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Spatial distribution, pollution characterization, and risk assessment of environmentally persistent free radicals in urban road dust from central China
2022
Feng, Wenli | Zhang, Yongfang | Huang, Liangliang | Li, Yunlin | Guo, Qingkai | Peng, Haoyan | Shi, Lei
Environmentally persistent free radicals (EPFRs) have aroused widespread concern due to their potential adverse health effects. Research on EPFRs in road dust is still very limited. In this study, 86 road dust samples were collected using vacuum sampling in a rapidly developing city in central China. The pollution characterization and health risk of EPFRs in the urban road dust were then systematically analyzed. The results showed the average concentrations of EPFRs in urban road dust and fraction of particle with aerodynamic diameters lower than 10 μm (PM₁₀) were 2.24 × 10¹⁷ to 3.72 × 10¹⁹ spins·g⁻¹ and 6.02 × 10¹⁷ to 1.41 × 10²⁰ spins g⁻¹, respectively. The concentrations of EPFRs in dust from expressways, arterial roads, and secondary trunk roads were significantly higher than those found in the remaining road types. The g-factors of 2.0032–2.0039 indicated that the EPFRs have consisted of oxygen-centered and carbon-centered radicals or carbon-centered radicals with nearby oxygen or halogen atoms. Moreover, three decay patterns of EPFRs were observed: a fast decay followed by a slow decay, a single slow decay, and the slowest decay. In addition, a comparative evaluation was made for probabilistic risk assessments of exposure to the EPFRs in road dust and the PM₁₀ fraction. Compared with road dust, the probability of the number of equivalent cigarettes to exceed the 100 and 200 cigarettes for inhaling EPFRs in the PM₁₀ fraction increased by 27.0% and 25.0%, respectively. The simulation results showed the PM₁₀ fraction were primarily deposited in the upper respiratory tract regions (57.1%) and pulmonary regions (28.8%). The findings of this study suggest a potential risk of EPFRs in inhalable particles and provide a new insight for further exploration of the EPFRs in fine particles of road dust.
显示更多 [+] 显示较少 [-]AOX contamination in Hangzhou Bay, China: Levels, distribution and point sources
2018
Xie, Ya-Wei | Chen, Lu-Jun | Liu, Rui | Tian, Jin-Ping
The parameter AOX (adsorbable organic halogens) indicates the total amount of organic halogens in an environment. Seawater and surface sediment samples from 12 sample sites in the Hangzhou Bay (HZB), China, were analyzed for AOX to investigate its contamination status. In this study, the AOX concentration ranged from 140.6 ± 45.6 μg/L to 716.1 ± 62.3 μg/L in seawater of the HZB, and from 11.3 ± 2.4 mg/kg to 112.7 ± 7.2 mg/kg in the sediment. Ocean currents, fluvial currents and the Yangtze River exerted profound influences on the distribution of AOX in the HZB. The point sources around the HZB, represented by wastewater treatment plants, discharged at least 645.4 t AOX into the HZB every year, most of which was generated by industrial activities rather than the human daily activities.
显示更多 [+] 显示较少 [-]Gradient measurements of gaseous elemental mercury (Hg0) in the marine boundary layer of the northwest Sea of Japan (East Sea)
2018
Kalinchuk, Viktor | Lopatnikov, Evgeny | Astakhov, Anatoly
Gaseous elemental mercury (Hg0) is a prolific and persistent contaminant in the atmosphere. Atmospheric concentrations of Hg0 were determined from 17 September to 7 October 2015 in the northwest Sea of Japan aboard the Russian research vessel Professor Gagarinsky. Simultaneous measurements of Hg0 concentrations were performed 2 m and 20 m above the sea surface using automatic Hg0 analysers RA-915M and RA-915+, respectively. Concentrations ranged from 0.3 to 25.9 ng/m3 (n = 5207) and from 0.3 to 27.8 ng/m3 (n = 4415), with medians of 1.7 and 1.6 ng/m3, respectively. Elevated Hg0 was observed during three episodes from 19 to 22 September, likely caused by one or more of the following factors: 1) atmospheric transport of Hg0 from the west and south-west (from N. Korea, China, and the Yellow Sea region); 2) Hg0 emission from the sea due to pollution by water from the Tumannaya River; or 3) underwater geological activities. Increased Hg0 concentration was observed during periods when air masses flowed from the south, and low concentrations were observed when air masses came from the north. A daytime increase of Hg0 concentrations at a height of 2 m occurred simultaneously with decreasing Hg0 at a height of 20 m. These diurnal variations suggest that two contrasting processes occur during the daytime in the marine boundary layer (MBL): Hg0 emission from the sea surface and Hg0 oxidation in the MBL by active halogens formed by photolysis.
