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Ferrate (VI)-mediated transformation of diethyl phthalate (DEP) in soil: Kinetics, degradation mechanisms and theoretical calculation 全文
2021
Yu, Yao | Qi, Yumeng | Li, Chenguang | Cao, Wanming | Chen, Jing | Qu, Ruijuan | Zhou, Dongmei | Wang, Zunyao
Diethyl phthalate (DEP), as a kind of universally used plasticizer, has aroused considerable public concern owing to its wide detection, environmental stability, and potential health risks. In this work, the highly efficient removal of DEP by ferrate (VI) (Fe(VI)) was systematically explored in soil environment. The effects of the oxidant dosages, soil types, as well as the presence of coexisting cations and anions in tested soil on DEP removal were evaluated. When the dosage of Fe(VI) was 20 mM, complete removal of DEP (50 μg/g) was achieved in the tested soil after 2 min of reaction. Furthermore, the removal rate of DEP was closely related to the soil types, and the degradation rates were decreased obviously in red soil (RS), black soil (BS) and paddy soil (PS), probably due to the acidic condition and high content of organic matters. Moreover, the presence of Ca²⁺, Mg²⁺ and Al³⁺ in soil can inhibit the removal of DEP by Fe(VI), while SO₄²⁻ has an slightly promotion effect. Six oxidation intermediates were detected in the reaction process of DEP, product analysis revealed that the transformation of DEP was mainly through two pathways, including hydrolysis and hydroxylation reactions, which were probably mediated by oxygen atom transfer process of Fe(VI). Based on the frontier electron density theory calculation, two ester groups of DEP were prone to be attacked by Fe(VI), and the hydroxyl addition tended to occur at the para-position of one of the ester groups on the benzene ring. This study provides a novel approach for phthalate esters removal from soil using Fe(VI) oxidation and shows new insights into the oxidation mechanisms.
显示更多 [+] 显示较少 [-]A spatio-temporal noise map completion method based on crowd-sensing 全文
2021
Huang, Min | Chen, Lina | Zhang, Yilin
The construction of noise maps is of great significance for the development of urban sustainability and the protection of residents’ physical and mental health. The traditional noise map construction method is difficult to be widely used because of its low update frequency and high drawing cost. Based on the crowd-sensing technology and Latent Factor Model (LFM), this paper proposes a new noise map completion method called Spatial-Temporally Related LFM (STR-LFM) for solving the problem of data sparseness. First, the geographic information features including Point of Interest (POI), road network and building outline are fully excavated, and then combine the correlation of the samples in the time dimension to construct the similarity matrixes. After that, use the k-nearest neighbor algorithm to find out the similar samples of missing positions, and finally regard their weighted fusion as the predicted values. Experimental results show that the recovery error is lower than other commonly used methods, and the proposed method has better stability when faced with data sparseness problems at different levels.
显示更多 [+] 显示较少 [-]Effects of waterborne exposure to environmentally relevant concentrations of selenite on reproductive function of female zebrafish: A life cycle assessment 全文
2021
Mo, Aijie | Wang, Xiaolin | Yuan, Yongchao | Liu, Chunsheng | Wang, Jianghua
Recently, bioaccumulation of dietary organic selenium (Se) in the ovaries and inhibition of reproduction in female aquatic animals have been reported. However, there is limited data on the subtle reproductive impacts of waterborne exposure to inorganic Se in fish. Here, zebrafish embryos (2 h post-fertilization) were exposed to solutions with environmentally relevant levels of Na₂SeO₃ with concentrations of 0 (control), 7.98 ± 0.31, 25.14 ± 0.15, and 79.60 ± 0.81 μg Se/L for 120 d until they reached sexual maturity. Female zebrafish were selected for reproductive toxicity assessment. In the early embryonic stage, whole-mount in situ hybridization of zebrafish embryos showed that waterborne Na₂SeO₃ exposure did not affect the observed location of vasa expression in primordial germ cells at 24, 48, and 72 h post-fertilization. Life-cycle exposure to 25.14 ± 0.15 and 79.60 ± 0.81 μg Se/L Na₂SeO₃ did not change the testosterone and 17β-estradiol contents in female zebrafish at the endpoint of exposure, but significantly reduced the proportion of early vitellogenic oocytes and mature oocytes. Follicle maturity retardation was accompanied by changes in transcriptional levels of the genes related to the hypothalamus-pituitary-gonad-liver (HPGL) axis. Transcriptional levels of cyp19a and lhr in the ovary were down-regulated, while the transcriptional level of fshr in the ovaries was up-regulated. In the 21-day cumulative spawning experiment, Na₂SeO₃ (25.14 ± 0.15 and 79.60 ± 0.81 μg Se/L) caused fewer eggs to be produced. Additionally, the malformation of zebrafish offspring significantly increased in the group exposed to 79.60 ± 0.81 μg Se/L. In conclusion, for the first time, this study shows that life-cycle exposure to environmentally relevant concentrations of waterborne Na₂SeO₃ significantly delays ovarian maturation and reduces the fertility of the female zebrafish.
