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Publisher: Elsevier BV
Date: 07-2017
Publisher: Elsevier BV
Date: 04-2021
Publisher: American Chemical Society (ACS)
Date: 10-12-2014
DOI: 10.1021/ES503724K
Abstract: Biocides are critical components of hydraulic fracturing ("fracking") fluids used for unconventional shale gas development. Bacteria may cause bioclogging and inhibit gas extraction, produce toxic hydrogen sulfide, and induce corrosion leading to downhole equipment failure. The use of biocides such as glutaraldehyde and quaternary ammonium compounds has spurred a public concern and debate among regulators regarding the impact of inadvertent releases into the environment on ecosystem and human health. This work provides a critical review of the potential fate and toxicity of biocides used in hydraulic fracturing operations. We identified the following physicochemical and toxicological aspects as well as knowledge gaps that should be considered when selecting biocides: (1) uncharged species will dominate in the aqueous phase and be subject to degradation and transport whereas charged species will sorb to soils and be less bioavailable (2) many biocides are short-lived or degradable through abiotic and biotic processes, but some may transform into more toxic or persistent compounds (3) understanding of biocides' fate under downhole conditions (high pressure, temperature, and salt and organic matter concentrations) is limited (4) several biocidal alternatives exist, but high cost, high energy demands, and/or formation of disinfection byproducts limits their use. This review may serve as a guide for environmental risk assessment and identification of microbial control strategies to help develop a sustainable path for managing hydraulic fracturing fluids.
Publisher: Elsevier BV
Date: 12-2023
Publisher: American Chemical Society (ACS)
Date: 16-09-2014
DOI: 10.1021/AC502163K
Abstract: Two series of ethylene oxide (EO) surfactants, polyethylene glycols (PEGs from EO3 to EO33) and linear alkyl ethoxylates (LAEs C-9 to C-15 with EO3-EO28), were identified in hydraulic fracturing flowback and produced water using a new application of the Kendrick mass defect and liquid chromatography/quadrupole-time-of-flight mass spectrometry. The Kendrick mass defect differentiates the proton, ammonium, and sodium adducts in both singly and doubly charged forms. A structural model of adduct formation is presented, and binding constants are calculated, which is based on a spherical cagelike conformation, where the central cation (NH4(+) or Na(+)) is coordinated with ether oxygens. A major purpose of the study was the identification of the ethylene oxide (EO) surfactants and the construction of a database with accurate masses and retention times in order to unravel the mass spectral complexity of surfactant mixtures used in hydraulic fracturing fluids. For ex le, over 500 accurate mass assignments are made in a few seconds of computer time, which then is used as a fingerprint chromatogram of the water s les. This technique is applied to a series of flowback and produced water s les to illustrate the usefulness of ethoxylate "fingerprinting", in a first application to monitor water quality that results from fluids used in hydraulic fracturing.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8EM00336J
Abstract: In the western U.S., produced water from oil and gas wells discharged to surface water augments downstream supplies used for irrigation and livestock watering.
Publisher: Elsevier BV
Date: 03-2021
Publisher: Springer Science and Business Media LLC
Date: 26-06-2019
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9EM00153K
Abstract: Chemical changes to hydraulic fracturing fluids within fractured unconventional reservoirs may affect hydrocarbon recovery and, in turn, the environmental impact of unconventional oil and gas development.
Publisher: Elsevier BV
Date: 09-2011
DOI: 10.1016/J.CHROMA.2011.07.020
Abstract: The widely used solvent hexamethylphosphoramide (HMPA) and its biological (metabolic) and chemical (abiotic) phosphoramide-based oxidation products may cause adverse health effects through occupational exposure and intake of contaminated groundwater. However, no current methods exist for the separation and the detection of the many polar HMPA oxidation products. Thus, we developed a new RPLC/ESI-TOF-MS method and further investigated the chromatographic performances of two columns (i.e., XTerra Phenyl and XBridge Phenyl). In addition, the impact of (forced) acid hydrolysis for optimized chromatographic performance of the XTerra Phenyl column is investigated. The XTerra Phenyl column showed the best separation of the less polar major metabolic oxidation products pentamethylphosphoramide and hydroxymethyl-pentamethylphosphoramide, however, only after treating the column with formic acid (acid-treated). The XTerra column separated most of the investigated HMPA oxidation products (11 of 16 compounds) in a single chromatographic run. In contrast, the XBridge Phenyl column requires one method for the less polar and another method for the more polar oxidation products. However, this results in an overall better separation performance of the XBridge Phenyl column, especially for the less polar major abiotic oxidation products hydroxymethyl-pentamethylphosphoramide and formyl-pentamethylphosphoramide, as well as for 11 highly polar oxidation products (R(S)>1.5). The RPLC/ESI-TOF-MS method presented and validated in this study is the first analytical method that can be used to separate and detect HMPA (LOD 0.10 μM without preconcentration) and all of its oxidation products.
