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Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants

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A special issue of Water (ISSN 2073-4441). This special issue belongs to the section "Water Quality and Contamination".

Deadline for manuscript submissions: closed (31 January 2023) | Viewed by 25266

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Dr. Tohren C. Kibbey

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Guest Editor

School of Civil Engineering and Environmental Science, University of Oklahoma, Norman, OK, USA
Interests: surface and interfacial interactions in complex natural and engineered environmental systems; physical–chemical interactions in complex systems; behaviors in unsaturated soils/multiple-phase systems; numerical model development for prediction and design in complex systems
Special Issues, Collections and Topics in MDPI journals

Dr. Charalambos Papelis

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Carlsbad Environmental Monitoring & Research Center (CEMRC), New Mexico State University, Carlsbad, NM, USA
Interests: aquatic chemistry; surface chemistry of mineral surfaces; spectroscopic investigations of complexes at the mineral/water interface; physicochemical characterization of mineral surfaces; modeling diffusion and adsorption in porous earth materials and adsorbents; water quality; physicochemical water treatment processes; chemical and geochemical fate and transport of trace elements
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

This Special Issue invites papers describing studies that explore all aspects of the underlying processes that impact the fate, transport and treatment—both in situ and ex situ—of environmental contaminants. Of interest are physicochemical, physical, and biological processes that influence the behavior of environmental contaminants, with particular interest in systems where complex interactions between mechanisms are important. Papers focused on emerging contaminants (e.g., nanoparticles, PFAS, pharmaceuticals, microplastics) are of particular interest, although papers that describe processes that could apply to any category of contaminants are welcome.

Dr. Tohren C. Kibbey
Dr. Charalambos Papelis
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Water is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

environmental processes
water quality
contaminant transport
treatment
surface water
groundwater
saturated zone
unsaturated zone
organic contaminants
inorganic contaminants
emerging contaminants

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Published Papers (10 papers)

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Research

13 pages, 4823 KiB

Open AccessArticle

Water Quality and the First-Flush Effect in Roof-Based Rainwater Harvesting, Part II: First Flush

by Jessica J. Lay, Jason R. Vogel, Jason B. Belden, Glenn O. Brown and Daniel E. Storm

Water 2024, 16(10), 1421; https://doi.org/10.3390/w16101421 - 16 May 2024

Cited by 3 | Viewed by 2267

Abstract

Rainwater runoff samples from a range of roofing materials were temporally collected from 19 small-scale roof structures and two commercial buildings through simulated and actual storm events, and the concentrations of polycyclic aromatic hydrocarbons (PAHs), phosphorus flame retardants (PFLs), and pyrethroid insecticides and other water quality parameters were analyzed. In Part I of this research, the concentrations of these contaminants in roof runoff and soils receiving runoff from a range of roofing materials were evaluated. In Part II, recommendations have been developed for a first-flush exclusion to improve the quality of water harvesting for nonpotable uses. Recommendations focus on a first-flush diversion based on mass removals of total suspended solids (TSS) and PAHs linked to conductivity measurements throughout a storm event. Additionally, an upper-confidence limit (UCL) was constructed to determine the minimum diversion required to obtain 50, 75, 90, and 95% mass removal of TSS and PAH contaminants. The majority of TSS were produced during the initial 1.2 mm of runoff. Likewise, the majority of PAHs were removed during the initial 1.2 mm of runoff, except for the asphalt shingle roofs, where high PAHs were observed after 6 mm of runoff. The Texas Water Development Board (TWDB)-recommended first-flush diversion of one gallon for every 100 square feet of rooftop was not always adequate for removing 50% of TSS and PAHs from the roofs. Rainwater runoff conductivity decreased drastically between 1.2 to 2.4 mm of rainwater runoff. Diverting the first flush based on conductivity has the potential to also divert the majority of TSS and PAHs in roof runoff. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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27 pages, 4416 KiB

