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The Robert  H Smith Faculty
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Publications

2018
Young, R. B. ; Avneri-Katz, S. ; McKenna, A. M. ; Chen, H. ; Bahureksa, W. ; Polubesova, T. ; Chefetz, B. ; Borch, T. Composition-Dependent Sorptive Fractionation of Anthropogenic Dissolved Organic Matter by Fe(III)-Montmorillonite. Soil Systems 2018, 2. Publisher's VersionAbstract
Water transports organic matter through soils, where mineral-organic associations form to retain dissolved organic matter (“DOM”), influencing terrestrial carbon cycling, nutrient availability for plant growth, and other soil organic matter functions. We combined Fourier transform ion cyclotron resonance mass spectrometry with novel data analysis techniques to examine the role of sorptive fractionation in the associations between Fe(III)-montmorillonite and DOM from composted biosolids (“anthropogenic DOM”). To examine the influence of DOM composition on sorption and sorptive fractionation, we used resin-based separation to produce DOM subsamples with different molecular compositions and chemical properties. A large proportion (45 to 64%) of the initial carbon in every DOM solution sorbed to the Fe(III)-montmorillonite. However, when the compositions of the initial solutions were compared to the sorbed organic matter, the computed changes in composition were lower (10 to 32%). In fact, non-selective sorption was more important than selective sorption in every sample, except for the hydrophilic neutral (HiN) fraction, where high nitrogen content and acidic conditions appeared to enhance sorptive fractionation. The results from this study demonstrate that the importance of sorptive fractionation varies with DOM composition and other factors, and that non-selective sorption can contribute substantially to the formation of mineral-organic associations.
Ben Mordechay, E. ; Tarchitzky, J. ; Chen, Y. ; Shenker, M. ; Chefetz, B. Composted biosolids and treated wastewater as sources of pharmaceuticals and personal care products for plant uptake: A case study with carbamazepine. Environmental Pollution 2018, 232, 164 - 172. Publisher's VersionAbstract
Irrigation with treated wastewater (TWW) and application of biosolids to arable land expose the agro-environment to pharmaceuticals and personal care products (PPCPs) which can be taken up by crops. In this project, we studied the effect of a carrier medium (e.g., biosolids and TWW) on plant (tomato, wheat and lettuce) uptake, translocation and metabolism of carbamazepine as a model for non-ionic PPCPs. Plant uptake and bioconcentration factors were significantly lower in soils amended with biosolids compared to soils irrigated with TWW. In soils amended with biosolids and irrigated with TWW, the bioavailability of carbamazepine for plant uptake was moderately decreased as compared to plants grown in soils irrigated with TWW alone. While TWW acts as a continuous source of PPCPs, biosolids act both as a source and a sink for these compounds. Moreover, it appears that decomposition of the biosolids in the soil after amendment enhances their adsorptive properties, which in turn reduces the bioavailability of PPCPs in the soil environment. In-plant metabolism of carbamazepine was found to be independent of environmental factors, such as soil type, carrier medium, and absolute amount implemented to the soil, but was controlled by the total amount taken up by the plant.
Engel, M. ; Hadar, Y. ; Belkin, S. ; Lu, X. ; Elimelech, M. ; Chefetz, B. Bacterial inactivation by a carbon nanotube–iron oxide nanocomposite: a mechanistic study using E. coli mutants. Environmental Science: Nano 2018, 5 372 - 380. Publisher's VersionAbstract
Waterborne pathogens are a major health threat and must be eliminated to guarantee safe usage of water for potable purposes. For this purpose, a new carbon-based nanomaterial composed of single-walled carbon nanotubes (SWCNTs) and iron oxides was constructed for bacterial inactivation. Owing to its magnetic properties, the SWCNT–iron oxide nanocomposite may serve as a reusable antimicrobial agent. The nanocomposite material exhibited high antimicrobial activity against Escherichia coli. Successful reuse of the nanocomposite material was achieved by washing with calcium chloride and distilled water, which restored its performance for several successive cycles. To investigate the cytotoxicity mechanisms of the nanocomposite material, we exposed it to single-gene knockout mutant strains of E. coli. Mutants bearing shorter lipopolysaccharide (LPS) layers in the outer membrane (ΔrfaC and ΔrfaG) demonstrated an increased sensitivity in comparison to the wildtype strain, exemplified in enhanced removal by the nanocomposite material. This finding suggests that the LPS acts as a protective shield against the nanocomposite material. Inactivation of mutants impaired in specific oxidative stress defense mechanisms (ΔsodA, ΔkatG and ΔsoxS) emphasized that oxidative stress plays a significant role in the inactivation mechanism of the nanocomposite. This study sheds light on the mechanisms of bacterial inactivation by carbon-based nanomaterials and advances their potential implementation for water disinfection.
