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Evaluating the influence of constant source profile presumption on PMF analysis of PM2.5 by comparing long- and short-term hourly observation-based modeling
2022
Xie, Mingjie | Lu, Xinyu | Ding, Feng | Cui, Wangnan | Zhang, Yuanyuan | Feng, Wei
Hourly PM₂.₅ speciation data have been widely used as an input of positive matrix factorization (PMF) model to apportion PM₂.₅ components to specific source-related factors. However, the influence of constant source profile presumption during the observation period is less investigated. In the current work, hourly concentrations of PM₂.₅ water-soluble inorganic ions, bulk organic and elemental carbon, and elements were obtained at an urban site in Nanjing, China from 2017 to 2020. PMF analysis based on observation data during specific pollution (firework combustion, sandstorm, and winter haze) and emission-reduction (COVID-19 pandemic) periods was compared with that using the whole 4-year data set (PMFwₕₒₗₑ). Due to the lack of data variability, event-based PMF solutions did not separate secondary sulfate and nitrate. But they showed better performance in simulating average concentrations and temporal variations of input species, particularly for primary source markers, than the PMFwₕₒₗₑ solution. After removing event data, PMF modeling was conducted for individual months (PMFₘₒₙₜₕ) and the 4-year period (PMF₄₋yₑₐᵣ), respectively. PMFₘₒₙₜₕ solutions reflected varied source profiles and contributions and reproduced monthly variations of input species better than the PMF₄₋yₑₐᵣ solution, but failed to capture seasonal patterns of secondary salts. Additionally, four winter pollution days were selected for hour-by-hour PMF simulations, and three sample sizes (500, 1000, and 2000) were tested using a moving window method. The results showed that using short-term observation data performed better in reflecting immediate changes in primary sources, which will benefit future air quality control when primary PM emissions begin to increase.
Afficher plus [+] Moins [-]Sulfur(IV) assisted oxidative removal of organic pollutants from source water
2022
Truzsi, Alexandra | Elek, János | Fábián, István
The removal of organic pollutants presents a major challenge for drinking water treatment plants. The chemical oxygen demand (COD) is essentially the measure of oxidizable organic matter in source waters. In this study, we report that COD can efficiently be decreased by adding Fe(II)/Fe(III) and sulfite ion to the source water while purging it with air. In this process, oxygen is activated to oxidize the main constituents of COD, i.e. organic substrates, via the generation of reactive inorganic oxysulfur radical ions. In the end, the total amount of sulfur(IV) is converted to the non-toxic sulfate ion. It has been explored how the COD removal efficiency depends on the concentration of S(IV), the total concentration of iron species, the concentration ratio of Fe(II) and Fe(III), the purging rate and the contact time by using source water from a specific location (Királyhegyes, Hungary). The process has been optimized by applying the Response Surface Methodology (RSM). Under optimum conditions, the predicted and experimentally found COD removal efficiencies are in excellent agreement: 85.4% and 87.5%, respectively. The robustness of the process was tested by varying the optimum values of the parameters by ± 20%. It was demonstrated that the method is universally applicable because a remarkable decrease was achieved in COD, 62.0–88.5%, with source waters of various compositions acquired from 9 wells at other locations using the same conditions as in the case of Királyhegyes.
Afficher plus [+] Moins [-]Elevated particle acidity enhanced the sulfate formation during the COVID-19 pandemic in Zhengzhou, China
2022
Yang, Jieru | Wang, Shenbo | Zhang, Ruiqin | Yin, Shasha
The significant reduction in PM₂.₅ mass concentration after the outbreak of COVID-19 provided a unique opportunity further to study the formation mechanism of secondary inorganic aerosols. Hourly data of chemical components in PM₂.₅, gaseous pollutants, and meteorological data were obtained from January 1 to 23, 2020 (pre-lockdown) and January 24 to February 17, 2020 (COVID-lockdown) in Zhengzhou, China. Sulfate, nitrate, and ammonium were the main components of PM₂.₅ during both the pre-lockdown and COVID-lockdown periods. Compared with the pre-lockdown period, even though the concentration and proportion of nitrate decreased, nitrate was the dominant component in PM₂.₅ during the COVID-lockdown period. Moreover, nitrate production was enhanced by the elevated O₃ concentration, which was favorable for the homogeneous and hydrolysis nitrate formation despite the drastic decrease of NO₂. The proportion of sulfate during the COVID-lockdown period was higher than that before. Aqueous-phase reactions of H₂O₂ and transition metal (TMI) catalyzed oxidations were the major pathways for sulfate formation. During the COVID-lockdown period, TMI-catalyzed oxidation became the dominant pathway for aqueous-phase sulfate formation because the elevated acidity favored the dissolution of TMI. Therefore, the enhanced TMI-catalyzed oxidation affected by the elevated particle acidity dominated the sulfate formation, resulting in the slight increase of sulfate concentration during the COVID-lockdown period in Zhengzhou.