显示更多 [+] 显示较少 [-]Estimations of benchmark dose for urinary metabolites of coke oven emissions among workers 全文
2021
Zou, Kaili | Wang, Sihua | Wang, Pengpeng | Duan, Xiaoran | Yang, Yongli | Yazdi, Mahdieh Danesh | Stowell, Jennifer | Wang, Yanbin | Yao, Wu | Wang, Wei
Coke oven emissions (COEs), usually composed of polycyclic aromatic hydrocarbons (PAHs) and so on, may alter the relative telomere length of exposed workers and have been linked with adverse health events. However, the relevant biological exposure limits of COEs exposure has not been evaluated from telomere damage. The purpose of this study is to estimate benchmark dose (BMD) of urinary PAHs metabolites from COEs exposure based on telomere damage with RTL as a biomarker. A total of 544 exposed workers and 238 controls were recruited for participation. High-performance liquid chromatography and qPCR were used to detect concentrations of urinary mono-hydroxylated PAHs and relative telomere length in peripheral blood leukocytes for all subjects. The benchmark dose approach was used to estimate benchmark dose (BMD) and its lower 95% confidence limit (BMDL) of urinary OH-PAHs of COEs exposure based on telomere damage. Our results showed that telomere length in the exposure group (0.75 (0.51, 1.08)) was shorter than that in the control group (1.05 (0.76,1.44))(P < 0.05), and a dose-response relationship was shown between telomere damage and both 1-hydroxypyrene and 3-hydroxyphenanthrene in urine. The BMDL of urinary 1-hydroxypyrene from the optimal model for telomere damage was 1.96, 0.40, and 1.01 (μmol/mol creatinine) for the total, males, and females group, respectively. For 3-hydroxyphenanthrene, the BMDL was 0.94, 0.33, and 0.49 (μmol/mol creatinine) for the total, males, and females. These results contribute to our understanding of telomere damage induced by COEs exposure and provide a reference for setting potential biological exposure limits.
显示更多 [+] 显示较少 [-]Cd bioavailability and nitrogen cycling microbes interaction affected by mixed amendments under paddy-pak choi continued planting 全文
2021
Li, Houfu | Abbas, Touqeer | Cai, Mei | Zhang, Qichun | Wang, Jingwen | Li, Yong | Di, Hongjie | Ṭāhir, Muḥammad
Cadmium (Cd) is the most concerning soil pollutant, and a threat to human health, especially in China. The in-situ immobilization of Cadmium by amendments is one of the most widely adopted methods to remedy soil contamination. The study was designed to evaluate the effect of organo-chemical amendments on soil Cd bioavailability and nitrogen cycling microbes under continuous planting of rice (Oryza sativa) and pak choi (Brassica chinensis L.). The experiment was carried out using four amendments, Lime, Zeolite, Superphosphate, and Biochar, at two different ratios; M1: at the ratio of 47:47:5:1, and M2 at the ratio of 71:23:5:1, respectively. Moreover, both M1 and M2 were enriched at four levels (T1: 0.5%; T2: 1%; T3: 2%; T4: 4%). Results showed that compared with CK (Cd enriched soils), the yield of rice under treatments of M1T1 and M2T1 increased by 8.93% and 8.36%, respectively. While the biomass (fresh weight) of pak choi under M1 and M2 amendments increased by 2.52–2.98 times and 0.76–2.89 times respectively, under enrichment treatments T1, T2, and T3. The total Cd concentrations in rice grains treated with M1T3 and M2T3 decreased by 89.25% and 93.16%, respectively, compared with CK. On the other hand, the total Cd concentrations in pak choi under M1T3 and M2T2 decreased by 92.86% and 90.23%, respectively. The results showed that soil pH was the main factor affecting Cd bioavailability in rice and pak choi. The Variance partitioning analysis (VPA) of rice and pak choi showed that soil pH was the most significant contributing factor. In the rice season, the contribution of soil pH (P) on Cd bioavailability was 10.14% (P = 0.102), and in the pak choi season, the contribution of soil pH was 8.38% (P = 0.133). Furthermore, the abundance of ammonia oxidation and denitrifying microorganisms had significantly correlation with soil pH and exchange Cd. In rice season, when the enrichment level of amendments increased from 0.5% (T1) to 2% (T3), the gene abundance of AOA, AOB, nirK, nirS and nosZ (І) tended to decrease. While in pak choi season, when the enrichment level increased at the level of 0.5% (T1), 1% (T2), and 2% (T3), the gene abundance of AOB, nirS, and nosZ (І) increased. Additionally, the gene abundance of AOA and nirK showed a reduction in the pak choi season contrasting to rice. And the mixed amendment M2 performed better at reducing Cd uptake than M1, which may have correlation with the ratio of lime and zeolite in them. Finally, we conclude that between these two amendments, when applied at a moderate level M2 type performed better than M1 in reducing Cd uptake, and also showed positive effects on both gene abundance and increase soil pH.
