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Graphene oxide-facilitated uranium transport and release in saturated medium: Effect of ionic strength and medium structure
2019
Zhao, Kang | Chen, Chong | Cheng, Tao | Shang, Jianying
Natural subsurface environment is a complex heterogeneous system. To investigate the effect of ionic strength (IS) and heterogeneity on the transport and remobilization of graphene oxide (GO)-facilitated uranium (U(VI)) in saturated porous media, column experiments were performed by the injection of U(VI) alone and U(VI)+GO mixtures into homogeneous and heterogeneous porous media under low and high ionic strength (1 and 50 mM) conditions, and then the columns were successively flushed with background solution and DI water. Results showed that when U(VI) only was introduced into the columns, IS had little effect on the migration of U(VI) alone in both media and the presence of preferential flow in heterogeneous media slightly enhanced the mobility of U(VI). As U(VI)+GO mixtures were injected into the columns, GO showed strong mobility at low IS and high released peak at high IS. The appearance of GO significantly enhanced U(VI) transport in both media. Under low IS condition, the mobility of U(VI) was significantly enhanced at the injection phase, and the medium heterogeneity further promoted the amount of GO-sorbed U(VI) transport. At high IS, less GO-sorbed U(VI) was observed during injection phase, and a large amount of retained GO-sorbed U(VI) were released with GO remobilization during water flushing phase, and the release showed the longer-tailing phenomenon and the release amount was more pronounced in heterogeneous media. The findings in this study showed that the coupled effect of solution chemistry and media heterogeneity played important roles on GO-facilitated U(VI) transport and release in soil and groundwater system.
Show more [+] Less [-]Bioturbation of Ag2S-NPs in soil columns by earthworms
2019
Baccaro, Marta | Harrison, Samuel | van den Berg, Hans | Sloot, Laura | Hermans, Davy | Cornelis, Geert | van Gestel, Cornelis A.M. | Brink, Nico W. van den
Sewage sludge contains Ag₂S-NPs causing NP exposure of soil fauna when sludge is applied as soil amendment. Earthworm bioturbation is an important process affecting many soil functions. Bioturbation may be affected by the presence of Ag₂S-NPs, but the earthworm activity itself may also influence the displacement of these NPs that otherwise show little transport in the soil. The aim of this study was to determine effects of Ag₂S-NPs on earthworm bioturbation and effect of this bioturbation on the vertical distribution of Ag₂S-NPs. Columns (12 cm) of a sandy loamy soil with and without Lumbricus rubellus were prepared with and without 10 mg Ag kg⁻¹, applied as Ag₂S-NPs in the top 2 cm of the soil, while artificial rainwater was applied at ∼1.2 mm day⁻¹. The soil columns were sampled at three depths weekly for 28 days and leachate collected from the bottom. Total Ag measurements showed more displacement of Ag to deeper soil layers in the columns with earthworms. The application of rain only did not significantly affect Ag transport in the soil. No Ag was detected in column leachates. X-ray tomography showed that changes in macro porosity and pore size distribution as a result of bioturbation were not different between columns with and without Ag₂S-NPs. Earthworm activity was therefore not affected by Ag₂S-NPs at the used exposure concentration. Ag concentrations along the columns and the earthworm density allowed the calculation of the bioturbation rate. The effect on the Ag transport in the soil shows that earthworm burrowing activity is a relevant process that must be taken into account when studying the fate of nanoparticles in soils.
Show more [+] Less [-]Role of surface functionalities of nanoplastics on their transport in seawater-saturated sea sand
2019
Dong, Zhiqiang | Zhu, Ling | Zhang, Wen | Huang, Rui | Lv, XiangWei | Jing, Xinyu | Yang, Zhenglong | Wang, Junliang | Qiu, Yuping
The transport and retention of nanoplastics (NP, 200 nm nanopolystyrene) functionalized with surface carboxyl (NPC), sulfonic (NPS), low-density amino (negatively charged, NPA−), and high-density amino (positively charged, NPA+) groups in seawater-saturated sand with/without humic acid were examined to explore the role of NP surface functionalities. The mass percentages of NP recovered from the effluent (Meff) with a salinity of 35 practical salinity units (PSU) were ranked as follows: NPC (19.69%) > NPS (16.37%) > NPA+ (13.33%) > NPA− (9.78%). The homoaggregation of NPS and NPA− was observed in seawater. The transport of NPA− exhibited a ripening phenomenon (i.e., a decrease in the transport rate with time) due to the high attraction of NP with previously deposited NP, whereas monodispersed NPA+ presented a low Meff value because of the electrostatic attraction between NPA+ and negatively charged sand. Retention experiments showed that the majority of NPC, NPS and NPA+ accumulated in a monolayer on the sand surface, whereas NPA− accumulated in multiple layers. Suwannee River humic acid (SRHA) could remarkably improve the transportability of NPC, NPS, and NPA− by increasing steric repulsion. The strong attraction between NPA+ and the deposited NPA+ in the presence of SRHA triggered the weak ripening phenomenon. As seawater salinity decreased from 35 PSU to 3.5 PSU, the increase in electrostatic repulsion of NP-NP and NP-sand enhanced the transport of NPC, NPS, and NPA−, and the ripening of NPA− breakthrough curves disappeared. In deionized water, NPC, NPS, and NPA− achieved complete column breakthrough because the electrostatic repulsion between NP and sand intensified. However, the Meff values of NPA+ in 3.5 PSU seawater and deionized water presented limited increments of 15.49% and 23.67%, respectively. These results indicated that the fate of NP in sandy marine environments were strongly affected by NP surface functionalities, seawater salinity, and coexisting SRHA.
