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1.
Birth Defects Res ; 115(14): 1264-1273, 2023 08 15.
Artigo em Inglês | MEDLINE | ID: mdl-37334869

RESUMO

Gadolinium (Gd), a toxic rare earth element, has been shown to dissociate from chelating agents and bioaccumulate within tissues, raising concerns about the possibility of their remobilization during pregnancy with subsequent free Gd exposures to developing fetuses. Gd chelates are among the most commonly used magnetic resonance imaging (MRI) contrast agents. This investigation was undertaken after the detection of elevated Gd (800-1000× higher than the usual rare earth element levels) in preliminary unpublished studies from the placentae of subjects in the NIH ECHO/UPSIDE Rochester Cohort Study and unpublished studies from placentae analyzed in formalin-fixed placental specimens from Surgical Pathology at the University of Rochester. Fifteen pregnancies with elevated Gd were studied (12 first pregnancies and 3 second pregnancies). Maternal bloods were collected from all three trimesters, maternal, and cord (fetal) bloods at delivery as well as placental tissue. Breastmilk was also collected from selected mothers. It was determined that Gd was present in maternal bloods from all three trimesters, and in cord bloods and breastmilk in both first and second pregnancies. These results emphasize the need to fully appreciate the implications of pre-pregnancy exposure to Gd chelates and its potential effects on maternal and fetal health.


Assuntos
Meios de Contraste , Gadolínio , Humanos , Feminino , Gravidez , Meios de Contraste/efeitos adversos , Gadolínio/efeitos adversos , Placenta/diagnóstico por imagem , Estudos de Coortes , Quelantes , Mães , Número de Gestações
3.
Placenta ; 131: 98-103, 2023 01.
Artigo em Inglês | MEDLINE | ID: mdl-36577279

RESUMO

INTRODUCTION: There is increasing interest in measuring metals concentrations in human placentas to better understand physiology, disease, and toxic and diagnostic exposures. For these purposes, formalin-fixed paraffin embedded (FFPE) tissues obtained at clinical pathology examination represent a valuable potential store of well-characterized tissues for analysis. However, the limited data that exist comparing metal concentrations in FFPE tissue to recently collected frozen tissues paints a confusing picture, and there is no published data directly comparing frozen and FFPE placental villus tissues. METHODS: Paired samples of fresh frozen and FFPE tissue from 22 rapidly processed human singleton placentae were weighed and digested using standard clean laboratory procedures and subsequently analyzed for a suite of 13 metals using a PerkinElmer DRC II ICP-MS. The analytical results were compared using either a paired t-test or a sign test depending on data normality. RESULTS: Concentrations of metals (aluminum (Al), arsenic (As), barium (Ba), cadmium (Cd), chromium (Cr), copper (Cu), iron (Fe), gadolinium (Gd), mercury (Hg), manganese (Mn), lead (Pb), strontium (Sr), and zinc (Zn)) measured in both types of tissue preparations (frozen and FFPE) displayed a consistent range with other studies and did not display significantly different values from each of the paired specimens for any of the 13 specific metals analyzed. DISCUSSION: Within placentae, metals concentrations of measured trace, toxic and diagnostic elements (Al, As, Ba, Cd, Cr, Cu, Fe, Gd, Hg, Mn, Pb, Sr, and Zn) are consistent between FFPE and fresh placental villus tissue, without indications of systematic element loss or bias. FFPE from archived pathology specimens may offer an important and convenient alternative for measuring trace metals in human frozen placental tissues.


Assuntos
Mercúrio , Oligoelementos , Gravidez , Humanos , Feminino , Oligoelementos/análise , Cádmio , Inclusão em Parafina , Chumbo , Placenta/química , Manganês , Cromo , Formaldeído
4.
Sci Total Environ ; 850: 157971, 2022 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-35963401