显示更多 [+] 显示较少 [-]Hydrolyzed polyacrylamide-containing wastewater treatment using ozone reactor-upflow anaerobic sludge blanket reactor-aerobic biofilm reactor multistage treatment system 全文
2021
Song, Tianwen | Li, Shanshan | Yin, Zichao | Bao, Mutai | Lu, Jinren | Li, Yang
Polymer flooding is one of the most important enhanced oil recovery techniques. However, a large amount of hydrolyzed polyacrylamide (HPAM)-containing wastewater is produced in the process of polymer flooding, and this poses a potential threat to the environment. In this study, the treatment of HPAM-containing wastewater was analyzed in an ozonic-anaerobic-aerobic multistage treatment process involving an ozone reactor (OR), an upflow anaerobic sludge blanket reactor (UASBR), and an aerobic biofilm reactor (ABR). At an HPAM concentration of 500 mg L⁻¹ and an ozone dose of 25 g O₃/g TOC, the HPAM removal rate reached 85.06%. With fracturing of the carbon chain, high-molecular-weight HPAM was degraded into low-molecular-weight compounds. Microbial communities in bioreactors were investigated via high-throughput sequencing, which revealed that norank_c_Bacteroidetes_vadinHA17, norank_f_Cytophagaceae, and Meiothermus were the dominant bacterial groups, and that Methanobacterium, norank_c_WCHA1-57, and Methanosaeta were the key archaeal genera. To the best of our knowledge, this is the first study in which HPAM-containing wastewater is treated using an ozonic-anaerobic-aerobic multistage treatment system. The ideal degradation performance and the presence of keystone microorganisms confirmed that the multistage treatment process is feasible for treatment of HPAM-containing wastewater.
显示更多 [+] 显示较少 [-]Source apportionment and human health risk assessment of trace metals and metalloids in surface soils of the Mugan Plain, the Republic of Azerbaijan 全文
2021
Han, Junho | Lee, Seoyeon | Mămmădov, Zaman | Kim, Minhee | Mammadov, Garib | Ro, Hee-Myong
The Mugan Plain is the most productive area in the Republic of Azerbaijan, but a previous study confirmed trace metal and metalloid (TM&M) contamination with Cr, Ni and Pb, and the potential ecological risk of As was estimated. However, no industrial activity was previously reported in this area; thus, a source apportionment model using positive matrix factorization (PMF) was employed to identify pollution sources, and a human health risk assessment was conducted to evaluate noncarcinogenic and carcinogenic risks. Surface soil samples were collected from 349 sites, and six major elements (Si, Ca, Cl, P, S and Sr) and 8 TM&Ms (As, Cd, Cr, Co, Cu, Ni, Pb and Zn) were analyzed by X-ray fluorescence and employed for further apportionment and risk assessment. As a result, the PMF model showed 7 factors, assigned to natural activity (12.9%), dry riverbed (13.6%), surface accumulation (3.1%), desalinization activity (3.2%), residential activity (12.3%), fossil fuel combustion (35.5%) and agricultural activity (19.3%). The PMF model characterized certain areas with desalinization activity in the previous Soviet period and with surface accumulation of salt, and these findings were confirmed by additional field surveys and historical Landsat satellite images. The risk assessment results showed that there was no risk for the adults, while for children, there was a noncarcinogenic risk, but no carcinogenic risk. Dermal contact was estimated to be the primary pathway, and Ni and As were identified as the most problematic TM&Ms for noncarcinogenic and carcinogenic risks, respectively. According to the results, fossil fuel combustion associated with heating and vehicle transportation was estimated to be the main source of pollution, contributing 42.6% of the noncarcinogenic and 48.0% of the carcinogenic risks. These results can provide scientific guidance to understand and prevent the risk of TM&Ms on the Mugan Plain.