Publisher: Elsevier BV
Date: 03-2018
Publisher: Wiley
Date: 2021
DOI: 10.1111/GWMR.12425
Abstract: Chloronitrobenzenes (CNBs) are important chemical intermediates that are resistant to natural degradation processes in anoxic environments. When receptors are threatened by CNB‐contaminated groundwater, advanced oxidation processes (AOPs) offer a rapid response to protect human health and the environment. While AOPs are effective for the transformation of persistent organic contaminants, driving chemical oxidation reactions to complete mineralization is often not energy‐ and cost‐efficient due to the formation of recalcitrant intermediates or competition by natural organic matter. In this study, we applied an electrochemical AOP to elucidate the degradation pathways and kinetics of CNB under varying treatment conditions and times. Nontargeted mass spectrometry revealed multiple ring hydroxylation and ring opening products such as dicarboxylic acids that became increasingly harder to chemically oxidize as treatment time progressed. To determine the universal biodegradability of the generated intermediates under anoxic conditions, AOP‐treated water s les collected at different stages of electrochemical oxidation were exposed to a microbial culture derived from generic rhizosphere soil. All ring opening products were completely biodegraded anaerobically within 28 days of microcosm incubation. While multiple oxygenated ring intermediates were substantially removed, CNB was stable in the absence of oxygen. Our findings demonstrate that the combination of limited and targeted chemical oxidation with subsequent biodegradation of incomplete oxidation products is a more sustainable approach than the exclusive application of AOPs for the treatment of groundwater contaminated with CNBs and likely other aromatic compounds.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D0EM00413H
Abstract: Oil and gas extraction generates large volumes of produced water (PW) in regions that are water-stressed. PW can be passively treated in retention ponds prior to beneficial use. Oxic conditions lead to sequestration and lower bioavailability of Ra.
Publisher: Elsevier BV
Date: 11-2022
Publisher: Springer Science and Business Media LLC
Date: 11-07-2008
Publisher: Elsevier BV
Date: 02-2023
Publisher: Wiley
Date: 09-08-2019
DOI: 10.1002/IEAM.4160
Abstract: Produced water is the largest waste stream associated with oil and gas exploration and production operations. Most produced water generated onshore is managed by permitted injection in deep underground wells, but alternative disposal options including reuse are increasingly being considered. However, insufficient understanding of the composition and toxicity of produced water imposes significant constraints on effective management of potential short-term and long-term risks associated with such alternative uses. As interest builds for management options, such as surface discharge, livestock watering, irrigation, and other industrial uses, research is needed to assess produced-water hazards and exposures to both humans and the environment. This challenge affords an opportunity to capitalize on emerging risk assessment tools. Innovative and comprehensive approaches to filling data gaps and assessing produced water risks will be imperative. A group of experts from industry, academia, and government were assembled to define research needs to support objective decision making on the acceptability, or lack thereof, of produced water disposal alternatives. Presented here are key outcomes from that workshop and recommendations for a research framework to assess toxicity of produced water and associated risks from above ground discharge and reuse options. Integr Environ Assess Manag 2019 :677-682. © 2019 SETAC.