Open AccessArticle

Water Quality and the First-Flush Effect in Roof-Based Rainwater Harvesting, Part I: Water Quality and Soil Accumulation

by Jessica J. Lay, Jason R. Vogel, Jason B. Belden, Glenn O. Brown and Daniel E. Storm

Water 2024, 16(10), 1402; https://doi.org/10.3390/w16101402 - 14 May 2024

Cited by 2 | Viewed by 2799

Abstract

Rainfall runoff may be captured and stored for later use, but the quality of this water can be detrimental in some uses without the use of appropriately designed first-flush diverters. The rainfall runoff water quality was measured on nineteen new small-scale and two aged commercial roofs located near high traffic highways. Roof coverings included asphalt shingles, sheet metal, clay tiles, and tar and gravel. Runoff samples were evaluated for polycyclic aromatic hydrocarbons (PAHs), phosphorus flame retardants (PFRs), and pyrethroid insecticides. Eighteen small-scale roofs were subjected to a range of simulated rainfall events, while natural runoff was sampled on the commercial roofs and one small-scale roof. Runoff was analyzed for pH, conductivity, turbidity, total suspended solids, boron, iron, copper, zinc, manganese, sodium adsorption ratio, nitrate-nitrogen, seventeen PAHs, tris(2-chloroethyl) phosphate, tris(1,3-dichloro-2-propyl)phosphate, bifenthrin, cypermethrin, and lambda-cyhalothrin. Samples from four natural storm events were also analyzed for total coliforms and Escherichia coli. In addition, soils below seventeen existing gutter downspouts were sampled to determine long-term pollutant accumulation. Atmospheric deposition was the main contributor of pollutants in the roof runoff. A majority of samples fell within the U.S. EPA guidelines for non-potable urban and agricultural water reuse. Trace levels of PAHs, PFRs, and insecticides were detected, but all detections were three orders of magnitude below the USGS health-based screening level benchmark concentrations. Results indicate that diverting the first flush, based on turbidity, total suspended solids, or conductivity, can improve the overall water quality and reduce the concentrations of PAHs in harvested rainwater. Downspout soil sampling showed potential for the long-term accumulation of PAHs at concentrations exceeding the minimum human-health risk-based screening levels at these high runoff-loading locations. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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15 pages, 5110 KiB

Open AccessArticle

Thermal Treatment of Trichloroethene by Electrical Resistance Heating: Visualization of Gas Production in Coarse Layers

by Ariel Nunez Garcia, Pengjie Wang, Paul R. Hegele and Kevin G. Mumford

Water 2023, 15(11), 1976; https://doi.org/10.3390/w15111976 - 23 May 2023

Cited by 1 | Viewed by 2092

Abstract

The effective implementation of in situ thermal treatment (ISTT) technologies requires understanding of gas production and migration in heterogenous media. However, investigations of the effects of high permeability contrast on gas formation, accumulation, and migration, as well as its potential effect on the redistribution of dense non-aqueous phase liquid (DNAPL), are relatively rare. In this study, electrical resistance heating (ERH) experiments were conducted in a thin sand-packed cell to simulate common yet not well-studied scenarios encountered during ISTT applications, such as coarse lenses surrounded by finer material. Two packing configurations were employed: 2 mm glass beads surrounded by 20/30 silica sand and 20/30 silica sand overlaying 40/50 silica sand. Each experiment contained an emplaced pool of trichloroethene (TCE) within the coarse material. If permeable material or pathways were present between the coarse lens and the upper cell boundary, the gas migrated along these pathways, and local DNAPL redistribution was limited to near the top of the pool before it vaporized. In contrast, if the coarse material was surrounded by finer material and contained a sufficient volume of DNAPL, the gas accumulated inside the coarse lens leading to DNAPL displacement from the lens. For five selected DNAPLs, this volume was estimated to be 0.1% to 0.5% of the total pore volume of the coarse material. The conceptual model developed in this study improves our understanding of this common geological scenario, demonstrating the importance of considering both lower- and higher-permeability material and their effects on multiphase flow during co-boiling, as well as the design of gas extraction systems during ISTT applications. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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12 pages, 1145 KiB