RESUMO

High concentrations of metal(loid)s in phosphate rocks and wastewater associated with phosphate mining and fertilizer production operations pose potential contamination risks to water resources. Here, we propose using Sr isotopes as a tracer to determine possible water quality impacts induced from phosphate mining and fertilizers production. We utilized a regional case study in the northeastern Negev in Israel, where salinization of groundwater and a spring have been attributed to historic leaking and contamination from an upstream phosphate mining wastewater. This study presents a comprehensive dataset of major and trace elements, combined with Sr isotope analyses of the Rotem phosphate rocks, local aquifer carbonate rocks, wastewater from phosphate operation in Mishor Rotem Industries, saline groundwater suspected to be impacted by Rotem mining activities, and two types of background groundwater from the local Judea Group aquifer. The results of this study indicate that trace elements that are enriched in phosphate wastewater were ubiquitously present in the regional and non-contaminated groundwater at the same levels as detected in the impacted waters, and thus cannot be explicitly linked to the phosphate wastewater. The 87Sr/86Sr ratios of phosphate rocks (0.707794 ±â€¯5 × 10-5) from Mishor Rotem Industries were identical to that of associated wastewater (0.707789 ±â€¯3 × 10-5), indicating that the Sr isotopic fingerprint of phosphate rocks is preserved in its wastewater. The 87Sr/86Sr (0.707949 ±â€¯3 × 10-6) of the impacted saline groundwater were significantly different from those of the Rotem wastewater and the background saline groundwater, excluding phosphate mining effluents as the major source for contamination of the aquifer. Instead, the 87Sr/86Sr ratio of the impacted water was similar to the composition of brines from the Dead Sea, which suggests that the salinization was derived primarily from industrial Dead Sea effluents with distinctive Sr isotope and geochemical fingerprints.


Assuntos
Água Subterrânea , Oligoelementos , Poluentes Químicos da Água , Carbonatos/análise , Monitoramento Ambiental/métodos , Fertilizantes/análise , Água Subterrânea/química , Isótopos/análise , Fosfatos/análise , Isótopos de Estrôncio/análise , Oligoelementos/análise , Águas Residuárias/análise , Poluentes Químicos da Água/análise
5.
Geohealth ; 6(6): e2021GH000556, 2022 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-35663618

RESUMO

As the global population ages and the proportion of individuals afflicted with musculoskeletal disease spirals upward, there is an increasing interest in understanding and preventing bone-related diseases. Bone diseases, such as osteoporosis and osteoarthritis, are known to be influenced by a variety of factors including age, gender, nutrition, and genetics, but are also inherently linked to the human body's ability to produce biominerals of suitable quality. Because the crystal lattice structure and mineralogy of bone hydroxyapatite is surprisingly analogous to geological hydroxyapatite, trace element levels and exposure have long been proposed to influence the structure of biominerals as they do geological minerals (e.g., strontium substitution changes the crystal lattice of bone minerals, while toxic lead disrupt bone cellular processes leading to bone disease). Here, we explore the distribution of trace elements in human bones to evaluate the distribution of these elements with respect to bone type (cortical vs. trabecular) and bone disease (osteoarthritis vs. osteoporosis). We find higher concentrations of many metabolically active transition metals, as well as lead, in cortical bone compared to trabecular bone. When compared to patients who have osteoarthritis, and thus presumably normal bone minerals, osteoporosis patients have higher concentrations of scandium and chromium (Cr) in trabecular bone, and Cr and lead in cortical bone. Lower concentrations of barium and titanium are associated with osteoporotic trabecular bone. This survey is an exploratory cross-sectional geochemical examination of several trace element concentrations previously understudied in human bone minerals.