Publisher: American Chemical Society (ACS)
Date: 28-09-2016
Abstract: Hydraulic fracturing fluid (HFF) additives are used to enhance oil and gas extraction from unconventional shale formations. Several kilometers downhole, these organic chemicals are exposed to temperatures up to 200 °C, pressures above 10 MPa, high salinities, and a pH range from 5-8. Despite this, very little is known about the fate of HFF additives under these extreme conditions. Here, stainless steel reactors are used to simulate the downhole chemistry of the commonly used HFF biocide glutaraldehyde (GA). The results show that GA rapidly (t
Publisher: American Chemical Society (ACS)
Date: 12-02-2021
Publisher: American Chemical Society (ACS)
Date: 10-10-2019
Abstract: Hexafluoropropylene oxide dimer acid (HFPO-DA, trade name GenX) is a perfluoroalkyl ether carboxylic acid (PFECA) that has been detected in watersheds around the world. Similar to other per- and polyfluoroalkyl substances (PFASs), few processes are able to break HFPO-DA's persistent carbon-fluorine bonds. This study provides both experimental and computational lines of evidence for HFPO-DA mineralization during electrochemical oxidation at a boron-doped diamond anode with a low potential for the generation of stable organofluorine intermediates. Our density functional theory calculations consider the major operative mechanism, direct electron transfer, throughout the entire pathway. Initial oxidative attack does not break the ether bond, but leads to stepwise mineralization of the acidic side chain. Our mechanistic investigations reveal that hydroxyl radicals are unreactive toward HFPO-DA, while electrochemically activated sulfate facilitates its oxidation. Furthermore, we demonstrate that an NF90 membrane is capable of removing 99.5% of HFPO-DA from contaminated water. Electrochemical treatment of the nanofiltration rejectate is shown to reduce both energy and electrode costs by more than 1 order of magnitude compared to direct electrochemical treatment of the raw water. Overall, a nanofiltration-electrochemical oxidation treatment train is a sustainable destructive approach for the cost-effective elimination of HFPO-DA and other PFASs from contaminated water.
Publisher: Elsevier BV
Date: 12-2021
Publisher: American Chemical Society (ACS)
Date: 13-11-2017
Abstract: Hydraulic fracturing fluids are injected into shales to extend fracture networks that enhance oil and natural gas production from unconventional reservoirs. Here we evaluated the biodegradability of three widely used nonionic polyglycol ether surfactants (alkyl ethoxylates (AEOs), nonylphenol ethoxylates (NPEOs), and polypropylene glycols (PPGs)) that function as weatherizers, emulsifiers, wetting agents, and corrosion inhibitors in injected fluids. Under anaerobic conditions, we observed complete removal of AEOs and NPEOs from solution within 3 weeks regardless of whether surfactants were part of a chemical mixture or amended as in idual additives. Microbial enzymatic chain shortening was responsible for a shift in ethoxymer molecular weight distributions and the accumulation of the metabolite acetate. PPGs bioattenuated the slowest, producing sizable concentrations of acetone, an isomer of propionaldehyde. Surfactant chain shortening was coupled to an increased abundance of the diol dehydratase gene cluster (pduCDE) in Firmicutes metagenomes predicted from the 16S rRNA gene. The pduCDE enzymes are responsible for cleaving ethoxylate chain units into aldehydes before their fermentation into alcohols and carboxylic acids. These data provide new mechanistic insight into the environmental fate of hydraulic fracturing surfactants after accidental release through chain shortening and biotransformation, emphasizing the importance of compound structure disclosure for predicting biodegradation products.
Publisher: Elsevier BV
Date: 04-2020
DOI: 10.1016/J.SCITOTENV.2020.136607
Abstract: Produced water (PW) is the largest waste stream associated with oil and gas extraction and contains organics, salts, metals and radioactive materials. In the United States, west of the 98th meridian, the National Pollutant Discharge Elimination System exemption allows for release of PW to surface waters for agricultural beneficial reuse if it is "of good enough quality". Due to the complex and variable composition of PW, the downstream impacts of these releases are not fully understood. In this study, a detailed chemical analysis was conducted on a stream composed of PW released for agricultural beneficial reuse. Over 50 geogenic and anthropogenic organic chemicals not specified in the effluent limits were detected at the discharge including hydrocarbons, halogenated compounds, and surfactants. Most were removed within 15 km of the discharge due to volatilization, biodegradation, and sorption to sediment. Inorganics detected at the discharge were within regulatory effluent limits. While some inorganic species (i.e., strontium, barium and radium) decreased in concentration downstream due to co-precipitation, concentrations of many inorganic species including sodium, sulfate and boron increased due to water evaporation. Consequently, downstream water quality changes need to be considered to adequately evaluate the potential impact of discharged PW. Regulatory health thresholds for humans, livestock, and aquatic species for most chemical species present at the discharge are still lacking. As a result, toxicity tests are necessary to determine the potential health impacts to downstream users.