Open AccessArticle

Effect of Nitrate Presence on Selenium Bioremediation in Chemically Modified Zeolite Columns

by Herath Mudiyanselage Ishani P. Kulasekara, Yanyan Zhang and Charalambos Papelis

Water 2023, 15(10), 1841; https://doi.org/10.3390/w15101841 - 12 May 2023

Cited by 3 | Viewed by 2787

Abstract

Selenium is an essential micro-nutrient for living organisms, but elevated concentrations of it in water can adversely affect health. Nitrate is often found in selenium-contaminated water and negatively correlates with selenium removal. In this study, we investigate the effect of nitrate co-existence on selenium bioremediation in chemically modified zeolite columns. Dynamic sorption-reduction experiments were conducted using natural and iron-coated zeolite columns to remove selenite and selenate oxyanions separately, with and without nitrate anions. Anaerobic sludge was included as microbial inoculum, while lactate was the sole electron donor. The initial selenium concentration (Se^IV or Se^VI) was 790 µg/L, the nitrate concentration was 620 mg/L, the pH was 7.5, and the flow rate was 3 mL/min. Before introducing nitrate ions, selenium reduction in all four columns reached approximately 99%. However, after introducing nitrate ions, selenate and selenite reduction efficiencies were reduced to approximately 93% and 60%, respectively. Biofilm microbial community composition, assessed by 16S rRNA sequencing, was distinct between the communities with and without nitrate anions. Specifically, in the absence of nitrate, biofilm communities are mainly composed of selenium-reducing bacteria (Veillonella, Bacteroides and Escherichia). In contrast, the presence of nitrate led to mostly denitrifying bacteria (Anaeromusa-Anaeroarcus, Lentimicrobium, Azospirillum and Endomicrobium). Further, comparison of diversity indices (Shannon index, Faith PD and Pielou’s) shows alteration in all indices in the presence of nitrate. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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17 pages, 4648 KiB

Open AccessArticle

Microbial Enhancement of Selenium Removal in Chemically Modified Zeolite Columns

by Herath Mudiyanselage Ishani P. Kulasekara, Yanyan Zhang and Charalambos Papelis

Water 2023, 15(10), 1837; https://doi.org/10.3390/w15101837 - 11 May 2023

Cited by 4 | Viewed by 2613

Abstract

Selenium (Se) is an essential micro-nutrient for living organisms, but elevated concentrations in water can adversely affect health. In this research, we investigate the removal of selenium oxyanions (selenate and selenite) in aqueous systems by integration of adsorption on modified zeolites and microbial reduction. Dynamic sorption-reduction experiments were conducted using two sets of zeolite columns for the removal of selenite and selenate oxyanions, respectively. In each case, one column was fully packed with natural, unmodified zeolites, while the other column was composed of 80% natural and 20% iron-coated zeolites, by mass. The initial selenium concentration, selenite (Se^IV) or selenate (Se^VI), was 790 μg/L, the pH was 7.5, and the flow rate was 3 mL/min. Initially, as expected, the higher selenate removal (34%) was observed with coated zeolite, twice as high compared to the results with unmodified zeolite. Maximum selenite removal was 89% in the column with modified zeolite. Within approximately 14 days, as the biofilm developed inside the columns, selenium reduction in all four columns reached approximately 99%. Biofilm microbial community composition, assessed by 16S rRNA sequencing, is consistent with the presence of mainly selenium-reducing bacteria (Veillonella, Bacteroides, and Escherichia). Selenium oxyanions were reduced to elemental selenium, visible within the bioreactors as red-color aggregates. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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16 pages, 12306 KiB

