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Aggregation and stability of sulfate-modified polystyrene nanoplastics in synthetic and natural waters
2021
Wang, Junyu | Zhao, Xiaoli | Wu, Aiming | Tang, Zhi | Niu, Lin | Wu, Fengchang | Wang, Fanfan | Zhao, Tianhui | Fu, Zhiyou
Nanoplastics (NPs) are becoming emerging pollutants of global concern. Understanding the environmental behavior of NPs is crucial for their environmental and human risk assessment. In this study, the aggregation and stability of polystyrene (PS) NPs were investigated under different hydrochemical conditions such as pH, salt type (NaCl, CaCl₂, Na₂SO₄), ionic strength (IS), and natural organic matter (NOM). The critical coagulation concentrations of PS NPs were determined to be 158.7 mM NaCl, 12.2 mM CaCl₂, and 80.0 mM Na₂SO₄. Ca²⁺ was more effective in destabilizing PS NPs, compared to Na⁺, owing to its stronger charge screening effect. In the presence of monovalent ions, NOM reduced aggregation through steric repulsion, whereas in the case of divalent ions, NOM induced aggregation through cation bridging. Initial and long-term stability studies demonstrated that, in waters with high IS and NOM content, NOM was the most significant factor affecting NPs aggregation. PS NPs would be highly suspended in all freshwaters, and even in wastewater, whereas they would aggregate rapidly and deposit in seawater. Finally, a statistical model was established to evaluate the hydrodynamic diameter of NPs in different waters. The results indicated the stability of PS NPs in natural aquatic environments and their potential for long-term transport.
Afficher plus [+] Moins [-]Effective removal of excessive fluoride from aqueous environment using activated pods of Bauhinia variegata: Batch and dynamic analysis
2021
Jayashree, D Eunice | Kumar, P Senthil | Ngueagni, P Tsopbou | Vo, Dai-VietN. | Chew, Kit Wayne
In this study, a novel biosorbent is prepared from the pods of Bauhinia variegata is used for defluoridation of the fluoride contaminated water. It is an eco-friendly and economically feasible material. Comparison of adsorption capacity of Physically Treated Bauhinia (PTB) and Chemically Treated Bauhinia (CTB) are carried in this work. Characterization studies like SEM, EDS, FTIR, and XRD are executed to analyze surface morphology and functional groups in PTB and CTB. The experimental procedure was implemented in a batch process where the operating constraints such as dosage, pH, initial fluoride concentration, time, and temperature are varied to attain optimized efficiency. PTB and CTB yield an adsorption capacities of 10.90 mg/g and 15.45 mg/g respectively in the batch process. PTB adheres fluoride in monolayer formation whereas CTB forms multilayer adsorption. The adsorption process was described by the Pseudo first-order model to state the mechanism of physisorption. The negative values of thermodynamic parameters indicate spontaneity and favorable conditions for adsorption process. As CTB has a higher adsorption capacity than PTB, the batch study has been extended to column adsorption. Bed depth, initial fluoride concentration, and flow rate are the experimental variables used to acquire breakthrough curves. Simplified column models like Adam-Bohart, Thomas, and Yoon-Nelson models were analyzed. In column studies, Yoon-Nelson model fitted well in describing the process of adsorption. The maximum adsorption capacity acquired during the column process was found to be 1.176 mg/g with a bed depth of 5 cm and a flow rate of 5 ml/min. Thus, the innocuous and sustainable adsorbent is developed and serves as an excellent defluoridation agent.
