O3 was reduced by 2.84 ppbv per ppbv PAN formation. Net O3 production rate was weakened (∼36%) due to PAN photochemistry, so as each individual production and loss pathway. The findings advanced our knowledge of atmospheric PAN and its impact on O3 production.
Show more [+] Less [-]Arthritis diagnosis and early-life exposure to air pollution
2019
Shepherd, Andrew | Mullins, Jamie T.
Evaluate the relationship between arthritis diagnosis in those over 50 and exposure to extreme air pollution in utero or infancy (<1 year of age).Compare rates of arthritis diagnosis between groups that experienced differential air pollution exposure in early-life due to quasi-random variation in birth location and date relative to the 1952 Great Smog in London. We use regression-estimated difference-in-differences analyses based on English Longitudinal Study of Aging (ELSA) data.In the 2816 respondent sample, aged 51–62, the arthritis diagnosis rate is 22.8%, with 16.4% reporting osteoarthritis and 4.6% reporting rheumatoid arthritis. We estimate that exposure to the Great Smog in infancy increases the arthritis diagnosis rate by 23.4 percentage points (95% CI: 1.97 to 44.8). Decomposing these results by type of arthritis reveals that the rheumatoid arthritis diagnosis rate increases due to infant exposure are larger and more significant than those for osteoarthritis: 14.9 percentage points (95% CI: 0.495 to 29.4) versus 9.5 percentage points (95% CI: −11.9 to 30.8). In utero exposure is not associated with significant increases in arthritis diagnosis rates.Our results are the first to link early-life air pollution exposure to later-life arthritis diagnoses, and suggest a particularly strong link for RA. These findings are consistent with those of shorter-term, correlational studies, and indicate that health effects of air pollution exposure can span decades and extend beyond cardiopulmonary systems.
Show more [+] Less [-]Redox properties and dechlorination capacities of landfill-derived humic-like acids
2019
Xiao, Xiao | Xi, Bei-Dou | He, Xiao-Song | Zhang, Hui | Li, Yan-Hong | Pu, Shengyan | Liu, Si-Jia | Yu, Min-Da | Yang, Chao
Electron transfer capacities (ETC) of humic-like acids (HLA) and their effects on dechlorination are dependent on their redox-active properties. Aging and minerals can affect the chemical compositions and structures of HLA. However, the underlying mechanism and the impacts on the dechlorination capacities of HLA are poorly understood. We investigated how redox properties change in association with the intrinsic chemical natures and exterior minerals of the HLA extracted from landfilled solid wastes. Furthermore, the ETC of the landfill-derived HLA could be strengthened by increasing landfill age and demineralization, thereby facilitating the dechlorination of pentachlorophenol (PCP). The HLA molecules started to polymerize aromatic macromolecules during landfilling, leading to an increase in ETC and dechlorination capacities. Macromolecular HLA were dissociated to smaller molecules and exposed more aromatic and carboxyl groups when separated from minerals, which enhanced the ETC and the dechlorination abilities of the HLA. Microbial-mediated dechlorination was an effective way to degrade PCP, and almost 80% of the PCP was transformed after 40 days of demineralized HLA and Shewanella oneidensis MR-1 incubation. The demineralization and aging further facilitated the microbial-mediated PCP dechlorination. The findings provide a scientific base for improving in-situ bioremediation of chlorinated compound-contaminated soils using freshly synthesized HLA.
Show more [+] Less [-]Effects of surfactant on the degradation of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) by nanoscale Ag/Fe particles: Kinetics, mechanisms and intermediates
2019
Zheng, Zhiqiang | Lu, Guining | Wang, Rui | Huang, Kaibo | Tao, Xueqin | Yang, Yulu | Zou, Mengyao | Xie, Yingying | Yin, Hua | Shi, Zhenqing | Dang, Zhi
Surfactants are known to enhance the degradation of halogenated organics by nanoscale zerovalent iron (n-ZVI) or n-ZVI-based bimetallic particles, but the mechanism of the promotion is not well understood. In this study, we used nanoscale Ag/Fe particles (n-Ag/Fe) to degrade 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) in different surfactant solutions. The results show that the nonionic surfactant TX-100 had the best promoting effect, which might be attributed to the decrease in particle agglomeration and improvement of mass transfer efficiency after the adsorption of TX-100 on n-Ag/Fe. The distribution analysis of BDE-47 in solid and liquid phases indicates that when the concentration of TX-100 in aqueous solution was above critical micelle concentration, BDE-47 started to dissolve in the liquid phase. Thus, TX-100 micelles can enhance the mass transfer efficiency of BDE-47. However, a too high concentration of TX-100 (above 1.0 mM) would influence the promotion effect of BDE-47 degration, which might be attributed to the excessive and thicker micelles of TX-100 hindering the contact between BDE-47 and n-Ag/Fe. We also studied the degradation pathway of BDE-47 and its products, and found that surfactants did not change the degradation pathway of BDE-47.
Show more [+] Less [-]Are the primary characteristics of polystyrene nanoplastics responsible for toxicity and ad/absorption in the marine diatom Phaeodactylum tricornutum?
2019
Sendra, Marta | Staffieri, Eleonora | Yeste, María Pilar | Moreno-Garrido, Ignacio | Gatica, José Manuel | Corsi, Ilaria | Blasco, Julián
Nowadays, the occurrence of a large volume of plastic litter in oceanic and coastal zones has increased concern about its impacts on marine organisms. The degradation of plastic polymers leads to the formation of smaller fragments at both micro and nano scale (<5 mm and <1 μm respectively). Nanoplastics (NPs), due to their smaller size and high specific surface area can establish colloidal interactions with marine microalgae, therefore potential toxicity can be led. . To assess this hypothesis, the aim of the present study is to examine the behaviour of polystyrene nanoparticles (PS NPs) of different sizes (50 and 100 nm) in marine water and their possible effects at different physiological and cellular levels in the marine diatom Phaeodactylum tricornutum. Different biomarkers and stress responses in P. tricornutum were analysed when organisms were exposed to environmentally relevant PS NPs concentrations between 0.1 and 50 mg L−1. Our results showed significant differences between controls and exposure microalgae, indicating toxicity. After 24 h, an increase in oxidative stress biomarkers, damage to the photosynthetic apparatus, DNA damage and depolarization of mitochondrial and cell membrane from 5 mg L−1 were observed. Further after 72 h the inhibition of population growth and chlorophyll content were observed. Examining effects the effects related to PS NPs size, the smallest (50 nm) induced greater effects at 24 h while bigger PS NPs (100 nm) at72 h. This bigger particles (100 nm) showed more stability (in size distribution and spherical form) in the different culture media assayed, when compared with the rest of particles used. Strong adsorption and/or internalization of PS NPs was confirmed through changes in cell complexity and cell size as well as the fluorescence of 100 nm fluoresbrite PS NPs after washing cell surface.
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