Publisher: American Chemical Society (ACS)
Date: 20-02-2011
DOI: 10.1021/ES1028662
Abstract: At contaminated field sites where active remediation measures are not feasible, monitored natural attenuation is sometimes the only alternative for surface water or groundwater decontamination. However, due to slow degradation rates of some contaminants under natural conditions, attenuation processes and their performance assessment can take several years to decades to complete. Here, we apply quantum chemical calculations to predict contaminant persistence in the aqueous phase. For the test compound hexamethylphosphoramide (HMPA), P-N bond hydrolysis is the only thermodynamically favorable reaction that may lead to its degradation under reducing conditions. Through calculation of aqueous Gibbs free energies of activation for all potential reaction mechanisms, it is predicted that HMPA hydrolyzes via an acid-catalyzed mechanism at pH < 8.2, and an uncatalyzed mechanism at pH 8.2-8.5. The estimated half-lives of thousands to hundreds of thousands of years over the groundwater-typical pH range of 6.0 to 8.5 indicate that HMPA will be persistent in the absence of suitable oxidants. At pH 0, where the hydrolysis reaction is rapid enough to enable measurement, the experimentally determined rate constant and half-life are in excellent agreement with the predicted values. Since the quantum chemical methodology described herein can be applied to virtually any contaminant or reaction of interest, it is especially valuable for the prediction of persistence when slow reaction rates impede experimental investigations and appropriate QSARs are unavailable.
Publisher: Elsevier BV
Date: 11-2014
DOI: 10.1016/J.CHEMOSPHERE.2014.03.109
Abstract: Polychlorinated biphenyls (PCBs) are well-known for being hydrophobic and persistent in the environment. Although many treatment approaches have been demonstrated to result in degradation of PCBs in water or water/cosolvent systems, few ex les exist where such approaches have been applied successfully for PCB degradation in soil-water systems. A possible explanation for the limited treatment of PCBs in soil-water systems is that reactants that are capable of degrading PCBs in the aqueous phase are unlikely to persist long enough to achieve meaningful treatment of slowly-desorbing PCBs associated with the soil phase. To investigate this explanation, laboratory studies were conducted to evaluate chemical reductants, including zero valent metals, palladium (Pd) catalyst, and emulsified zero valent iron (EZVI), for dechlorination of PCBs in the presence and absence of soil. In the absence of soil, Pd-catalyzed treatments (Pd with electrolytic ZVI or iron/aluminum alloy) achieved rapid destruction of a model PCB congener, 2-chlorobiphenyl, with half-lives ranging from 43 to 110 min. For treatment of soils containing Aroclor 1248 at an initial concentration of approximately 1,500 mg kg(-1), Pd-catalyzed treatments achieved no measurable enhancement over the background PCB depletion rate (i.e., that measured in the untreated control) of 5.3 mg kg(-1)week(-1). In the presence of soils, EZVI was the only approach evaluated that resulted in a clear enhancement in PCB dechlorination rates. EZVI achieved PCB concentration reductions of greater than 50% at an average rate of 19 mg kg(-1)week(-1). The results suggest that slow PCB desorption limits treatment effectiveness in soils.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1EM00311A
Abstract: Produced water (PW) is the largest waste stream associated with oil and gas (O& G) operations and contains petroleum hydrocarbons, heavy metals, salts, naturally occurring radioactive materials and any remaining chemical additives.