Show more [+] Less [-]Effects of myo-inositol hexakisphosphate, ferrihydrite coating, ionic strength and pH on the transport of TiO2 nanoparticles in quartz sand
2019
Tang, Yadong | Wang, Xiaoming | Yan, Yupeng | Zeng, Huan | Wang, Gang | Tan, Wenfeng | Liu, Fan | Feng, Xionghan
Evaluating the fate and transport of nanoparticles (NPs) in the subsurface environment is critical for predicting the potential risks to both of the human health and environmental safety. It is believed that numerous environmental factors conspire to control the transport dynamics of nanoparticles, yet the effects of organic phosphates on nanoparticles transport remain largely unknown. In this work, we quantified the transport process of TiO2 nanoparticle (nTiO2) and their retention patterns in water-saturated sand columns under various myo-inositol hexakisphosphate (IHP) or phosphate (Pi) concentrations (0–180 μM P), ferrihydrite coating fractions (λ, 0–30%), ionic strengths (1–50 mM KCl), and pH values (4–8). The transport of nTiO2 was enhanced at increased P concentration due to the enhanced colloidal stability. As compared with Pi at the equivalent P level, IHP showed stronger effect on the electrokinetic properties of nTiO2 particles due to its relatively more negative charge and higher adsorption affinity, thereby facilitating the nTiO2 transport (and thus reduced retention) in porous media. At the IHP concentration of 5 μM, the retention of nTiO2 increased with increasing λ and ionic strength, while decreased with pH. In addition, the retention profiles of nTiO2 showed a typical hyperexponential pattern for most scenarios mainly due to the unfavorable attachment, and can be well described by a hybrid mathematical model that coupled convection dispersion equations with a two-site kinetic model and DLVO theory. These quantitative estimations revealed the importance of IHP on affecting the transport of nTiO2 typically in phosphorus-enriched environments. It provides new insights into advanced understanding of the co-transport of nanoparticles and phosphorus in natural systems, essential for both nanoparticle exposure and water eutrophication.
Show more [+] Less [-]Transport and retention of reduced graphene oxide materials in saturated porous media: Synergistic effects of enhanced attachment and particle aggregation
2019
Xia, Tianjiao | Ma, Pengkun | Qi, Yu | Zhu, Lingyan | Qi, Zhichong | Chen, Wei
The increasing production and use of graphene-based nanomaterials (e.g., graphene oxide (GO) and reduced graphene oxide (RGO)) will lead to their environmental release. To date, transport of RGOs in saturated porous media is poorly understood. Here, we examined the transport behaviors of three RGO materials obtained by reducing a GO product with commonly used reducing agents – N₂H₄, NaBH₄ and L-ascorbic acid (referred to as N₂H₄-RGO, NaBH₄-RGO and VC-RGO, respectively). When the dominant background cation was Na⁺, K⁺ or Mg²⁺, the mobility of the RGOs and GO in saturated quartz sand correlated well with their surface C/O ratio. Interestingly, the lower mobility of the more reduced materials (the ones with higher C/O values) was not only the results of their less negative surface charges and larger particle sizes, but also the outcome of their greater hydrophobicity, in line with the calculated extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) profiles. Counterintuitively, when the background cation was Ca²⁺, the least reduced material among the three RGOs, VC-RGO, exhibited the lowest mobility. Analysis of electrophoretic and aggregation properties, as well as pH-effect experiments, indicated that the surprisingly low mobility of VC-RGO was attributable to the strong cation-bridging effect (primarily Ca²⁺-bridging between RGO and quartz sand) associated with this material, as VC-RGO contained the highest amount of surface carboxyl group (a strong metal-binding moiety). Notably, enhanced attachment (due to increased hydrophobic effect and cation-bridging) and particle aggregation appeared to work synergistically to increase RGO retention, as the attachment of large RGO aggregates significantly enhanced particle straining by narrowing the flow path. These observations reveal a largely overlooked link between the mobility of graphene-based materials and their key physicochemical properties.