Afficher plus [+] Moins [-]Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
2021
Liu, Na | Hu, Qing | Wang, Chao | Tong, Lizhi | Weng, Chih-Huang | Ding, Longzhen
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kₒbₛ values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
Afficher plus [+] Moins [-]A synthesis framework using machine learning and spatial bivariate analysis to identify drivers and hotspots of heavy metal pollution of agricultural soils
2021
Yang, Shiyan | Taylor, David | Yang, Dong | He, Mingjiang | Liu, Xingmei | Xu, Jianming
Source apportionment can be an effective tool in mitigating soil pollution but its efficacy is often limited by a lack of information on the factors that influence the accumulation of pollutants at a site. In response to this limitation and focusing on a suite of heavy metals identified as priorities for pollution control, the study established a comprehensive pollution control framework using factor identification coupled with spatial agglomeration for agricultural soils in an industrialized part of Zhejiang Province, China. In addition to elucidating the key role of industrial and traffic activities on heavy metal accumulation through implementing a receptor model, specific influencing factors were identified using a random forest model. The distance from the soil sample location to the nearest likely industrial source was the most important factor in determining cadmium and copper concentrations, while distance to the nearest road was more important for lead and zinc pollution. Soil parent materials, pH, organic matter, and clay particle size were the key factors influencing accumulation of arsenic, chromium, and nickel. Spatial auto-correlation between levels of soil metal pollution and industrial agglomeration can enable a more targeted approach to pollution control measures. Overall, the approach and results provide a basis for improved accuracy in source apportionment, and thus improved soil pollution control, at the regional scale.
Afficher plus [+] Moins [-]Leaching behavior of polycyclic aromatic hydrocarbons (PAHs) from oil-based residues of shale gas drill cuttings
2021
Xie, Bingxin | Qin, Jihong | Sun, Hui | Wang, Shu | Li, Xin
Cuttings are the main solid residues which are generated from drilling operations. Due to the presence of heavy and radioactive elements, the environment risk posed by cuttings has attracted increasing attention. In this work, a short-term static immersion experiment was carried out to investigate the leaching of polycyclic aromatic hydrocarbons (PAHs) from oil-based residues of shale gas drilling cuttings. Furthermore, the effects of some relevant environmental factors controlling the leaching behavior were evaluated, including the different particle sizes, pH, extraction time, solid-to-liquid (S/L) ratio and dissolved organic matter (DOM) concentration. The results showed that (1) the concentrations of leached PAHs gradually increased with prolonged leaching time, but the cumulative amount of PAHs released during leaching was less than 3% of the total. (2) The Elovich, parabolic diffusion and power function models were found to fit the experimental data better than the first-order kinetic equation, indicating that the leaching of PAHs was controlled by the coupling of diffusion and chemical reactions at the source surface. (3) Different environmental factors had different impacts on the leaching of PAHs: the shaking time and presence of DOM increased leachability, the particle size and S/L ratio decreased leachability, and the pH did not affect the leachability of PAHs. Therefore, PAHs leaching was a complex process, and it is of scientific and environmental interest to conduct the leaching tests under the simulated environmental conditions.
Afficher plus [+] Moins [-]Preparation of biochar-interpenetrated iron-alginate hydrogel as a pH-independent sorbent for removal of Cr(VI) and Pb(II)
2021
Zhao, Chenhao | Hu, Linlin | Zhang, Changai | Wang, Shengsen | Wang, Xiaozhi | Huo, Zhongyang
Herein, a pH-independent interpenetrating polymeric networks (Fe-SA-C) were fabricated from graphitic biochar (BC) and iron-alginate hydrogel (Fe-SA) for removal of Cr(VI) and Pb(II) in aqueous solution. Fourier transform infrared spectroscopy (FTIR), Raman spectroscopy and scanning electron microscope (SEM) results demonstrated that graphitic BC interpenetration increased surface porosity and distorted surfaces of Fe-SA, which boosted availability of hydroxyl (-OH) group. Fe³⁺ as a cross-linking agent of the alginate endowed Fe-SA-C with positive surfaces (positive zeta potential) and excellent pH buffering capacity, while excessive Fe³⁺ was soldered on Fe-SA-C matrix as FeO(OH) and Fe₂O₃. Cr(VI) removal at pH of 3 by Fe-SA-C (20.3 mg g⁻¹) were 30.3% and 410.6% greater than that by Fe-SA and BC, respectively. Fe-SA-C exhibited minor pH dependence over pH range of 2–7 towards Cr(VI) retention. Greater zeta potential of Fe-SA-C over Fe-SA conferred a better electrostatic attraction with Cr(VI). FTIR and XPS of spent sorbents confirmed the reduction accounted for 98.5% for Cr(VI) removal mainly due to participation of –OH. Cr(VI) reduction was further favored by conductive carbon matrix in Fe-SA-C, as evidenced by more negative Tafel corrosion potential. Reductively formed Cr(III) was subsequently complexed with carboxylic groups originating from oxidation of –OH. Thus, Cr(VI) removal invoked electrostatic attraction, reduction, and surface complexation mechanisms. Pb(II) removal with excellent pH independence was mainly ascribed to surface complexation and possible precipitation. Thus, the functionalized, conductive, and positively-charged Fe-SA-C extended its applicability for Cr(VI) and Pb(II) removal from aqueous solutions in a wide pH range. This research could expand the application of hydrogel materials for removal of both cationic and anionic heavy metals in solutions over an extended pH range.