Bhaduri, B. ; Engel, M. ; Polubesova, T. ; Chefetz, B. Multifunctional carbon nanotubes-iron oxide-Ag composite for water purification. In EGU General Assembly Conference Abstracts; EGU General Assembly Conference Abstracts; 2018; Vol. 20, pp. 2434.
Topaz, T. ; Egozi, R. ; Eshel, G. ; Chefetz, B. Pesticide load dynamics during stormwater flow events in Mediterranean coastal streams: Alexander stream case study. Science of The Total Environment 2018, 625, 168 - 177. Publisher's VersionAbstract
Cultivated land is a major source of pesticides, which are transported with the runoff water and eroded soil during rainfall events and pollute riverine and estuarine environments. Common ecotoxicological assessments of riverine systems are mainly based on water sampling and analysis of only the dissolved phase, and address a single pesticide's toxicological impact under laboratory conditions. A clear overview of mixtures of pesticides in the adsorbed and dissolved phases is missing, and therefore the full ecotoxicological impact is not fully addressed. The aim of this study was to characterize and quantify pesticide concentrations in both suspended sediment and dissolved phases, to provide a better understanding of pesticide-load dynamics during storm events in coastal streams in a Mediterranean climate. High-resolution sampling campaigns of seven flood events were conducted during two rainy seasons in Alexander stream, Israel. Samples of suspended sediments were separated from the solution and both media were analyzed separately for 250 pesticides. A total of 63 pesticides were detected; 18 and 16 pesticides were found solely in the suspended sediments and solution, respectively. Significant differences were observed among the pesticide groups: only 7% of herbicide, 20% of fungicide and 42% of insecticide load was transported with the suspended sediments. However, in both dissolved and adsorbed phases, a mix of pesticides was found which were graded from “mobile” to “non-mobile” with varied distribution coefficients. Diuron, and tebuconazole were frequently found in large quantities in both phases. Whereas insecticide and fungicide transport is likely governed by application time and method, the governing factor for herbicide load was the magnitude of the stream discharge. The results show a complex dynamic of pesticide load affected by excessive use of pesticides, which should be taken into consideration when designing projects to monitor riverine and estuarine water quality.
Wu, W. ; Zhang, R. ; McClements, D. J. ; Chefetz, B. ; Polubesova, T. ; Xing, B. Transformation and Speciation Analysis of Silver Nanoparticles of Dietary Supplement in Simulated Human Gastrointestinal Tract. Environmental Science & Technology 2018, 52, 8792 - 8800. Publisher's VersionAbstract
Knowledge of the physicochemical properties of ingestible silver nanoparticles (AgNPs) in the human gastrointestinal tract (GIT) is essential for assessing their bioavailability, bioactivity, and potential health risks. The gastrointestinal fate of AgNPs and silver ions from a commercial dietary supplement was therefore investigated using a simulated human GIT. In the mouth, no dissolution or aggregation of AgNPs occurred, which was attributed to the neutral pH and the formation of biomolecular corona, while the silver ions formed complexes with biomolecules (Ag-biomolecule). In the stomach, aggregation of AgNPs did not occur, but extensive dissolution was observed due to the low pH and the presence of Cl–. In the fed state (after meal), 72% AgNPs (by mass) dissolved, with 74% silver ions forming Ag-biomolecule and 26% forming AgCl. In the fasted state (before meal), 76% AgNPs dissolved, with 82% silver ions forming Ag-biomolecule and 18% forming AgCl. A biomolecular corona around AgNPs, comprised of mucin with multiple sulfhydryl groups, inhibited aggregation and dissolution of AgNPs. In the small intestine, no further dissolution or aggregation of AgNPs occurred, while the silver ions existed only as Ag-biomolecule. These results provide useful information for assessing the bioavailability of ingestible AgNPs and their subsequently potential health risks, and for the safe design and utilization of AgNPs in biomedical applications.Knowledge of the physicochemical properties of ingestible silver nanoparticles (AgNPs) in the human gastrointestinal tract (GIT) is essential for assessing their bioavailability, bioactivity, and potential health risks. The gastrointestinal fate of AgNPs and silver ions from a commercial dietary supplement was therefore investigated using a simulated human GIT. In the mouth, no dissolution or aggregation of AgNPs occurred, which was attributed to the neutral pH and the formation of biomolecular corona, while the silver ions formed complexes with biomolecules (Ag-biomolecule). In the stomach, aggregation of AgNPs did not occur, but extensive dissolution was observed due to the low pH and the presence of Cl–. In the fed state (after meal), 72% AgNPs (by mass) dissolved, with 74% silver ions forming Ag-biomolecule and 26% forming AgCl. In the fasted state (before meal), 76% AgNPs dissolved, with 82% silver ions forming Ag-biomolecule and 18% forming AgCl. A biomolecular corona around AgNPs, comprised of mucin with multiple sulfhydryl groups, inhibited aggregation and dissolution of AgNPs. In the small intestine, no further dissolution or aggregation of AgNPs occurred, while the silver ions existed only as Ag-biomolecule. These results provide useful information for assessing the bioavailability of ingestible AgNPs and their subsequently potential health risks, and for the safe design and utilization of AgNPs in biomedical applications.