Open AccessArticle

Experiments and Simulations to Describe Alkalinity Release from Particle-Containing Oil-in-Water Emulsions and Particle Suspensions

by Katherine A. Muller and C. Andrew Ramsburg

Water 2023, 15(8), 1611; https://doi.org/10.3390/w15081611 - 20 Apr 2023

Cited by 2 | Viewed by 1883

Abstract

Among the most common amendments added to groundwater during site remediation are compounds used to adjust or maintain the pH. This research describes an approach to encapsulate mineral particles (MgO and CaCO₃) within oil droplets suspended within an aqueous phase for the purpose of delivery to the subsurface environment. A series of batch experiments was combined with mathematical modeling to illustrate the encapsulation and understand the influence of particle encapsulation on rates and extents of alkalinity release. The encapsulation of the alkalinity-releasing particles results in slower rates of amendment release as compared to rates obtained using suspensions of bare mineral particles, allowing for the possibility of control as a function of the pH. The results indicate that the alkalinity release from particle suspensions followed a mineral dissolution mechanism that could not explain the rate of the alkalinity release of the encapsulated particles. The reduction in mineral dissolution rates observed with the encapsulated particles was found to result from a mass transfer limitation. This limitation was well described using a linear driving force expression to account for the resistance to mass transfer at the oil–water interface. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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26 pages, 5602 KiB

Open AccessArticle

Experimental Investigation of Fluid Flow through Zinc Open-Cell Foams Produced by the Excess Salt Replication Process and Suitable as a Catalyst in Wastewater Treatment

by Amel Hind Hassein-Bey, Abd-Elmouneïm Belhadj, Hichem Tahraoui, Selma Toumi, Asma Nour El Houda Sid, Mohammed Kebir, Derradji Chebli, Abdeltif Amrane, Jie Zhang and Lotfi Mouni

Water 2023, 15(7), 1405; https://doi.org/10.3390/w15071405 - 4 Apr 2023

Viewed by 2249

Abstract

The “excess salt replication process” is a new simple method of fabrication of open-cell metal foam based on the commonly known salt replication method. Porous materials with porosity between 46% and 66% result when the employed alloy is 25% antimonial lead alloy and when it is 58% to 65% zamak 5. These foams are proposed as structured catalysts instead of packed beds in the treatment of wastewater. The local regimes influencing macroscopic air flow behaviour through these foams are delimited and boundaries are analysed in terms of sample length. Most of the experimental tests in this work exhibited a general trend of air flow in ESR foams dominated by the “strong inertia regime”. It was established that the law governing the unidirectional air flow through these foams was the full cubic law. The permeability and inertia coefficient of five samples with a cell diameter between 2.5 and 4.5 mm were calculated, and an empirical correlation was fitted. The irregular cuboid shape of salt grains used in the ESR foam was the origin of the special cell form of ESR foams leading to an anisotropic ordered porous media. This can explain the macroscopic turbulence of air flow because there were many dead zones present in the corner of each cubic cell, thus causing kinetic energy loss starting at earlier regimes. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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15 pages, 3037 KiB

Open AccessArticle

Characterization of Bubble Transport in Porous Media Using a Microfluidic Channel

by Ryan Haggerty, Dong Zhang, Jongwan Eun and Yusong Li

Water 2023, 15(6), 1033; https://doi.org/10.3390/w15061033 - 9 Mar 2023

Cited by 5 | Viewed by 3740

Abstract

This study investigates the effect on varying flow rates and bubble sizes on gas–liquid flow through porous media in a horizontal microchannel. A simple bubble generation system was set up to generate bubbles with controllable sizes and frequencies, which directly flowed into microfluidic channels packed with different sizes of glass beads. Bubble flow was visualized using a high-speed camera and analyzed to obtain the change in liquid holdup. Pressure data were measured for estimation of hydraulic conductivity. The bubble displacement pattern in the porous media was viscous fingering based on capillary numbers and visual observation. Larger bubbles resulted in lower normalized frequency of the bubble breakthrough by 20 to 60 percent. Increasing the flow rate increased the change in apparent liquid holdup during bubble breakthrough. Larger bubbles and lower flow rate reduced the relative permeability of each channel by 50 to 57 percent and 30 to 64 percent, respectively. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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17 pages, 2810 KiB