Afficher plus [+] Moins [-]Deposition and mobilization of viruses in unsaturated porous media: Roles of different interfaces and straining
2021
Zhang, Wenjing | Wu, Shengyu | Qin, Yunqi | Li, Shuo | Lei, Liancheng | Sun, Simiao | Yang, Yuesuo
The vadose zone is the first natural layer preventing groundwater pollution. Understanding virus transport and retention in the vadose zone is necessary. The effects of different interfaces and mechanisms on virus transport and retention were investigated by studying Escherichia coli phage migration in laboratory-scale columns under unsaturated conditions. The E. coli phage was used as a model virus. Colloid filtration theory, extended Derjagin–Landau–Verwey–Overbeek theory and two−site kinetic deposition model were used to calculate fitted parameters and interaction energies to assess virus retention at different interfaces. The collector diameters and the size of E. coli phages in the influent and effluent were compared to assess the effect of straining. The results indicated that the roles of solid–water interfaces (SWIs) and air–water interfaces (AWIs) in retaining E. coli phages are strongly controlled by the moisture content and hydrochemical conditions. Decreasing the moisture content and increasing the ionic strength (IS) of the suspension increased E. coli phage retention. At suspension ISs of 0.01 or 0.03 M and various moisture contents, E. coli phages were mainly retained at the SWIs rather than AWIs. When the IS was increased to 0.06 M, the viruses were strongly retained by becoming attached to both SWIs and AWIs. The role of straining in virus retention could not be ignored. Viruses were retained more at the SWIs and less straining occurred under acidic conditions than under neutral or alkaline conditions. This was mainly because of the effects of the pH and IS on surface charges and the model virus particle size. This study has important implications for modeling and predicting virus transport in soil affected by rainfall, snowmelt, and human activities (e.g., irrigation and artificial groundwater recharging).
Afficher plus [+] Moins [-]Cross-linked sulfydryl-functionalized graphene oxide as ultra-high capacity adsorbent for high selectivity and ppb level removal of mercury from water under wide pH range
2021
Bao, Shuangyou | Wang, Yingjun | Yu, Yongsheng | Yang, Weiwei | Sun, Yinyong
It is highly desirable but remains extremely challenging to develop a facile strategy to prepare adsorbent for dealing with heavy metal pollution in water. Here, we report a facile approach for preparing sulfydryl-functionalized graphene oxide (S-GO) by cross-linking method with an unprecedented adsorption capacity and ultrahigh selectivity for efficient Hg(II) removal. The adsorbents exhibit a prominent performance in capturing Hg(II) from wastewater with a record-high adsorption capacity of 3490 mg/g and rapid kinetics to reduce Hg(II) contaminants below the discharge standard of drinking water (2 ppb) within 60 min under a wide pH range even in the coexistent of other interfering metal ions. In addition, the adsorbents can be also easily recycled and reused multiple times with no apparent decline in removal efficiency. Considering the broad diversity, we developed also a magnetic Fe₃O₄/S-GO adsorbent by a simple chemical cross-linking reaction to achieve rapid separation of S-GO from their aqueous solution. In addition, the adsorbents were successfully applied in dealing with the practical industrial wastewater. The results indicate the potential of rationally designed sulfydryl-functionalized graphene oxide for high performance Hg(II) removal.
