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Transport behavior of micro polyethylene particles in saturated quartz sand: Impacts of input concentration and physicochemical factors
2020
Hou, Jun | Xu, Xiaoya | Lan, Lin | Miao, Lingzhan | Xu, Yi | You, Guoxiang | Liu, Zhilin
The long-term contamination of soil by microplastics may pose risks that are often still not well understood, and the ecological effects of microplastics are mainly dependent on their environmental behavior in environments. This study used saturated quartz sand as a solid porous medium to study the migration and influencing factors of 40–48 μm polyethylene (PE) particles in saturated porous media. The breakthrough curves at different injection concentrations (0.3, 0.4, 0.5 mg/L), flow rates (1.0, 1.5, 2.0, 2.5 ml/L), porous medium particle sizes (1–2, 2–4 mm), ionic strengths (0, 0.01, 0.05 mol/L) and concentrations of fulvic acid (FA) (0, 5, 10 mg/L) were compared and analyzed. The Derjaguin-Landau-Verwey-Overbeek (DLVO) theory was used to more accurately explain relevant transport behaviors. The results showed that the input concentration, flow rate, and particle size can affect the migration of PE particles individually or in combination. As ionic strength increased, the repulsion between microplastics and quartz sand gradually disappeared according to DLVO theory, and their attraction gradually strengthened. As a result, fewer microplastics could penetrate the sand column and reach the water body. With the continuous addition of FA, the repulsive energy between microplastics and quartz sand rose from DLVO theory, and the migration ability of microplastics initially increased before becoming stable because of the effect of straining. In all cases, the migration ability of PE was low (C/C₀ < 0.35), and most PE particles remained in the porous media during the whole experimental periods. This study provides new insights of understanding the migration of microplastics in environment.
Show more [+] Less [-]The role of Fe oxyhydroxide coating, illite clay, and peat moss in nanoscale titanium dioxide (nTiO2) retention and transport in geochemically heterogeneous media
2020
Rastghalam, Zahra Sadat | Yan, Chaorui | Shang, Jianying | Cheng, Tao
Natural media such as soil and sediment contain mineralogical and organic components with distinct chemical, surface, and electrostatic properties. To better understand the role of various soil and sediment components on particle transport, columns were packed with quartz sand and natural sediment with added Fe oxyhydroxide coating, illite clay, and peat moss to investigate how these added components influence nTiO₂ retention and transport in geochemically heterogeneous medium. Results showed that nTiO₂ transport was low at pH 5, attributable to the electrostatic attraction between positively-charged nTiO₂ and negatively-charged medium. While illite did not notably affect nTiO₂ transport at pH 5, Fe oxyhydroxide coating increased nTiO₂ transport due to electrostatic repulsion between Fe oxyhydroxide and nTiO₂. Peat moss also increased nTiO₂ transport at pH 5, attributable to the increased DOC concentration, which resulted in higher DOC adsorption to nTiO₂ and intensified electrostatic repulsion between nTiO₂ and the medium. At pH 9, nTiO₂ transport was high due to the electrostatic repulsion between negatively-charged nTiO₂ and medium surfaces. Fe oxyhydroxide coating at pH 9 slightly delayed nTiO₂ transport due to electrostatic attraction, while illite clay and peat moss substantially inhibited nTiO₂ transport via straining/entrapment or electrostatic attraction. Overall, this study demonstrated that pH has a considerable effect on how minerals and organic components of a medium influence nTiO₂ transport. At low pH, electrostatic attraction was the dominant mechanism, therefore, nTiO₂ mobility was low regardless of the differences in mineralogical and organic components. Conversely, nTiO₂ mobility was high at high pH and nTiO₂ retention was dominated by straining/entrapment and sensitive to the mineralogical and organic composition of the medium.