Afficher plus [+] Moins [-]Sediment spiking and equilibration procedures to achieve partitioning of uranium similar to contamination in tropical wetlands near a mine site
2022
Harford, Andrew J. | Simpson, Stuart L. | Humphrey, Christopher L. | Parry, David L. | Kumar, Anu | Chandler, Lisa | Stauber, Jennifer L. | van Dam, Rick A.
The derivation of sediment quality guideline values (SQGVs) presents significant challenges. Arguably the most important challenge is to conduct toxicity tests using contaminated sediments with physico-chemistry that represents real-world scenarios. We used a novel metal spiking method for an experiment that ultimately aims to derive a uranium SQGV. Two pilot studies were conducted to inform the final spiking design, i.e. percolating a uranyl sulfate solution through natural wetland sediments. An initial pilot study that used extended mixing equilibration phases produced hardened sediments not representative of natural sediments. A subsequent percolation method produced sediment with similar texture to natural sediment and was used as the method for spiking the sediments. The range of total recoverable uranium (TR-U) concentrations achieved was 8–3200 mg/kg. This reflected the concentrations found in natural wetlands and water management ponds found on a uranium mine site and was above natural levels. Dilute-acid extractable uranium (AE-U) concentrations were >80% of total concentrations, indicating that much of the uranium in the spiked sediment was labile and potentially bioavailable. The portion of TR-U extractable as AE-U was similar at the start and end of the 4.5-month field-deployment. Porewater uranium (PW–U) analyses indicated that partition coefficients (Kd) were 2000–20,000 L/kg, and PW-U was greater in post- than pre-field-deployed samples when TR-U was ≤1500 mg/kg, indicating the binding became weaker during the field-deployment period. At higher spiked-U concentrations, the PW-U was lower post-field-deployment. Comparing the physico-chemical data of the spiked sediments with environmental monitoring data from sediments in the vicinity of a uranium mining operation indicated that they were representative of sediments contaminated by mining and that the U-spiked sediments had a clear U concentration gradient. This confirmed the suitability of the spiking procedure for preparing sediments that were suitable for deriving a SQGV for uranium.
Afficher plus [+] Moins [-]Comprehensive investigation of persistent and mobile chemicals and per- and polyfluoroalkyl substances in urine of flemish adolescents using a suspect screening approach
2022
Kim, Da-Hye | Jeong, Yunsun | Belova, Lidia | Roggeman, Maarten | Fernández, Sandra F. | Poma, Giulia | Rémy, Sylvie | Verheyen, Veerle J. | Schoeters, Greet | van Nuijs, Alexander L.N. | Covaci, Adrian
Persistent and mobile chemicals (PMs) and per- and polyfluoroalkyl substances (PFAS) are groups of chemicals that have received recent global attention due to their potential health effects on the environment and humans. In this study, exposure to a broad range of PMs and PFAS was investigated in Flemish adolescents’ urine samples (n = 83) using a suspect screening approach. For this purpose, three sample preparation methods were evaluated, and a basic liquid-liquid extraction was optimized for urine analysis based on the extraction efficiency of PMs (53–80%) and PFAS (>70%). In total, 9 PMs were identified in urine samples at confidence levels (CL) 1–3 and, among them, acetaminophen, 4-aminophenol, 2,2,6,6-tetramethyl-4-piperidone, trifluoroacetic acid (TFAA), sulisobenzone, ethyl sulfate, and 1,2-benzisothiazol-3(2H)-one 1,1-dioxide were confirmed at CL 1 and 2. In addition, the detection and identification of 2,2,6,6-tetramethyl-4-piperidone, 4-aminophenol, TFAA, and m-(2,3-epoxypropoxy)-N,N-bis(2,3-epoxypropyl) aniline (CL 3), has been reported for the first time in human urine in this study. For PFAS, only 2 compounds were identified at CL 4, implying that urine is not a suitable matrix for suspect screening of such compounds. A significant difference between sexes was observed in the detection rate of identified PMs, in particular for acetaminophen, 4-aminophenol, and sulisobenzone. The findings of this study can be used in future human biomonitoring programs, such as by including the newly identified compounds in quantitative methods or monitoring in other human matrices (e.g., serum).