Publisher: Elsevier BV
Date: 02-2019
Publisher: American Chemical Society (ACS)
Date: 12-07-2017
Abstract: Combining horizontal drilling with high volume hydraulic fracturing has increased extraction of hydrocarbons from low-permeability oil and gas (O&G) formations across the United States accompanied by increased wastewater production. Surface water discharges of O&G wastewater by centralized waste treatment (CWT) plants pose risks to aquatic and human health. We evaluated the impact of surface water disposal of O&G wastewater from CWT plants upstream of the Conemaugh River Lake (dam controlled reservoir) in western Pennsylvania. Regulatory compliance data were collected to calculate annual contaminant loads (Ba, Cl, total dissolved solids (TDS)) to document historical industrial activity. In this study, two CWT plants 10 and 19 km upstream of a reservoir left geochemical signatures in sediments and porewaters corresponding to peak industrial activity that occurred 5 to 10 years earlier. Sediment cores were sectioned for the collection of paired s les of sediment and porewater, and analyzed for analytes to identify unconventional O&G wastewater disposal. Sediment layers corresponding to the years of maximum O&G wastewater disposal contained higher concentrations of salts, alkaline earth metals, and organic chemicals. Isotopic ratios of
Publisher: Elsevier BV
Date: 03-2022
Publisher: Elsevier BV
Date: 11-2021
Publisher: Elsevier BV
Date: 10-2023
Publisher: Elsevier BV
Date: 03-2022
Publisher: American Society of Civil Engineers (ASCE)
Date: 11-2022
Publisher: American Chemical Society (ACS)
Date: 30-10-2017
Abstract: Biodegradation of the persistent groundwater contaminant 1,4-dioxane is often hindered by the absence of dissolved oxygen and the co-occurrence of inhibiting chlorinated solvents. Using flow-through electrolytic reactors equipped with Ti/IrO
Publisher: Elsevier BV
Date: 05-2020
Publisher: Elsevier BV
Date: 06-2020
Publisher: Elsevier BV
Date: 06-2021
Publisher: Elsevier BV
Date: 10-2016
DOI: 10.1016/J.CHEMOSPHERE.2016.06.048
Abstract: Irrigation with reclaimed wastewater may result in the ubiquitous presence of pharmaceutical compounds (PCs) and their metabolites in the agroecosystem. In this study, we focused on two highly persistent anticonvulsant drugs, lamotrigine and carbamazepine and two of its metabolites (EP-CBZ and DiOH-CBZ), aiming to elucidate their behavior in agricultural ecosystem using batch and lysimeter experiments. Sorption of the studied compounds by soils was found to be governed mainly by the soil organic matter level. Sorption affinity of compounds to soils followed the order lamotrigine > carbamazepine > EP-CBZ > DiOH-CBZ. Sorption was reversible, and no competition between sorbates in bi-solute systems was observed. The results of the lysimeter studies were in accordance with batch experiment findings, demonstrating accumulation of lamotrigine and carbamazepine in top soil layers enriched with organic matter. Detection of carbamazepine and one of its metabolites in rain-fed wheat previously irrigated with reclaimed wastewater, indicates reversibility of their sorption, resulting in their potential leaching and their availability for plant uptake. This study demonstrates the long-term implication of introduction of PCs to the agroecosystem.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8EM00354H
Abstract: Hydraulic fracturing generates large volumes of produced water, and treatment of produced water may be necessary for disposal or reuse.
Publisher: Elsevier BV
Date: 06-2019
DOI: 10.1016/J.SCITOTENV.2019.03.041
Abstract: Hydraulic fracturing fluids are injected into unconventional oil and gas systems to stimulate hydrocarbon production, returning to the surface in flowback and produced waters containing a complex mixture of xenobiotic additives and geogenic compounds. Nonionic polyethoxylates are commonly added surfactants that act as weatherizers, emulsifiers, wetting agents, and corrosion inhibitors in hydraulic fracturing fluid formulations. Understanding the biodegradability of these ubiquitous additives is critical for produced water pre-treatment prior to reuse and for improving treatment trains for external beneficial reuse. The objective of this study was to determine the effect of produced water total dissolved solids (TDS) from an unconventional natural gas well on the aerobic biodegradation of alkyl ethoxylate and nonylphenol ethoxylate surfactants. Changes in surfactant concentrations, speciation and metabolites, as well as microbial community composition and activity were quantified over a 75-day aerobic incubation period. Alkyl ethoxylates (AEOs) were degraded faster than nonylphenol ethoxylates (NPEOs), and both compound classes and bulk organic carbon biodegraded slower in TDS treatments (10 g L
Publisher: Elsevier BV
Date: 02-2022
DOI: 10.1016/J.ENVPOL.2021.118603
Abstract: Granular activated carbon (GAC) has been used to remove per- and polyfluoroalkyl substances (PFASs) from industrial or AFFF-impacted waters, but its effectiveness can be low because adsorption of short-chained PFASs is ineffective and its sites are exhausted rapidly by co-contaminants. To increase adsorption of anionic PFASs on GAC by electrostatic attractions, we modified GAC's surface with the cationic polymer poly diallyldimethylammonium chloride (polyDADMAC) and tested its capacity in complex water matrices containing dissolved salts and humic acid. Amending with concentrations of polyDADMAC as low as 0.00025% enhanced GAC's adsorption capacity for PFASs, even in the presence of competing ions. This suggests that electrostatic interactions with polyDADMAC's quaternary ammonium functional groups helped bind organic and inorganic ions as well as the headgroup of short-chain PFASs, allowing more overall PFAS removal by GAC. Evaluating the effect of polymer dose is important because excessive addition can block pores and reduce overall PFAS removal rather than increase it. To decrease the waste associated with this adsorption strategy by making the adsorbent viable for more than one saturation cycle, a regeneration method is proposed which uses low-power ultrasound to enhance the desorption of PFASs from the polyDADMAC-GAC with minimum disruption to the adsorbent's structure. Re-modification with the polymer after sonication resulted in a negligible decrease in the sorbent's capacity over four saturation rounds. These results support consideration of polyDADMAC-modified GAC as an effective regenerable adsorbent for ex-situ concentration step of both short and long-chain PFASs from real waters with high concentrations of competing ions and low PFAS loads.