6.
Sci Total Environ ; 808: 151914, 2022 Feb 20.
Artigo em Inglês | MEDLINE | ID: mdl-34856287

RESUMO

This critical review presents the key factors that control the occurrence of natural elements from the uranium- and thorium-decay series, also known as naturally occurring radioactive materials (NORM), including uranium, radium, radon, lead, polonium, and their isotopes in groundwater resources. Given their toxicity and radiation, elevated levels of these nuclides in drinking water pose human health risks, and therefore understanding the occurrence, sources, and factors that control the mobilization of these nuclides from aquifer rocks is critical for better groundwater management and human health protection. The concentrations of these nuclides in groundwater are a function of the groundwater residence time relative to the decay rates of the nuclides, as well as the net balance between nuclides mobilization (dissolution, desorption, recoil) and retention (adsorption, precipitation). This paper explores the factors that control this balance, including the relationships between the elemental chemistry (e.g., solubility and speciation), lithological and hydrogeological factors, groundwater geochemistry (e.g., redox state, pH, ionic strength, ion-pairs availability), and their combined effects and interactions. The various chemical properties of each of the nuclides results in different likelihoods for co-occurrence. For example, the primordial 238U, 222Rn, and, in cases of high colloid concentrations also 210Po, are all more likely to be found in oxic groundwater. In contrast, in reducing aquifers, Ra nuclides, 210Pb, and in absence of high colloid concentrations, 210Po, are more mobile and frequently occur in groundwater. In highly permeable sandstone aquifers that lack sufficient adsorption sites, Ra is often enriched, even in low salinity and oxic groundwater. This paper also highlights the isotope distributions, including those of relatively long-lived nuclides (238U/235U) with abundances that depend on geochemical conditions (e.g., fractionation induced from redox processes), as well as shorter-lived nuclides (234U/238U, 228Ra/226Ra, 224Ra/228Ra, 210Pb/222Rn, 210Po/210Pb) that are strongly influenced by physical (recoil), lithological, and geochemical factors. Special attention is paid in evaluating the ability to use these isotope variations to elucidate the sources of these nuclides in groundwater, mechanisms of their mobilization from the rock matrix (e.g., recoil, ion-exchange), and retention into secondary mineral phases and ion-exchange sites.


Assuntos
Água Subterrânea , Rádio (Elemento) , Urânio , Poluentes Radioativos da Água , Humanos , Rádio (Elemento)/análise , Tório , Urânio/análise , Poluentes Radioativos da Água/análise
7.
Environ Sci Technol ; 55(15): 10387-10397, 2021 08 03.
Artigo em Inglês | MEDLINE | ID: mdl-34282893

RESUMO

Coal combustion residuals (CCRs), in particular, coal fly ash, are one of the major industrial solid wastes in the U.S., and due to their high concentrations of toxic elements, they could pose environmental and human health risks. Yet detecting coal fly ash in the environment is challenging given its small particle size. Here, we explore the utility and sensitivity of using geochemical indicators (trace elements, Ra nuclides, and Pb stable isotopes), combined with physical observation by optical point counting, for detecting the presence of trace levels of coal fly ash particles in surface soils near two coal-fired power plants in North Carolina and Tennessee. Through experimental work, mixing models, and field data, we show that trace elements can serve as a first-order detection tool for fly ash presence in surface soils; however, the accuracy and sensitivity of detection is limited for cases with low fly ash proportion (i.e., <10%) in the soil, which requires the integration of more robust Ra and Pb isotopic tracers. This study revealed the presence of fly ash particles in surface soils from both the recreational and residential areas, which suggests the fugitive emission of fly ash from the nearby coal-fired power plants.


Assuntos
Cinza de Carvão , Carvão Mineral , Carvão Mineral/análise , Cinza de Carvão/análise , Humanos , Resíduos Industriais , Centrais Elétricas , Solo
8.
Proc Natl Acad Sci U S A ; 117(42): 26145-26150, 2020 10 20.
Artigo em Inglês | MEDLINE | ID: mdl-33020284

RESUMO

Irrigated agriculture contributes 40% of total global food production. In the US High Plains, which produces more than 50 million tons per year of grain, as much as 90% of irrigation originates from groundwater resources, including the Ogallala aquifer. In parts of the High Plains, groundwater resources are being depleted so rapidly that they are considered nonrenewable, compromising food security. When groundwater becomes scarce, groundwater withdrawals peak, causing a subsequent peak in crop production. Previous descriptions of finite natural resource depletion have utilized the Hubbert curve. By coupling the dynamics of groundwater pumping, recharge, and crop production, Hubbert-like curves emerge, responding to the linked variations in groundwater pumping and grain production. On a state level, this approach predicted when groundwater withdrawal and grain production peaked and the lag between them. The lags increased with the adoption of efficient irrigation practices and higher recharge rates. Results indicate that, in Texas, withdrawals peaked in 1966, followed by a peak in grain production 9 y later. After better irrigation technologies were adopted, the lag increased to 15 y from 1997 to 2012. In Kansas, where these technologies were employed concurrently with the rise of irrigated grain production, this lag was predicted to be 24 y starting in 1994. In Nebraska, grain production is projected to continue rising through 2050 because of high recharge rates. While Texas and Nebraska had equal irrigated output in 1975, by 2050, it is projected that Nebraska will have almost 10 times the groundwater-based production of Texas.