Bhaduri, B. ; Engel, M. ; Polubesova, T. ; Wu, W. ; Xing, B. ; Chefetz, B. Dual functionality of an Ag-Fe3O4-carbon nanotube composite material: Catalytic reduction and antibacterial activity. Journal of Environmental Chemical Engineering 2018, 6 4103 - 4113. Publisher's VersionAbstract
Carbon-based nanomaterials have remarkable chemical and biological features. The introduction of supporting magnetic materials onto carbon-based nanoparticles has gained interest owing to their easy separation from heterogeneous systems. Herein, we report the synthesis of a novel composite comprised of single-walled carbon nanotubes, Fe3O4 and Ag nanoparticles with an aim to develop a bifunctional composite for water purification that maintains both high catalytic and antibacterial activities. The composite facilitated decomposition of nitrophenols and methyl orange in the presence of NaBH4 as the reducing agent – maintaining high activity (>90%) following three regeneration cycles. The composite’s catalytic activity was unaffected by the presence of dissolved organic matter (DOM) at an environmentally relevant concentration of 5 mg C L−1. DOM concentration of 50 mg C L−1 slightly decreased the reduction of p-nitrophenol, 2-methyl-p-nitrophenol, and methyl orange (by ∼14%, ∼11%, and ∼10% respectively) but significantly decreased that of o-nitrophenol (by 38%). The composite exhibited high antibacterial activity towards gram-negative and gram-positive bacteria even in the presence of DOM at an environmentally relevant concentration. However, the composite’s efficiency decreased with increase in DOM concentration. This study demonstrates dual catalytic and antibacterial activity of a novel Ag-Fe3O4-single walled carbon nanotube composite material in the absence and presence of DOM, and considers its potential implementation in water/wastewater treatment applications.
Karpov, M. ; Seiwert, B. ; Mordehay, V. ; Reemtsma, T. ; Polubesova, T. ; Chefetz, B. Transformation of oxytetracycline by redox-active Fe(III)- and Mn(IV)-containing minerals: Processes and mechanisms. Water Research 2018, 145, 136 - 145. Publisher's VersionAbstract
Abiotic mechanisms of oxytetracycline degradation by redox-active minerals, Fe(III)-saturated montmorillonite (Fe-SWy) and birnessite (δ-MnO2), were studied to better understand the environmental behavior of tetracycline antibiotics in aqueous systems. Kinetics of dissipation (adsorption, oxidation and formation of transformation products (TPs)), was investigated up to 7 days, and reaction mechanisms were elucidated based on identification of TPs by liquid chromatography mass spectrometry. Oxytetracycline was completely removed from solution by both minerals, however kinetics, TPs and mechanisms were distinct for each mineral. Oxytetracycline oxidation by δ-MnO2 occurred within minutes; 54 identified TPs were detected only in solution, most of them exhibited decreasing levels with time. In contrast, oxytetracycline was completely adsorbed by Fe-SWy, its degradation was slower, only 29 TPs were identified, among them 13 were surface-bound, and most of the TPs accumulated in the system with time. Oxytetracycline transformation by δ-MnO2 involved radicals, as was proven by electrochemical degradation. Reductive dissolution was observed for both minerals. X-ray photoelectron spectroscopy demonstrated accumulation of Fe(II) on Fe-SWy surface, whereas Mn(II) was primarily released from δ-MnO2 surface. Highly oxidized carbon species (i.e., newly formed TPs) were observed on the surface of both minerals interacting with oxytetracycline. This study demonstrates the impact of structure and reactivity of redox-active minerals on removal and decomposition of tetracycline antibiotics in aqueous systems.