Show more [+] Less [-]Importance of surface roughness on perfluorooctanoic acid (PFOA) transport in unsaturated porous media
2020
Lyu, Xueyan | Liu, Xing | Sun, Yuanyuan | Gao, Bin | Ji, Rong | Wu, Jichun | Xue, Yuqun
Understanding the subsurface transport of perfluorooctanoic acid (PFOA) is of considerable interest for evaluating its potential risks to humans and ecosystems. In this study, packed-column experiments were conducted to examine the influence of surface roughness on PFOA transport in unsaturated glass beads, quartz sand and limestone porous media. Results showed decreasing moisture content significantly increased the air-water interfacial adsorption of PFOA and led to greater retardation in all three types of porous media. Particularly, rougher surface (limestone > quartz sand > glass beads) and smaller grain size (i.e. a larger solid specific surface area, SSSA) significantly enhanced PFOA retardation under unsaturated conditions. These results were further supported by bubble column experiments and SSSA analysis of porous media, which demonstrate that except for the factors affecting PFOA transport in solid-water interface (e.g. surface charge and chemical heterogeneity), the greater retardation of PFOA during transport is attributed to the larger air-water interfacial areas associated with rougher surface and smaller grain size and hence greater interfacial adsorption of PFOA. Our results indicated the importance of surface roughness on the retention and transport of PFOA in the unsaturated zone.
Show more [+] Less [-]Rapid vitrification of uranium-contaminated soil: Effect and mechanism
2020
Shu, Xiaoyan | Li, Yaping | Huang, Wenxiao | Chen, Shunzhang | Xu, Chen | Zhang, Shuai | Li, Bingsheng | Wang, Xiaoqiang | Qing, Qi | Lu, Xirui
Nuclear contaminated soil can seriously threaten human security. In this study, uranium-contaminated soil (0–50000 μg/g of uranium) was successfully vitrified in 30 min without complex pretreatment or any additional components. The microstructure of the vitrified forms, the immobilizing mechanism of uranium, the inner structural evolution with increased uranium concentration, and the performance in terms of chemical durability were studied in detail. In the vitrified form, uranium was surrounded by a three-dimensional network structure comprising silicon and aluminum oxide polyhedra. When the uranium content increased above 50000 μg/g, the network adjusted and local structures precipitated as mottle-shaped quartz. The normalized leaching rates of uranium were maintained at a low value (∼1 × 10⁻⁶ g/(m²·d) level) in distilled water at 90 °C after 42 days. These results suggested the feasibility of vitrifying nuclear contaminated soil in a simple and rapid way.
Show more [+] Less [-]Photodegradation of polychlorinated naphthalene in mixtures
2020
Hanari, Nobuyasu | Falandysz, Jerzy | Yamazaki, Eriko | Yamashita, Nobuyoshi
Solutions of technical polychlorinated naphthalene (PCN) Halowax formulations (Halowax 1014 and Halowax 1051) diluted with Milli-Q water and sealed in the Pyrex glass tubes and quartz tubes were subjected to artificial solar and natural solar irradiation under different time intervals and field conditions. In particular, the results of several field irradiation experiments have shown increased PCN photodegradation as altitude increases above sea level. Irradiation in artificial solar conditions caused a substantial change in the PCN congener profiles of Halowax 1014 and Halowax 1051 test solutions. Interestingly, in long-term experiments, the relative abundance of congeners that contribute to dioxin-like activity, i.e. the compounds such as 1,2,3,5,7- and 1,2,4,6,7-PentaCN (PeCNs #52/60), 1,2,3,4,6,7- and 1,2,3,5,6,7-HexaCN (HxCNs #66/67), and 1,2,3,4,5,6,7-HeptaCN (HpCN #73), temporally increased substantially. In the field photodegradation experiments, the PCNs #52/60 and #66/67 were formed, while a relative persistence of PCN #73 was evident. Highest chlorinated octachloronaphthalene (OcCN #75), exposed to strong UV radiation at high altitude, was much less stable than lower molecular mass PCNs. Photodegradation of the technical PCN formulations produced also an unidentified aromatic compound. We conclude, that photodegradation of PCNs, which are considered as a widespread anthropogenic pollutants, is not restricted to any specific environmental condition. It can also be observed at low altitudes.