Assuntos
Irrigação Agrícola/normas , Conservação dos Recursos Hídricos/métodos , Produtos Agrícolas/crescimento & desenvolvimento , Grão Comestível/crescimento & desenvolvimento , Água Subterrânea/análise , Modelos Teóricos , Abastecimento de Água/normas , Recursos Hídricos/provisão & distribuição
9.
Environ Sci Technol ; 54(16): 10068-10077, 2020 08 18.
Artigo em Inglês | MEDLINE | ID: mdl-32672450

RESUMO

Hexavalent chromium (Cr(VI)) is known to occur naturally in shallow oxic groundwater, typically from aquifers associated with mafic and ultramafic formations, but information on the occurrence of Cr(VI) in deep groundwater from large sedimentary basins is limited. This study shows that groundwater from the Baiyangdian Lake Basin (BYB), home to the future second capital city of China, had high Cr concentration (>10 µg/L, up to 86 µg/L) in the deep aquifer (>150 m), while shallow groundwater had lower Cr concentration (<10 µg/L). Chromium occurred predominantly as Cr(VI) (>95%). Shallow groundwater was characterized by higher Mn and Fe concentrations relative to deep groundwater, likely indicating more reducing conditions. Sequential extraction experiments from aquifer sediments suggest that Cr(VI) may derive from silicate weathering and that Mn oxides in the aquifer play a major role in the formation of Cr(VI) in groundwater. Inverse correlations between Mn and Cr(VI) suggest that reductive dissolution of Mn oxides constrains Cr(VI) mobilization in the shallow groundwater, while oxic-suboxic conditions in the deep aquifer limit Mn solubility, which enhances oxidation of Cr(III) to Cr(VI) and promotes desorption of Cr(VI) under alkaline conditions. This study demonstrates the potential geogenic occurrence of high Cr(VI) concentration in deep groundwater from a nonmafic, large sedimentary basin containing Mn oxides in the aquifer sediments.


Assuntos
Água Subterrânea , Poluentes Químicos da Água , China , Cromo/análise , Poluentes Químicos da Água/análise
10.
Environ Sci Technol ; 54(7): 4367-4375, 2020 04 07.
Artigo em Inglês | MEDLINE | ID: mdl-32167307

RESUMO

The co-occurrence of contaminants in drinking water may pose enhanced risks to health beyond the effects of single contaminants. Here, we investigated the co-occurrence of four health-relevant redox-sensitive elements (U, As, V, and Cr) in 1494 groundwater wells across North Carolina. The highest concentrations of these elements were measured mostly in groundwater from fractured igneous and metamorphic formations throughout the Piedmont region. Arsenic occurred most frequently in suboxic to mixed redox character groundwater, whereas U, V, and Cr occurred mostly in oxic groundwater. Occurrences of As, and to a lesser extent U, increased with pH, likely reflecting desorption, while higher Cr and V levels were measured in near-neutral pH and oxic groundwater, reflecting greater sensitivity to redox conditions. Due to similar geochemistry, V and Cr co-occurred most frequently. Concentrations of V and Cr(VI) co-exceeded health recommendations from the NC Department of Health and Human Services in up to 84% of wells from the King's Mountain Belt and the Charlotte and Milton Belts of the Piedmont region. This study highlights the large gap between health recommendations and enforceable regulations and demonstrates a degree of co-occurrence between redox-sensitive elements, which may pose additional risks to groundwater-reliant individuals.