Publisher: Wiley
Date: 04-2019
DOI: 10.1111/GWMR.12323
Publisher: American Chemical Society (ACS)
Date: 08-08-2018
Abstract: The permanganate ion (MnO
Publisher: Wiley
Date: 28-04-2022
DOI: 10.1111/GWMR.12523
Abstract: Forecasting groundwater contaminant plume development is critical for determining risks to downgradient receptors and predicting the time to site closure. However, accurate forecasts are a formidable challenge due to the complexities of a heterogeneous subsurface. While historically groundwater well data in combination with numerical flow models have been used for this task, the advent of machine learning offers new data‐driven opportunities for improving contaminant fate and transport predictions. In this study, we interrogate the viability of two forecasting models—Prophet and d ed Holt's exponential smoothing model—for predicting groundwater contaminant plume development. The impacts of spatial and temporal data density on the accuracy of the forecasts are evaluated. For wells with declining contaminant concentrations, the d ed Holt's method achieves more accurate forecasts. However, only Prophet allows for the inclusion of exogenous regressors, enabling predictions of future declining trends in wells with still increasing contaminant concentrations. Application of these models does not only require robust training data, but also an understanding of model biases. Overall, powerful data‐driven models are already available for contaminant plume prediction, but groundwater s ling approaches will have to improve, for instance, through the collection of real‐time spatial and temporal high‐resolution data, to take full advantage of their capabilities.
Publisher: American Chemical Society (ACS)
Date: 29-07-2016
Abstract: 1,4-dioxane is an emerging groundwater contaminant with significant regulatory implications. Because it is resistant to traditional groundwater treatments, remediation of 1,4-dioxane is often limited to costly ex situ UV-based advanced oxidation. By varying applied voltage, electrical conductivity, seepage velocity, and influent contaminant concentration in flow-through reactors, we show that electrochemical oxidation is a viable technology for in situ and ex situ treatment of 1,4-dioxane under a wide range of environmental conditions. Using novel titanium dioxide (TiO2) pellets, we demonstrate for the first time that this prominent catalyst can be activated in the dark even when electrically insulated from the electrodes. TiO2-catalyzed reactors achieved efficiencies of greater than 97% degradation of 1,4-dioxane, up to 4.6 times higher than noncatalyzed electrolytic reactors. However, the greatest catalytic enhancement (70% degradation versus no degradation without catalysis) was observed in low-ionic-strength water, where conventional electrochemical approaches notoriously fail. The TiO2 pellet's dark-catalytic oxidation activity was confirmed on the pharmaceutical lamotrigine and the industrial solvent chlorobenzene, signifying that electrocatalytic treatment has tremendous potential as a transformative remediation technology for persistent organic pollutants in groundwater and other aqueous environments.