Open AccessArticle

The Influence of pH on Subsurface Denitrification Stimulated with Emulsified Vegetable Oil

by Veronica L. Gonsalez, Paul M. Dombrowski, Michael D. Lee and C. Andrew Ramsburg

Water 2023, 15(5), 883; https://doi.org/10.3390/w15050883 - 24 Feb 2023

Cited by 1 | Viewed by 2141

Abstract

Treatment of nitrate rich groundwater using permeable reactive barriers (PRBs) established with injection of emulsified vegetable oil is receiving attention in areas where groundwater discharges contribute to eutrophication (e.g., Cape Cod, MA). To better understand the biogeochemical process kinetics when emulsified vegetable oil (EVO) is used to stimulate denitrification within the subsurface, microcosm experiments and process-based modeling were conducted for pH conditions ranging from 4 to 8. Biomass variability in soil and pH variations were found to affect denitrification, with limited nitrate reduction observed below pH 5.0. Different rates for denitrification associated with biomass variability suggest that a greater characterization of the indigenous biological community may improve PRB design and operation. Process-based modeling employed the activated sludge model No 3 (AMS3) framework that assumes denitrification as a two-step anoxic process dependent primarily on heterotrophic bacteria, soluble substrate, nitrate, and nitrite. Experimental data were used to calibrate the model under neutral to low pH, resulting in a robust set of equations that can be coupled with transport in future research to improve PRB effectiveness. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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11 pages, 2181 KiB

Open AccessFeature PaperArticle

The Influence of Evaporation and Seasonal Effects on the Water Content in the Unsaturated Zone: A Multi-Year Laboratory Study

by Aderonke O. Adegbule and Tohren C. G. Kibbey

Water 2022, 14(20), 3294; https://doi.org/10.3390/w14203294 - 19 Oct 2022

Cited by 1 | Viewed by 1847

Abstract

The unsaturated zone of the subsurface plays a critical role in the environmental fate and transport of a wide range of environmental contaminants, and is also important for plant growth and agriculture. Quantitative prediction of processes in the unsaturated zone requires knowledge of how water content varies with elevation above the water table, a relationship known as the capillary pressure (P_c)–saturation (S) relationship. While the P_c–S relationship is conventionally thought of as being primarily a property of the porous medium and fluids, previous work found evidence suggesting that it actually results from a dynamic equilibrium between capillary forces and phenomena driven by evaporation. The focus of this work was on gaining a further understanding of the role of evaporation on the P_c–S relationship. The work made use of a tall instrumented laboratory column connected to an external reservoir for maintaining water table height. Following an initial imbibition experiment, the column was saturated and allowed to drain, and then water content was monitored in the column as a function of height over 1207 days (3.31 years). While initial imbibition and drainage were rapid, on the order of hours, redistribution and evaporation effects became apparent over longer time scales (hundreds of hours). A drying front moving downward in the column was apparent from changes in the slopes of saturation vs. time curves as it passed individual sensors; unlike previous experiments with a more fully-vented column, the evaporation front appeared to stall, balanced by the capillary-driven upward flow of water. Over the full multi-year duration of the experiment, seasonal trends in water saturation were apparent, with significant, reversible variations observed that closely followed atmospheric conditions. Specifically, saturation above the water table appeared to increase during the spring and summer months and decrease during the fall and winter months, despite the constant water table location, consistent with a changing driving force for evaporation. This result may suggest the likelihood of seasonal effects in the long-term transport and fate of contaminants in the unsaturated zone. Full article

(This article belongs to the Special Issue Natural and Engineered Phenomena Impacting the Fate, Transport and Treatment of Environmental Contaminants)

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