显示更多 [+] 显示较少 [-]Protective effect of Urtica dioica in induced neurobehavioral changes, nephrotoxicity and hepatotoxicity after chronic exposure to potassium bromate in rats
2021
Dhouibi, Raouia | Affes, Hanen | Ben Salem, Maryem | Charfi, Slim | Marekchi, Rim | Hammami, Serria | Zeghal, Khaled | Ksouda, Kamilia
Chronic exposure to potassium bromate (KBrO₃), a toxic halogen in the environment, has become a global problem of public health. The current study aims to elucidate for the first time the effect of Urtica dioica (UD) on behavioural changes, oxidative stress, and histopathological changes induced by KBrO₃ in the cerebellum, kidney, liver and other organs of adult rats.The rats were divided into four groups: group 1 served as a control received physiological serum, Group 2 received KBrO₃ (2 g/L of drinking water), group 3 received KBrO₃ and Urtica dioica (100 mg/kg), and group 4 received KBrO₃ and Urtica dioica (400 mg/kg). We then measured behavioural changes, oxidative stress, and biochemical and histological changes in the cerebellum, liver, kidney and others organs in these rats. After 30 days of treatment, the animals were sacrificed.We observed significant behavioural changes in KBrO₃-exposed rats. When investigating redox homeostasis in the cerebellum, we found that mice treated with KBrO₃ had increased lipid peroxidation and protein oxidation in the cerebellum. In addition, it inhibits hepatic and lipid peroxidation (malondialdehyde), advanced oxidation protein product (AOPP), attenuates KBrO₃-mediated enzyme depletion, catalase, superoxide dismutase, glutathione peroxidase enzymatic and antioxidant activities in the liver and kidney. Rats that were co-managed with Urtica dioica at the high portion of 400 mg/kg indicated a higher effect than that treated with the low dose of 100 mg/kg practically in all the tests carried out.Our results demonstrate that Urtica dioica is a potential therapeutic agent for oxidative stress associated with neurodegenerative diseases.
显示更多 [+] 显示较少 [-]Amino, nitro, chloro, hydroxyl and methyl substitutions may inhibit the binding of PAHs with DNA
2021
Qin, Chao | Hu, Xiaojie | Yang, Bing | Liu, Juan | Gao, Yanzheng
The binding of PAHs with DNA to form PAH-DNA adducts is a crucial step in PAH-induced carcinogenesis. How functional groups affect this binding is largely unknown. Here, we observed that functional group substitutions strongly inhibited PAH-DNA binding. Additionally, –OH substitution has the most potent inhibitory effect as it causes the smallest change in the electrostatic surface potential. Fourier transform infrared spectroscopy and molecular docking analyses demonstrated that PAH derivatives bind with guanine via intercalation and groove binding and then non-specifically insert into the major/minor grooves of DNA. Quantum chemical calculations suggested that hydrogen/halogen bonding may be essential in affecting the binding of functional group-substituted PAHs with DNA. It was further revealed that Log KOA and the PAH derivatives’ melting points correlated significantly with binding affinity, implying that changes in the physicochemical characteristics are important factors. This study opens a new window for understanding the relationship between highly toxic PAH derivatives and genetic materials.