Show more [+] Less [-]Influence of titanium dioxide nanoparticles on the transport and deposition of microplastics in quartz sand
2019
Cai, Li | He, Lei | Peng, Shengnan | Li, Meng | Tong, Meiping
The influence of titanium dioxide nanoparticles (nTiO₂) on the transport and deposition of polystyrene microplastics (MPs) in saturated quartz sand was investigated in NaCl solutions with ionic strengths from 0.1 to 10 mM at two pH conditions (pH 5 and 7). Three different-sized polystyrene (PS) MPs (diameter of 0.2, 1, and 2 μm) were concerned in present study. We found that for all three different-sized MPs in NaCl solutions (0.1, 1 and 10 mM) at both pH 5 and 7, lower breakthrough curves and higher retained profiles of MPs with nTiO₂ copresent in suspensions relative to those without nTiO₂ were obtained, demonstrating that the copresence of nTiO₂ in MPs suspensions decreased MPs transport and increased their deposition in quartz sand under all examined conditions. The mechanisms contributing to the increased MPs deposition with nTiO₂ in suspensions at two pH conditions were different. The formation of MPs-nTiO₂ heteroaggregates and additional deposition sites provided by previously deposited nTiO₂ were found to drive to the increased MPs deposition with nTiO₂ in suspensions at pH 5, while the formation of MPs-nTiO₂ aggregates, additional deposition sites and increased surface roughness induced by the pre-deposited nTiO₂ on quartz sand surfaces were responsible for the enhanced MPs deposition at pH 7. The results give insights to predict the fate and transport of different-sized MPs in porous media in the copresence of engineered nanoparticles.
Show more [+] Less [-]Deepwater Horizon Oil could have naturally reached Texas beaches
2019
Thyng, Kristen M.
Following the Deepwater Horizon (DWH) spill, oil residues were found in all five Gulf states of the United States (Texas, Louisiana, Mississippi, Alabama and Florida). However, only a small amount was found in Texas, leading to speculation that it may have arrived there via ship through bilge water instead of naturally via currents. We report on a numerical modeling effort to simulate surface drifters during and after the DWH spill to demonstrate that surface water parcels – and therefore oil carried by those parcels – could reasonably have reached Texas waters at the appropriate time and location from known oiled locations without human interference. We additionally give context for the conditions in 2010 through a study of summer connectivity with the Galveston Bay coastline, which shows that in some years oil from the DWH pipe likely would not have reached Texas.
Show more [+] Less [-]Responses of salinity and chlorophyll-a to extreme rainfall events in the northwest Arabian Gulf: Emphasis on Shatt Al-Arab
2019
Alosairi, Y. | Alsulaiman, N. | Petrov, P. | Karam, Q.
Recent extreme hydrological events, such as high rainfall and storms, have been linked to climate change worldwide due to their relatively uncommon trends, which are generally described as having varying frequencies and higher intensities. Similar extreme rainfall trends were observed in the northwest Arabian Gulf during the 2018–2019 season. Heavy rainfall events have triggered high discharges in the river of Shatt Al-Arab, where, prior to these events, the discharge rate has exhibited a declining trend over the past 40 years. Shatt Al-Arab provides various physical, chemical, and biological functions in the region. In this study, some recent and extensive measurements of salinity and post-processed satellite images of chlorophyll-a in the northwest Arabian Gulf were recorded to assess the response of the region to the higher discharges. The results indicated that the salinity decreased significantly during and after the rainfall events in response to the higher discharges from Shatt Al-Arab. The effects of higher discharges extended over most of Kuwait's coastline, including Kuwait Bay. The chlorophyll-a distributions doubled after the extreme events, emphasising the effects of Shatt Al-Arab. Collectively, the results indicated that the discharge from Shatt Al-Arab during the extreme event exceeded 1400 m³/s, while, in the previous seasons, it rarely exceeded 80 m³/s. The higher discharge levels of discharge would result in various changes in ecology at multiple levels due to the sudden and reversing shift in the hydro-environmental processes.
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