Assuntos
Arsênio , Água Subterrânea , Urânio , Poluentes Químicos da Água , Cromo , Monitoramento Ambiental , Humanos , North Carolina , Oxirredução , Estados Unidos , Vanádio
11.
Sci Total Environ ; 711: 135135, 2020 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-32000345

RESUMO

Hexavalent chromium (Cr(VI)) is a groundwater contaminant that is potentially harmful to human health. Understanding the occurrence of Cr(VI) in groundwater resources is critical for evaluating its risks to human health. Here we report a large dataset (n = 1362) of Cr(VI) and total chromium (CrT) concentrations in public, private, and monitoring wells from different aquifers across North Carolina. These water quality data come from new and previous measurements conducted at Duke University, as well as data reported by the U.S. Environmental Protection Agency, the N.C. Department of Environmental Quality, and the U.S. Geological Survey. The data confirm that Cr(VI) is the predominant species of dissolved Cr and that groundwater from aquifers in the Piedmont region contain significantly higher concentrations than groundwater from the coastal plain. Though there is only one exceedance of the U.S. EPA Maximum Contaminant Level (100 µg/L for CrT) in the dataset, over half of all wells measured for Cr(VI) (470 out of 865) in the dataset exceeded the N.C. Health Advisory Level of 0.07 µg/L. Using information from this dataset, we explore three different approaches to predicting Cr(VI) in groundwater: (1) CrT concentrations as a proxy for Cr(VI); (2) Exceedance probabilities of health goals for groundwater from aquifers located in specific geologic areas; and (3) Censored linear regression using commonly measured field parameters (pH, electrical conductivity, dissolved oxygen) with relationships to Cr(VI) as regressors. Combining these approaches, we have identified several areas in the Piedmont region where Cr(VI) in drinking water wells is expected to be higher than the advisory level, which coincide with large population groundwater reliant populations. While this study focuses on N.C., the wide-spread occurrence of Cr(VI) in groundwater at concentrations above health guidelines in aquifers of the Piedmont region could pose high human health risks to large populations in the eastern U.S.

12.
Sci Total Environ ; 688: 1216-1227, 2019 Oct 20.
Artigo em Inglês | MEDLINE | ID: mdl-31726552

RESUMO

Northwest India suffers from severe water scarcity issues due to a combination of over-exploitation and climate effects. Along with concerns over water availability, endemic water quality issues are critical and affect the usability of available water and potential human health risks. Here we present data from 243 groundwater wells, representing nine aquifer lithologies in 4 climate regions that were collected from the Northwestern Indian state of Rajasthan. Rajasthan is India's largest state by area, and has a significant groundwater reliant population due to a general lack of surface water accessibility. We show that the groundwater, including water that is used for drinking without any treatment, contains multiple inorganic contaminants in levels that exceed both Indian and World Health Organization (WHO) drinking water guidelines. The most egregious of these violations were for fluoride, nitrate, and uranium; 76% of all water samples in this study had contaminants levels that exceed the WHO guidelines for at least one of these species. In addition, we show that much of the groundwater contains high concentrations of dissolved organic carbon (DOC) and halides, both of which are risk factors for the formation of disinfectant byproducts in waters that are treated with chemical disinfectants such as chlorine. By using geochemical and isotopic (oxygen, hydrogen, carbon, strontium, and boron isotopes) data, we show that the water quality issues derive from both geogenic (evapotranspiration, water-rock interactions) and anthropogenic (agriculture, domestic sewage) sources, though in some cases anthropogenic activities, such as infiltration of organic- and nitrate-rich water, may contribute to the persistence and enhanced mobilization of geogenic contaminants. The processes affecting Rajasthan's groundwater quality are common in many other worldwide arid areas, and the lessons learned from evaluation of the mechanisms that affect the groundwater quality are universal and should be applied for other parts of the world.

13.
Environ Sci Technol ; 53(20): 12007-12017, 2019 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-31549828

RESUMO

The implementation of chlorine disinfection in low-income countries reduces the risk of waterborne illness but initiates exposure to disinfection byproducts (DBPs). Like high-income countries, low-income countries typically are adopting regulations focusing on trihalomethanes (THM4) as an indicator of overall DBP exposure. However, the use of impaired water sources can decouple the formation of THM4 from other DBP classes that are more potent toxins. The documentation of DBP species other than THM4 is rare in low-income countries, where water sources may be degraded by inadequate sanitation infrastructure and other uncontrolled wastewater discharges. We measured THM4 and 21 unregulated DBPs in tap waters and laboratory-treated source waters from two cities in northwestern India. The contribution of each DBP class to the cumulative toxicity was estimated by weighting each species by metrics of toxic potency; haloacetonitriles typically were the dominant contributor, while the contribution of THM4 was negligible. THM4 concentrations did not correlate with the total toxic potency-weighted DBP concentrations. Although THM4 rarely exceeded international guidelines, DBPs of greater toxicological concern were observed in high concentrations. The total toxic potency-weighted DBP concentrations in some waters were elevated compared to conventional drinking waters in high-income countries and more closely resembled chlorine-disinfected wastewater effluents. Artificial sweeteners confirmed widespread contamination of both surface and groundwaters by domestic sewage. The results suggest that THM4 may not be an adequate indicator of overall DBP exposure in impaired water supplies prevalent in some low-income nations.