Afficher plus [+] Moins [-]Mercury vertical and horizontal concentrations in agricultural soils of a historically contaminated site: Role of soil properties, chemical loading, and cultivated plant species in driving its mobility
2021
Morosini, Cristiana | Terzaghi, Elisa | Raspa, Giuseppe | Zanardini, Elisabetta | Anelli, Simone | Armiraglio, Stefano | Petranich, Elisa | Covelli, Stefano | Di Guardo, Antonio
The long term vertical and horizontal mobility of mercury (Hg) in soils of agricultural areas of a historically contaminated Italian National Relevance Site (SIN Brescia-Caffaro) was investigated. The contamination resulted from the continuous discharge of Hg in irrigation waters by an industrial plant (Caffaro S.p.A), equipped with a mercury-cell chlor-alkali process. The contamination levels with depth ranged from about 20 mg/kg dry weight (d.w.) of soil in the top (plow) layer to less than 0.1 mg/kg d.w. at 1 m depth. The concentrations varied also spatially, up to one order of magnitude within the same field and showing a decreasing trend from the Hg source (i.e., irrigation ditches). The concentration profiles and gradients measured were explained considering Hg loading, soil properties, such as the texture, organic carbon content, pH and cation exchange capacity. A Selective Sequential Extraction (SSE) was also applied on soil samples from an ad hoc greenhouse experiment to investigate the role of different plant species in influencing Hg speciation in soils. Although most of the extracted Hg was included in scarcely mobile or immobile forms, some plant species (i.e., alfalfa) showed to importantly increase the soluble and exchangeable fractions with respect to the unplanted control soils, thus affecting mobility and potential bioavailability of Hg.
Afficher plus [+] Moins [-]Distance dilution of antibiotic resistance genes of sediments in an estuary system in relation to coastal cities
2021
Lu, Xiao-Ming | Peng, Xin | Xue, Feng | Qin, Song | Ye, Shen | Dai, Li-Bo
Coastal tourist and industrial cities are most likely to have differential effects on the distance dilution of antibiotic resistance genes (ARGs) in an estuary system. This study used high-throughput fluorescence quantitative polymerase chain reaction to identify sediment ARGs in two typical estuaries of coastal tourist and industrial cities (Xiamen and Taizhou) in China. The distance dilution of ARGs and its relationship with key environmental factors were analysed. The results indicated that along the river inlet towards the sea, the distance dilution effect on ARG abundance in estuary sediments of Taizhou was approximately double that in Xiamen, and the macrolide, lincosamide, and streptogramin B (MLSB) and vancomycin genes were replaced by the fluoroquinolone, quinolone, florfenicol, chloramphenicol, and amphenicol (FCA) and β-lactam genes in Taizhou, whereas β-lactam genes succeeded the MLSB and sul genes in Xiamen. The abundance and number of ARGs and mobile genetic elements (MGEs) were positively correlated with the particle size and total organic carbon (TOC) contents of sediments, whereas they were negatively associated with the oxidation and reduction potential (Eₕ) and pH of sediments, as well as the seawater salinity. The sediment particle size (SPZ) was the dominant physicochemical factor affecting the abundance of ARGs (r = 0.826, p < 0.05) and MGEs (r = 0.850, p < 0.01). These findings suggest that although the distance dilution effect on the ARG abundance of estuary sediments of the industrial city is greater than that of the tourist city, the larger SPZ, higher TOC content, and lower salinity, pH, and Eₕ in estuary regions adjacent to the industrial city can more significantly facilitate the proliferation and propagation of ARGs in the sediments.
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