Publisher: Wiley
Date: 15-10-2018
DOI: 10.1111/GWMR.12307
Publisher: Elsevier BV
Date: 09-2023
Publisher: American Chemical Society (ACS)
Date: 26-05-2022
Publisher: Elsevier BV
Date: 10-2021
Publisher: American Chemical Society (ACS)
Date: 19-05-2016
Abstract: Hydraulic fracturing frequently occurs on agricultural land. Yet the extent of sorption, transformation, and interactions among the numerous organic frac fluid and oil and gas wastewater constituents upon environmental release is hardly known. Thus, this study aims to advance our current understanding of processes that control the environmental fate and toxicity of commonly used hydraulic fracturing chemicals. Poly(ethylene glycol) surfactants were completely biodegraded in agricultural topsoil within 42-71 days, but their transformation was impeded in the presence of the biocide glutaraldehyde and was completely inhibited by salt at concentrations typical for oil and gas wastewater. At the same time, aqueous glutaraldehyde concentrations decreased due to sorption to soil and were completely biodegraded within 33-57 days. While no aqueous removal of polyacrylamide friction reducer was observed over a period of 6 months, it cross-linked with glutaraldehyde, further lowering the biocide's aqueous concentration. These findings highlight the necessity to consider co-contaminant effects when we evaluate the risk of frac fluid additives and oil and gas wastewater constituents in agricultural soils in order to fully understand their human health impacts, likelihood for crop uptake, and potential for groundwater contamination.
Publisher: American Chemical Society (ACS)
Date: 07-07-2010
DOI: 10.1021/ES1006675
Abstract: Models used to predict the fate of aqueous phase contaminants are often limited by their inability to address the widely varying redox conditions in natural and engineered systems. Here, we present a novel approach based on quantum chemical calculations that identifies the thermodynamic conditions necessary for redox-promoted degradation and predicts potential degradation pathways. Hexamethylphosphoramide (HMPA), a widely used solvent and potential groundwater contaminant, is used as a test case. Its oxidation is estimated to require at least iron-reducing conditions at low to neutral pH and nitrate-reducing conditions at high pH. Furthermore, the transformation of HMPA by permanganate is predicted to proceed through sequential N-demethylation. Experimental validation based on LC/TOF-MS analysis confirms the predicted pathways of HMPA oxidation by permanganate to phosphoramide via the formation of less methylated as well as singly and multiply oxygenated reaction intermediates. Pathways predicted to be thermodynamically or kinetically unfavorable are similarly absent in the experimental studies. Our newly developed methodology will enable scientists and engineers to estimate the favorability of contaminant degradation at a specific field site, suitable approaches to enhance degradation, and the persistence of a contaminant and its reaction intermediates.
Publisher: Elsevier BV
Date: 12-2023
Publisher: American Chemical Society (ACS)
Date: 06-10-2021
Publisher: Elsevier BV
Date: 05-2020
Publisher: Elsevier BV
Date: 04-2022
Publisher: Elsevier BV
Date: 09-2021
Publisher: Springer Science and Business Media LLC
Date: 12-2006
Publisher: Wiley
Date: 06-2021
DOI: 10.1111/GWMR.12479
Publisher: Elsevier BV
Date: 04-2018
DOI: 10.1016/J.SCITOTENV.2017.11.078
Abstract: Hydraulic fracturing (HF) has allowed for the utilization of previously unattainable shale oil and gas (O&G) resources. After HF is complete, the waters used to increase the facies' permeability return uphole as wastewaters. When these waters return to the surface, they are characterized by complex organic and inorganic chemistry, and can pose a health risk if not handled correctly. Therefore, these waters must be treated or disposed of properly. However, the variability of these waters' chemical composition over time is poorly understood and likely limits the applicability of their reuse. This study examines the water chemistry of a hydraulically fractured site in the Niobrara formation throughout the flowback period. S les were collected every other day for the first 18days, then on a regular basis for three months. We identified HF fluid additives, including benzalkonium chlorides (BACs), alkyl ethoxylates (AEOs), and polyethylene glycols (PEGs), as well as geogenic components present in flowback and produced waters, their overall temporal pattern, and variables affecting the reuse of these waters. Observations indicate that alkalinity and iron may limit the reuse of these waters in HF, while chloride and alkalinity may limit the use of these waters for well-casing cement. The presence of numerous surfactant homologs, including biocides, was also observed, with the highest levels at the beginning of the flowback period. Principal component analysis identified three unique groupings in the chemical data that correspond to different stages in the flowback period: (1) the flowback stage (days 1-2) (2) the transition stage (days 6-21) and (3) the produced water stage (days 21-87). Results from this study will be important when designing decision frameworks for assessing water treatment options, particularly if onsite treatment is attempted. Successful reclamation of these waters may alleviate stress on water resources that continues to negatively impact the U. S.
Location: Australia
No related grants have been discovered for Jens Blotevogel.