Show more [+] Less [-]Sulfide reduction can significantly enhance transport of biochar fine particles in saturated porous medium
2020
Ma, Pengkun | Chen, Wei
The release of fine particles from biochar materials applied in the environment may have important environmental implications, such as mobilization of environmental contaminants. In natural environments biochar fine particles can undergo various transformation processes, which may change their surface chemistry and consequently, the mobility of the particles. Here, we show that sulfide reduction can significantly alter the transport of wheat-straw- and pine-wood-derived biochar fine particles in saturated porous media. Counterintuitively, the sulfide-reduced biochar particles exhibited greater mobility in artificial groundwater than their non-reduced counterparts, even though reduction led to decrease of surface charge negativity and increase of hydrophobicity (from the removal of surface O-functional groups), both should favor particle deposition, as predicted based on extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) theory. Using transport experiments conducted in single-cation background solutions containing K⁺, Mg²⁺ or Ca²⁺ under different pH conditions, we show that the surprisingly greater mobility of sulfide-reduced biochar particles was attributable to the removal of surface carboxyl groups during reduction, as this markedly alleviated particle deposition through cation bridging, wherein Ca²⁺ acted as the bridging agent in linking the surface O-functional groups of biochar particles and quartz sand. These findings show the critical roles of surface properties in dictating the mobility of biochar fine particles and call for further understanding of their transport properties, which apparently cannot be simply extrapolated based on the findings of other (engineered) carbonaceous nanomaterials.
Show more [+] Less [-]Mass concentrations and lung cancer risk assessment of PAHs bound to PM1 aerosol in six industrial, urban and rural areas in the Czech Republic, Central Europe
2020
Křůmal, Kamil | Mikuška, Pavel
The daily concentrations of 15 polycyclic aromatic hydrocarbons (PAHs) in PM₁ aerosol samples, including 7 carcinogenic PAHs, were determined in six urban/rural areas in the Czech Republic in winter seasons between 2013 and 2017. The PM₁ aerosol was collected on quartz fibre filters using high-volume samplers for 24 h and PAHs were analysed by GC-MS. The highest concentrations of PAHs were found in the industrial city Ostrava (60.8 ng m⁻³), which is one of the most polluted areas in the Czech Republic, while the lowest concentrations were obtained in the small town Čelákovice (11.7 ng m⁻³) and in the background rural area Košetice (12.3 ng m⁻³). Carcinogenic PAHs formed 43.9%–57.8% of total analysed PAHs.The toxic equivalence factors for individual PAHs adopted from literature and two unit risks (Cal-EPA and WHO) were used for the evaluation of carcinogenic risk of PAHs exposure. The inhalation cancer risk models assume a lifetime exposure (70 years), whereas our measurement was realized for a relatively short duration in winters where concentrations of PAHs are usually high. The average of PAHs concentrations will be lower for the whole year resulting in lower lung cancer risk values. The calculated lifetime lung cancer risk of PAHs exposure for the measured winter periods suggested 1545 cases per 1 million people in Ostrava (industrial area), 192–456 cases per 1 million people in other four investigated cities/towns and 182 cases per 1 million people in Košetice (rural area). The calculated lifetime lung cancer risk values are related only to ambient concentrations of PAHs in atmospheric aerosols. Nevertheless, other factors can influence and increase the lung cancer risk, e.g., occupation, smoking, indoor emissions of coal/wood combustion in stoves or genetic factors of individuals. Our results can also be underestimated due to the determination of PAHs only in PM₁ aerosol.