Assuntos
Desinfetantes , Poluentes Químicos da Água , Purificação da Água , Desinfecção , Halogenação , Índia , Trialometanos
14.
Environ Res ; 177: 108618, 2019 10.
Artigo em Inglês | MEDLINE | ID: mdl-31419714

RESUMO

Well water is the primary drinking source for nearly a quarter of North Carolina residents. Many communities across the state have been concerned about their well water quality and inorganic contamination. The "Well Empowered" study worked alongside a community in Stokes County, North Carolina to measure toxic metals in their well water as well as provide and test ZeroWater® filter pitchers in homes with arsenic (As) or lead (Pb) contamination. Multiple water samples, including a First Draw sample from the kitchen tap and a sample taken directly from the well, were collected from 39 homes in Stokes County. The samples were analyzed for 17 different inorganic contaminants, including As, boron (B), Pb, and manganese (Mn), using inductively coupled plasma mass spectrometry (ICP-MS). High concentrations of Pb along with copper (Cu), cadmium (Cd), and zinc (Zn) were only found in the First Draw sample and therefore likely originate in the home plumbing system while As, iron (Fe), and Mn were consistent across all samples and therefore are present in the groundwater. The low concentrations of B (<100 parts per billion (ppb)) make it unlikely that the source of As and Mn contamination was coal ash-derived. Out of the 39 homes, four had As levels exceeding the federal standard of 10 ppb and an additional two exceeded the Pb standard of 15 ppb. These homes were provided with a ZeroWater® filter pitcher and a water sample was taken pre- and post-filtration. The ZeroWater® filter removed 99% of As and Pb from the water, dropping the levels well below the drinking water standard levels. These ZeroWater® filter pitchers, while not a permanent solution, are a low-cost option for homeowners experiencing As or Pb contamination.


Assuntos
Monitoramento Ambiental , Poluentes Químicos da Água , Poços de Água , Arsênio , Água Subterrânea , Manganês , Metais Pesados , North Carolina , Projetos Piloto
15.
Sci Total Environ ; 686: 1090-1103, 2019 Oct 10.
Artigo em Inglês | MEDLINE | ID: mdl-31200305

RESUMO

Coal combustion residuals (CCRs, also known as "coal ash") contain high concentrations of toxic and carcinogenic elements that can pose ecological and human health risks upon their release into the environment. About half of the CCRs that are generated annually in the U.S. are stored in coal ash impoundments and landfills, in most cases adjacent to coal plants and waterways. Leaking of coal ash ponds and CCR spills are major environmental concerns. One factor which may impact the safety of CCRs stored in impoundments and landfills is the storage area's predisposition to flooding. The southeastern U.S., in particular, has a large number of coal ash impoundments located in areas that are vulnerable to flooding. In order to test for the possible presence of CCR solids in lake sediments following Hurricane Florence, we analyzed the magnetic susceptibility, microscopic screening, trace element composition, and strontium isotope ratios of bottom sediments collected in 2015 and in 2018 from Sutton Lake in eastern North Carolina and compared them to a reference lake. The results suggest multiple, apparently previously unmonitored, CCR spills into Sutton Lake from adjacent CCR storage sites. The enrichment of metals in Sutton Lake sediments, particularly those with known ecological impact such as As, Se, Cu, Sb, Ni, Cd, V, and Tl, was similar to or even higher than those in stream sediments impacted by the Tennessee Valley Authority (TVA) in Kingston, Tennessee, and the Dan River, North Carolina coal ash spills, and exceeded ecological screening standards for sediments. High levels of contaminants were also found in leachates extracted from Sutton Lake sediments and co-occurring pore water, reflecting their mobilization to the ambient environment. These findings highlight the risks of large-scale unmonitored spills of coal ash solids from storage facilities following major storm events and contamination of nearby water resources throughout the southeastern U.S.