显示更多 [+] 显示较少 [-]Co-oxidative removal of arsenite and tetracycline based on a heterogeneous Fenton-like reaction using iron nanoparticles-impregnated biochar 全文
2021
Fu, Dun | Kurniawan, Tonni Agustiono | Li, Heng | Wang, Haitao | Wang, Yuanpeng | Li, Qingbiao
A highly efficient, eco-friendly and relatively low-cost catalyst is necessary to tackle bottlenecks in the treatment of industrial wastewater laden with heavy metals and antibiotic such as livestock farm and biogas liquids. This study investigated co-oxidative removal of arsenite (As(III)) and tetracycline (TC) by iron nanoparticles (Fe NP)-impregnated carbons based on heterogeneous Fenton-like reactions. The composites included Fe NP@biochar (BC), Fe NP@hydrochar (HC), and Fe NP@HC-derived pyrolysis char (HDPC). The functions of N and S atoms and the loading mass of the Fe NP in the Fe NP@BC in heterogeneous Fenton-like reactions were studied. To sustain its cost-effectiveness, the spent Fe NP@BC was regenerated using NaOH. Among the composites, the Fe NP@BC achieved an almost complete removal of As(III) and TC under optimized conditions (1.0 g/L of dose; 10 mM H₂O₂; pH 6; 4 h of reaction; As(III): 50 μM; TC: 50 μM). The co-oxidative removal of As(III) and TC by the Fe NP@ BC was controlled by the synergistic interactions between the Fe NPs and the active N and S sites of the BC for generating reactive oxygen species (ROS). After four consecutive regeneration cycles, about 61 and 95% of As(III) and TC removal were attained. This implies that the spent carbocatalyst still has reasonable catalytic activities for reuse. Overall, this suggests that adding technological values to unused biochar as a carbocatalyst like Fe NP@BC was promising for co-oxidative removal of As(III) and TC from contaminated water.
显示更多 [+] 显示较少 [-]Contribution of anthropogenic and natural sources in PM10 during North African dust events in Southern Europe 全文
2021
Millán-Martínez, María | Sánchez-Rodas, Daniel | Sánchez de la Campa, Ana M. | Rosa, Jesús de la
The influence of North African (NAF) dust events on the air quality at the regional level (12 representative monitoring stations) in Southern Europe during a long time series (2007–2014) was studied. PM10 levels and chemical composition were separated by Atlantic (ATL) and NAF air masses. An increase in the average PM10 concentrations was observed on sampling days with NAF dust influence (42 μg m⁻³) when compared to ATL air masses (29 μg m⁻³). Major compounds such as crustal components and secondary inorganic compounds (SIC), as well as toxic trace elements derived from industrial emissions, also showed higher concentrations of NAF events. A source contribution analysis using positive matrix factorisation (PMF) 5.0 of the PM10 chemical data, discriminating ATL and NAF air mass origins, allowed the identification of five sources: crustal, sea salt, traffic, regional, and industrial. A higher contribution (74%) of the natural sources to PM10 concentrations was confirmed under NAF episodes compared with ATL. Furthermore, there was an increase in anthropogenic sources during these events (51%), indicating the important influence of the NAF air masses on these sources. The results of this study highlight that environmental managers should take appropriate actions to reduce local emissions during NAF events to ensure good air quality.
显示更多 [+] 显示较少 [-]Covalent bonding of aromatic amine daughter products of 2,4-dinitroanisole (DNAN) with model quinone compounds representing humus via nucleophilic addition 全文
2021
Kadoya, Warren M. | Sierra-Alvarez, Reyes | Jagadish, Bhumasamudram | Wong, Stanley | Abrell, Leif | Mash, Eugene A. | Field, Jim A.
2,4-Dinitroanisole (DNAN) is a component of insensitive munitions (IM), which are replacing traditional explosives due to their improved safety. Incomplete IM combustion releases DNAN onto the soil, where it can leach into the subsurface with rainwater, encounter anoxic conditions, and undergo (a)biotic reduction to aromatic amines 2-methoxy-5-nitroaniline (MENA), 4-methoxy-3-nitroaniline (iMENA, isomer of MENA), and 2,4-diaminoanisole (DAAN). We report here studies of nucleophilic addition mechanisms that may account for the sequestration of aromatic amine daughter products of DNAN into soil organic matter (humus), effectively removing these toxic compounds from the aqueous environment. Because quinones are important moieties in humus, we incubated MENA, iMENA, DAAN, and related analogs with model compounds 1,4-benzoquinone and 2,3-dimethyl-1,4-benzoquinone under anoxic conditions. Mass spectrometry and ultra-high performance liquid chromatography revealed that the aromatic amines had covalently bonded to either carbonyl carbons or ring carbons β to carbonyl carbons of the quinones, producing a mixture of imines and Michael adducts, respectively. These products formed rapidly and accumulated in the one-to four-day incubations. Nucleophilic addition reactions, which do not require catalysis or oxic conditions, are proposed as a mechanism resulting in the binding of DNAN to soil observed in previous studies. To remediate sites contaminated with DNAN or other nitroaromatics, reducing conditions and humus amendments may promote their immobilization into the soil matrix.
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