Show more [+] Less [-]Modelling of multi-minerals kinetic evolution in hyper-alkaline leachate for a 15-year experiment
2020
Baqer, Yousef | Chen, Xiaohui | Rochelle, Christopher | Thornton, Steven
Cement has been widely used for low- to intermediate-level radioactive waste management; however, the long-term modelling of multiple mineral transfer between the cement leachate and the host rock of a geological disposal facility remains a challenge due to the strong physical-chemical interactions within the chemically disturbed zone. This paper presents a modelling study for a 15-year experiment simulating the reaction of crystalline basement rock with evolved near-field groundwater (pH = 10.8). A mixed kinetic equilibrium (MKE) modelling approach was employed to study the dolomite-rich fracture-filling assemblage reacting with intermediate cement leachate. The study found that the mineralogical and geochemical transformation of the system was driven by the kinetically controlled dissolution of the primary minerals (dolomite, calcite, quartz, k-feldspar and muscovite). The initial high concentration of calcium ions appeared to be the main driving force initiating the dedolomitization process, which played a significant role in the precipitation of secondary talc, brucite and Mg-aluminosilicate minerals. The modelling study also showed that most of the initially precipitated calcium silicon hydrate phases redissolved and formed more stable calcium silicon aluminium hydrate phases. The findings highlight the importance of a deep and insightful understanding of the geochemical transformations based on the type and characteristics of the host rock, where the system is under out of equilibrium conditions, and the rates of mineral reactions.
Show more [+] Less [-]A Simple and Green Vortex-Assisted Switchable Solvent-Based Microextraction Method by Using Schiff Base Ligand Complexation for Iron Determination in Mineral Spring Water Samples Prior to Slotted Quartz Tube Flame Atomic Absorption Spectrophotometry
2020
Kasa, Nursu Aylin | Bakirdere, Emine Gülhan | Bakirdere, Sezgin
In this study, a vortex-assisted switchable solvent microextraction (VA-SSME) method was developed for the determination of iron by slotted quartz tube flame atomic absorption spectrometry (SQT-FAAS). A ligand synthesized from the reaction of ortho-phenylenediamine and 5-bromosalicylaldehyde was used to form a coordinate complex of iron. All experimental variables such as switchable solvent amount, sodium hydroxide concentration, sodium hydroxide amount, and diluent amount were optimized to increase extraction efficiency for the iron complex. Optimum conditions were applied to aqueous standard solutions in the range of 20–750 ng/mL, and the percent relative standard deviation (%RSD) was less than 2.0%. The limit of detection (LOD) and limit of quantification (LOQ) were determined as 4.8 and 16.2 ng/mL, respectively. The optimized method recorded approximately 53 times enhancement according to the conventional FAAS system. The proposed method was applied to mineral spring water samples, and satisfactory percent recovery results (100–105%) were obtained for iron, indicating good applicability in addition to high accuracy.
Show more [+] Less [-]Coupled effect of flow velocity and structural heterogeneity on transport and release of kaolinite colloids in saturated porous media
2020
Mao, Meng | Zheng, Xiaoli | Chen, Chong | Zhao, Kang | Yan, Chaorui | Sharma, Prabhakar | Shang, Jianying
Understanding the behavior and fate of clay colloids in water-saturated porous media is critical to assess its environmental impact and potential risk since clay is commonly a carrier of many contaminants. Column experiments with four-packing configurations were designed to understand the coupled effects of column structural heterogeneity and the flow velocity on the transport and fate of kaolinite colloids in the saturated porous media. The results showed that the structural heterogeneity could have facilitated the transport of kaolinite colloids in saturated porous media. For the columns with strong heterogeneity, the preferential flow paths led to an early breakthrough of kaolinite. Only few kaolinite colloids were released with slow flow rate; however, the released peak concentration and release percentage of kaolinite colloids had further increased with the high flow velocity. In the layered column, there was significant kaolinite’s retention at the interface where water passed from fine to coarse quartz sand. All results indicated that both flow rates and media characteristics played an important role in controlling kaolinite’s fate and transport in porous media. A thorough understanding of these processes had an important significance for pollution control in subsurface natural environment where heterogeneous soil and variation in flow pattern are usually common.
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