16.
Environ Sci Technol ; 52(24): 14519-14527, 2018 12 18.
Artigo em Inglês | MEDLINE | ID: mdl-30419747

RESUMO

Shale gas extraction through hydraulic fracturing and horizontal drilling is increasing in China, particularly in Sichuan Basin. Production of unconventional shale gas with minimal environmental effects requires adequate management of wastewater from flowback and produced water (FP water) that is coextracted with natural gas. Here we present, for the first time, inorganic chemistry and multiple isotope (oxygen, hydrogen, boron, strontium, radium) data for FP water from 13 shale gas wells from the Lower Silurian Longmaxi Formation in the Weiyuan gas field, as well as produced waters from 35 conventional gas wells from underlying (Sinian, Cambrian) and overlying (Permian, Triassic) formations in Sichuan Basin. The chemical and isotope data indicate that the formation waters in Sichuan Basin originated from relics of different stages of evaporated seawater modified by water-rock interactions. The FP water from shale gas wells derives from blending of injected hydraulic fracturing water and entrapped saline (Cl ∼ 50,000 mg/L) formation water. Variations in the chemistry, δ18O, δ11B, and 87Sr/86Sr of FP water over time indicate that the mixing between the two sources varies with time, with a contribution of 75% (first 6 months) to 20% (>year) of the injected hydraulic fracturing water in the blend that compose the FP water. Mass-balance calculation suggests that the returned hydraulic fracturing water consisted of 28-49% of the volume of the injected hydraulic fracturing water, about a year after the initial hydraulic fracturing. We show differential mobilization of Na, B, Sr, and Li from the shale rocks during early stages of operation, which resulted in higher Na/Cl, B/Cl, Li/Cl, and 87Sr/86Sr and lower δ11B of the FP water during early stages of FP water formation relative to the original saline formation water recorded in late stages FP water. This study provides a geochemical framework for characterization of formation waters from different geological strata, and thus the ability to distinguish between different sources of oil and gas wastewater in Sichuan Basin.


Assuntos
Poluentes Químicos da Água , China , Gás Natural , Campos de Petróleo e Gás , Águas Residuárias
17.
Sci Total Environ ; 630: 349-356, 2018 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-29482143

RESUMO

Shale gas is likely to play a major role in China's transition away from coal. In addition to technological and infrastructural constraints, the main challenges to China's sustainable shale gas development are sufficient shale gas production, water availability, and adequate wastewater management. Here we present, for the first time, actual data of shale gas production and its water footprint from the Weiyuan gas field, one of the major gas fields in Sichuan Basin. We show that shale gas production rates during the first 12 months (24 million m3 per well) are similar to gas production rates in U.S. shale basins. The amount of water used for hydraulic fracturing (34,000 m3 per well) and the volume of flowback and produced (FP) water in the first 12 months (19,800 m3 per well) in Sichuan Basin are also similar to the current water footprints of hydraulic fracturing in U.S. basins. We present salinity data of the FP water (5000 to 40,000 mgCl/L) in Sichuan Basin and the treatment operations, which include sedimentation, dilution with fresh water, and recycling of the FP water for hydraulic fracturing. We utilize the water use data, empirical decline rates of shale gas and FP water productions in Sichuan Basin to generate two prediction models for water use for hydraulic fracturing and FP water production upon achieving China's goals to generate 100 billion m3 of shale gas by 2030. The first model utilizes the current water use and FP production data, and the second assumes a yearly 5% intensification of the hydraulic fracturing process. The predicted water use for hydraulic fracturing in 2030 (50-65 million m3 per year), FP water production (50-55 million m3 per year), and fresh water dilution of FP water (25 million m3 per year) constitute a water footprint that is much smaller than current water consumption and wastewater generation for coal mining, but higher than those of conventional gas production in China. Given estimates for water availability in Sichuan Basin, our predictions suggest that water might not be a limiting factor for future large-scale shale gas development in Sichuan Basin.

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