显示更多 [+] 显示较少 [-]Study on emission of hazardous trace elements in a 350 MW coal-fired power plant. Part 1. Mercury
2017
Zhao, Shilin | Duan, Yufeng | Chen, Lei | Li, Yaning | Yao, Ting | Lichuanjushi, | Liu, Meng | Lu, Jianhong
Hazardous trace elements (HTEs), especially mercury, emitted from coal-fired power plants had caused widespread concern worldwide. Field test on mercury emissions at three different loads (100%, 85%, 68% output) using different types of coal was conducted in a 350 MW pulverized coal combustion power plant equipped with selective catalytic reduction (SCR), electrostatic precipitator and fabric filter (ESP + FF), and wet flue gas desulfurization (WFGD). The Ontario Hydro Method was used for simultaneous flue gas mercury sampling for mercury at the inlet and outlet of each of the air pollutant control device (APCD). Results showed that mercury mass balance rates of the system or each APCD were in the range of 70%–130%. Mercury was mainly distributed in the flue gas, followed by ESP + FF ash, WFGD wastewater, and slag. Oxidized mercury (Hg2+) was the main form of mercury form in the flue gas emitted to the atmosphere, which accounted for 57.64%–61.87% of total mercury. SCR was favorable for elemental mercury (Hg0) removal, with oxidation efficiency of 50.13%–67.68%. ESP + FF had high particle-bound mercury (Hgp) capture efficiency, at 99.95%–99.97%. Overall removal efficiency of mercury by the existing APCDs was 58.78%–73.32%. Addition of halogens or oxidants for Hg0 conversion, and inhibitors for Hg0 re-emission, plus the installation of a wet electrostatic precipitator (WESP) was a good way to improve the overall removal efficiency of mercury in the power plants. Mercury emission factor determined in this study was from 0.92 to 1.17 g/1012J. Mercury concentration in the emitted flue gas was much less than the regulatory limit of 30 μg/m3. Contamination of mercury in desulfurization wastewater should be given enough focus.
显示更多 [+] 显示较少 [-]Effects of microplastic sorption on microbial degradation of halogenated polycyclic aromatic hydrocarbons in water
2022
Sun, Qing | Ren, Shu-Yan | Ni, Hong-Gang
Halogenated PAHs (HPAHs) are ubiquitous in the environment and have a toxicity similar to that of dioxin. Microplastics exist widely in the environment, and their sorption allows them to act as carriers of HPAHs, potentially changing the bioavailability of HPAHs. However, to the best of our knowledge related studies are limited. In this study, degrading bacteria of five HPAHs were cultivated from mangrove sediments. Among them, the Hyphomicrobium genus has good degradation ability on 9−BrAnt, 2−BrPhe and 2−ClPhe. The degradation process is in line with the first−order degradation kinetic characteristics. The kinetic equations of five kinds of HPAHs showed that the degradation half−lives are 0.65 days (2−BrFle), 0.79 days (9−ClPhe), 1.50 days (2−ClAnt), 5.94 days (9−BrPhe) and 14.1 days (9−BrAnt). The greater the number of benzene rings and the heavier the halogen substituents, the slower the degradation of HPAHs. The sorption of microplastics inhibited the biodegradation of HPAHs, and the degradation half−life of HPAHs will be extended from 0.65 to 14.1 days (the average is 4.59 days) to 1.71–9.93 days (average 5.40 days) for PA, 0.70–35.2 days (average 12.8 days) for PE, 6.02–28.2 (average 15.7 days) days for POM, and 4.60–24.0 (average 19.2 days) days for PP, which is mainly related to the partition coefficient between microplastics and water. This study provides a reference for reducing the uncertainty of the ecological risk assessment of HOCs in the aquatic environment.