Afficher plus [+] Moins [-]Effect of zinc and iron oxide nanoparticles on plant physiology, seed quality and microbial community structure in a rice-soil-microbial ecosystem
2022
Afzal, Shadma | Singh, Nand K.
In this study, we assessed the impact of zinc oxide (ZnO) and iron oxide (FeO) (<36 nm) nanoparticles (NPs) as well as their sulphate salt (bulk) counterpart (0, 25, 100 mg/kg) on rice growth and seed quality as well as the microbial community in the rhizosphere environment of rice. During the rice growing season 2021–22, all experiments were conducted in a greenhouse (temperature: day 30 °C; night 20 °C; relative humidity: 70%; light period: 16 h/8 h, day/night) in rice field soil. Results showed that low concentrations of FeO and ZnO NPs (25 mg/kg) promoted rice growth (height (29%, 16%), pigment content (2%, 3%)) and grain quality parameters such as grains per spike (8%, 9%), dry weight of grains (12%, 14%) respectively. As compared to the control group, the Zn (2%) and Fe (5%) accumulations at their respective low concentrations of NP treatments showed stimulation. Interestingly, our results showed that at low concentration of both the NPs the soil microbes had more diversity and richness than those in the bulk treated and control soil group. Although a number of phyla were affected by the presence of NPs, the strongest effects were observed for change in the abundance of the three phyla for Proteobacteria, Actinobacteria, and Planctomycetes. The rhizosphere environment was notably enriched with potential streptomycin producers, carbon and nitrogen fixers, and lignin degraders with regard to functional groups of microorganisms. However, microbial communities mainly responsible for chitin degradation, ammonia oxidation, and nitrite reduction were found to be decreased. The results from this study highlight significant changes in several plant-based endpoints, as well as the rhizosphere soil microorganisms. It further adds information to our understanding of the nanoscale-specific impacts of important micronutrient oxides on both rice and its associated soil microbiome.
Afficher plus [+] Moins [-]Catchment-scale microbial sulfate reduction (MSR) of acid mine drainage (AMD) revealed by sulfur isotopes
2022
Fischer, Sandra | Jarsjö, Jerker | Rosqvist, Gunhild | Mörth, Carl-Magnus
Laboratory experiments and point observations, for instance in wetlands, have shown evidence that microbial sulfate reduction (MSR) can lower sulfate and toxic metal concentrations in acid mine drainage (AMD). We here hypothesize that MSR can impact the fate of AMD in entire catchments. To test this, we developed a sulfur isotope fractionation and mass-balance method, and applied it at multiple locations in the catchment of an abandoned copper mine (Nautanen, northern Sweden). Results showed that MSR caused considerable, catchment-scale immobilization of sulfur corresponding to a retention of 27 ± 15% under unfrozen conditions in the summer season, with local values ranging between 13 ± 10% and 53 ± 18%. Present evidence of extensive MSR in Nautanen, together with previous evidence of local MSR occurring under many different conditions, suggest that field-scale MSR is most likely important also at other AMD sites, where retention of AMD may be enhanced through nature-based solutions. More generally, the developed isotope fractionation analysis scheme provides a relatively simple tool for quantification of spatio-temporal trends in MSR, answering to the emerging need of pollution control from cumulative anthropogenic pressures in the landscape, where strategies taking advantage of MSR can provide viable options.
Afficher plus [+] Moins [-]Morphological and chemical classification of fine particles over the Yellow Sea during spring, 2015–2018
2022
Kwak, Nohhyeon | Lee, Haebum | Maeng, Hyunok | Seo, Arom | Lee, Kwangyul | Kim, Seojeong | Lee, Meehye | Cha, Joo Wan | Shin, Beomcheol | Park, Kihong
Airborne fine particles can affect climate change and human health; moreover, they can be transported over significant distances. However, studies on characteristics of individual particles and their morphology, elemental composition, aging processes, and spatial distribution after long-range transport over the Yellow Sea are limited. Therefore, in this study, we conducted shipborne measurements of fine particulate matter of less than 2.5 μm in diameter (PM₂.₅) over the Yellow Sea and classified the individual particles into seven types based on their morphology and composition. Overall, the percentage of organic-rich particles was the highest, followed by that of sea spray, sulfur-rich, dust, metals, fly ash, soot, and other particles. Near Shandong, China, the percentage of fly ash and sulfur-rich particles increased, while an increased percentage of only sulfur-rich particles was observed near the Korean Peninsula. In the open sea, the PM₂.₅ concentrations were the lowest, and sea spray particles predominated. During the cruises, three types (Types 1, 2, and 3) of events with substantially increased PM₂.₅ concentrations occurred, each with different dominant particles. Type 1 events frequently featured air masses from northern China and Mongolia with high wind speeds and increased dust particles. Type 2 events involved air masses from China with high wind speeds; fly ash, soot, organic-rich particles, and the sulfate percentage in PM₂.₅ increased. Type 3 events displayed stagnant conditions and local transport (from Korea); soot, dust particles, and the secondary sulfate and nitrate percentages in PM₂.₅ increased. Thus, different types of transport affected concentrations and dominant types of fine particles over the Yellow Sea during spring.
Afficher plus [+] Moins [-]Strategies for improving the catalytic activity of metal-organic frameworks and derivatives in SR-AOPs: Facing emerging environmental pollutants
2022
Jiang, Danni | Fang, Di | Zhou, Yu | Wang, Zhiwei | Yang, Zihao | Zhu, Jian | Liu, Zhiming
As persulfate activator, Metal organic frameworks (MOFs) and derivatives are widely concerned in degradation of emerging environmental pollutants by advanced oxygen technology dominated by sulfate radical (▪) (SR-AOPs). However, the poor stability and low catalytic efficiency limit the performance of MOFs, requiring multiple strategies to further enhance their catalytic activity. The aim of this paper is to improve the catalytic activity of MOFs and their derivatives by physical and chemical enhancement strategies. Physical enhancement strategies mainly refer to the activation strategies including thermal activation, microwave activation and photoactivation. However, the physical enhancement strategies need energy consumption and require high stability of MOFs. As a substitute, chemical enhancement strategies are more widely used and represented by optimization, modification, composites and derivatives. In addition, the identification of reactive oxygen species, active site and electron distribution are important for distinguishing radical and non-radical pathways. Finally, as a new wastewater treatment technology exploration of unknown areas in SR-AOPs could better promote the technology development.
Afficher plus [+] Moins [-]Toxicity and fate of chiral insecticide pyriproxyfen and its metabolites in zebrafish (Danio rerio)
2021
Wei, Yimu | Cui, Jingna | Zhai, Wangjing | Liu, Xueke | Zhou, Zhiqiang | Wang, Peng | Liu, Donghui
Pyriproxyfen is a juvenile hormone analogue insecticide used worldwide. At present, the potential threat of pyriproxyfen to aquatic organism has not been well explored. In this work, the bioaccumulation, metabolic profile and toxicity of pyriproxyfen and its metabolites to zebrafish were studied, and the enantioselectivity of pyriproxyfen and the major chiral metabolites were also determined. Sixteen metabolites of pyriproxyfen in zebrafish were identified. Hydroxylation, ether linkage cleavage and oxidation in phase I metabolism, followed by sulfate and glucuronic acid conjugation. The bioconcentration factors ranged from 1175 to 1246. Hydroxylation metabolites of pyriproxyfen showed enantioselective behavior in zebrafish with enantiomer fractions (EFs) of 4′–OH– pyriproxyfen and 5″–OH– pyriproxyfen ranged from 0.50 to 0.71. Toxicological indexes including acute toxicity, joint toxicity and oxidative stress were tested. Among all the metabolites, 4′–OH– pyriproxyfen was found 2 folds more toxic to zebrafish than pyriproxyfen. (−)-Pyriproxyfen was found 2 folds more toxic than rac- and (+)-pyriproxyfen. Antagonistic effects were found in binary joint toxicity of pyriproxyfen and its hydroxylated metabolites. Pyriproxyfen and its metabolites also showed oxidative stress damage by inhibiting the activity of CAT and SOD and increasing MDA. This work provided deep insight into the metabolism and the potential risks of pyriproxyfen to aquatic organisms.
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