显示更多 [+] 显示较少 [-]Photolytic kinetics of pharmaceutically active compounds from upper to lower estuarine waters: Roles of triplet-excited dissolved organic matter and halogen radicals
2021
Hou, Zhichao | Fang, Qi | Liu, Huaying | Li, Yingjie | Zhao, Qun | Zhang, Zhiyu | Lei, Yajie | Tian, Senlin
Photodegradation is a major elimination route of many pharmaceutically active compounds (PhACs) in natural surface waters, yet their photolytic behavior in estuarine waters with salinity gradient change is largely unknown. Herein, sulfamethazine and carbamazepine were taken as representative PhACs to explore the photolytic kinetic differences in Qinzhou Bay estuarine water samples collected from upper to lower reaches. Rapid photodegradation of sulfamethazine was found in lower estuarine water relative to upstream estuarine water; whereas for carbamazepine, photolytic rate was inversely proportional to the salinity of estuarine waters. Experiments with extracted estuarine dissolved organic matter (E-DOM) imply that the multivariate effects of triplet-excited E-DOM (³E-DOM∗) and halide ions are responsible for the enhancement photolysis of sulfamethazine. Radical scavenging experiments suggest that the photolysis enhancement can be ascribed to the contribution of reactive halogen species (RHS), while their contribution to carbamazepine is negligible and ³E-DOM∗ is the dominant reactive species for its photodegradation. This indicates that the reactivity differences with RHS and ³DOM∗ affect the photolytic kinetics of PhACs from upper estuarine waters to lower reaches, which is also supported by a good linear relationship between the ratios of photolytic rates for ten PhACs in E-DOM solution with/without halides and the ratios of the reactivity of these pollutants with RHS and ³DOM∗. These findings show that the different reactivity of PhACs with ³E-DOM∗ and RHS influences the photolytic kinetics in estuarine waters with different salinity, and highlights the photochemical behavior of organic micropollutants from upstream to downstream estuarine waters.
显示更多 [+] 显示较少 [-]Effect of microplastic size on the adsorption behavior and mechanism of triclosan on polyvinyl chloride
2019
Ma, Jie | Zhao, Jinghua | Zhu, Zhilin | Li, Liqing | Yu, Fei
Microplastics in water environment and its ability to load various environmental pollutants have attracted wide attention in recent years. However, effect of microplastic size on the adsorption behavior of environmental pollutants and interaction mechanism has not been thoroughly explored. In this study, triclosan (TCS) was selected as model pollutant, and polyvinyl chloride (PVC) with different particle sizes (small size (<1 μm) is recorded as PVC-S and PVC-L means large particle size of about 74 μm) were used as the typical microplastics, the adsorption behavior of TCS on PVC was investigated by studying kinetics, isotherms, and other influencing factors, such as pH and salinity. The results indicate PVC-S has greater distribution coefficient kd values of TCS (1.35 L/g > 1.05 L/g) and stronger adsorption capacity (12.7 mg/g > 8.98 mg/g) compared with PVC-L, which may be due to higher specific surface area, stronger hydrophobicity and relatively small electronegative property of PVC-S. Moreover, the initial pH value and salinity of the solution played crucial role in the adsorption process. The distribution diffusion mechanisms (including liquid-film diffusion and intra-particle diffusion), hydrophobic interaction, electrostatic interaction, halogen bonding, and hydrogen bonding may be the important reasons for adsorption. These findings show that MPs with different particle sizes have vary adsorption behaviors and load capacities for environmental pollutants, which deserve our further concerned.
显示更多 [+] 显示较少 [-]Indirect photodegradation of sulfisoxazole: Effects of environmental factors (CDOM, pH, salinity, HCO3−, metal ions, halogen ions and NO3−)
2022
Duan, Jiaqi | Jian, Huimin | Dou, Qiwei | Shi, Xiaoyong | Su, Rongguo
It's a new perspective to explore the influences of chromophoric dissolved organic matter (CDOM) components and environmental factors on the removal of sulfisoxazole (SIX) from the water matrix. Reactive intermediates (RIs) trapping experiments demonstrated that excited triplet-state CDOM (³CDOM⁎) played a dominant promoting role (54.11%) in the CDOM-mediated SIX indirect photodegradation. Additionally, terrestrial humic-like (C1, C3 and C4) and marine humic-like (C2) fluorescent components were identified by parallel factor (PARAFAC) analysis of CDOM excitation-emission matrix spectroscopy (EEMs). C1 and C4 were significantly correlated (R² > 0.91) with the SIX degradation rate owing to their higher productivity of RIs and a greater contribution to the production of ³CDOM⁎ compared to others. Salinity, pH and HCO₃⁻ were conducive to the SIX indirect photodegradation, while metal ions (Fe³⁺ and Cu²⁺), halogen ions (Cl⁻ and Br⁻) and NO₃⁻ were opposite. These findings are essential for understanding the environmental fate of SIX in coastal waters.
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