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1.
Nanomaterials (Basel) ; 9(5)2019 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-31052363

RESUMO

Many analytical techniques have limited sensitivity to quantify multi-walled carbon nanotubes (MWCNTs) at environmentally relevant exposure concentrations in wastewaters. We found that trace metals (e.g., Y, Co, Fe) used in MWCNT synthesis correlated with MWCNT concentrations. Because of low background yttrium (Y) concentrations in wastewater, Y was used to track MWCNT removal by wastewater biomass. Transmission electron microscopy (TEM) imaging and dissolution studies indicated that the residual trace metals were strongly embedded within the MWCNTs. For our specific MWCNT, Y concentration in MWCNTs was 76 µg g-1, and single particle mode inductively coupled plasma mass spectrometry (spICP-MS) was shown viable to detect Y-associated MWCNTs. The detection limit of the specific MWCNTs was 0.82 µg L-1 using Y as a surrogate, compared with >100 µg L-1 for other techniques applied for MWCNT quantification in wastewater biomass. MWCNT removal at wastewater treatment plants (WWTPs) was assessed by dosing MWCNTs (100 µg L-1) in water containing a range of biomass concentrations obtained from wastewater return activated sludge (RAS) collected from a local WWTP. Using high volume to surface area reactors (to limit artifacts of MWCNT loss due to adsorption to vessel walls) and adding 5 g L-1 of total suspended solids (TSS) of RAS (3-h mixing) reduced the MWCNT concentrations from 100 µg L-1 to 2 µg L-1. The results provide an environmentally relevant insight into the fate of MWCNTs across their end of life cycle and aid in regulatory permits that require estimates of engineered nanomaterial removal at WWTPs upon accidental release into sewers from manufacturing facilities.

2.
Environ Sci Technol ; 53(12): 7114-7125, 2019 06 18.
Artigo em Inglês | MEDLINE | ID: mdl-31132247

RESUMO

Cookstoves emit many pollutants that are harmful to human health and the environment. However, most of the existing scientific literature focuses on fine particulate matter (PM2.5) and carbon monoxide (CO). We present an extensive data set of speciated air pollution emissions from wood, charcoal, kerosene, and liquefied petroleum gas (LPG) cookstoves. One-hundred and twenty gas- and particle-phase constituents-including organic carbon, elemental carbon (EC), ultrafine particles (10-100 nm), inorganic ions, carbohydrates, and volatile/semivolatile organic compounds (e.g., alkanes, alkenes, alkynes, aromatics, carbonyls, and polycyclic aromatic hydrocarbons (PAHs))-were measured in the exhaust from 26 stove/fuel combinations. We find that improved biomass stoves tend to reduce PM2.5 emissions; however, certain design features (e.g., insulation or a fan) tend to increase relative levels of other coemitted pollutants (e.g., EC ultrafine particles, carbonyls, or PAHs, depending on stove type). In contrast, the pressurized kerosene and LPG stoves reduced all pollutants relative to a traditional three-stone fire (≥93% and ≥79%, respectively). Finally, we find that PM2.5 and CO are not strong predictors of coemitted pollutants, which is problematic because these pollutants may not be indicators of other cookstove smoke constituents (such as formaldehyde and acetaldehyde) that may be emitted at concentrations that are harmful to human health.


Assuntos
Poluentes Atmosféricos , Poluentes Ambientais , Biomassa , Culinária , Combustíveis Fósseis , Humanos , Material Particulado
3.
Water Res ; 150: 466-472, 2019 03 01.
Artigo em Inglês | MEDLINE | ID: mdl-30576897

RESUMO

N-nitrosodimethylamine (NDMA) is a chloramine disinfection by-product, and its formation in drinking waters can increase due to the addition of cationic polydiallyldimethylammonium chloride (polyDADMAC). PolyDADMAC is a cationic polymer added as a coagulant or coagulant aid to enhance turbidity removal during sedimentation and filtration. This paper answers two central questions to understanding the nature of the NDMA precursors in polyDADMAC. First, what is the reactivity of different molecular weight (MW) fractions of polyDADMAC with chloramines? NDMA formation potential (NDMAFP) and kinetic experiments with chloramines were conducted for non-fractionated (raw) and size-excluded fractions (<3K, 3-10K, and >10K Da.) of polyDADMAC. The lower MW fraction (<3K Da.) of polyDADMAC solutions was responsible for forming 64 ±â€¯6% of the NDMA, despite containing only 8.7 and 9.8% of the carbon or nitrogen present in the bulk polymer. The chloramine demand kinetics of the lowest MW fraction were also >2× faster than the higher MW fractions. Therefore, in a water treatment application the lower MW polyDADMAC likely contributes to most of the NDMA attributed to the use of polyDADMAC. The second question was: can 1H and 13C nuclear magnetic resonance spectroscopy (NMR) be used to characterize the molecular structures in polyDADMAC that react with chloramines? A peak for 1H NMR dimethylamine (DMA), a known low MW NDMA precursor, was found in a commercial polyDADMAC solution and decreased upon chloramination. The estimated DMA alone could not account for the observed NDMAFP, indicating the presence of other low MW precursors. Diffusion order spectroscopy (DOSY) NMR also showed multiple lower MW organics in polyDADMAC that change upon chloramination, including a 1.5× decrease in MW, suggesting chloramines cleave CC or CN bonds. These reactions may produce intermediates responsible for NDMA formation. Polymer manufacturers could use NMR to synthesize polyDADMAC with less DMA and other low MW compounds that produce NDMA upon chloramination.


Assuntos
Água Potável , Poluentes Químicos da Água , Purificação da Água , Dimetilnitrosamina , Desinfecção , Peso Molecular
4.
Nat Nanotechnol ; 13(8): 661-669, 2018 08.
Artigo em Inglês | MEDLINE | ID: mdl-30082812

RESUMO

Natural nanoparticles (NNPs) in rivers, lakes, oceans and ground water predate humans, but engineered nanoparticles (ENPs) are emerging as potential pollutants due to increasing regulatory and public perception concerns. This Review contrasts the sources, composition and potential occurrence of NNPs (for example, two-dimensional clays, multifunctional viruses and metal oxides) and ENPs in surface water, after centralized drinking water treatment, and in tap water. While analytical detection challenges exist, ENPs are currently orders of magnitude less common than NNPs in waters that flow into drinking water treatment plants. Because such plants are designed to remove small-sized NNPs, they are also very good at removing ENPs. Consequently, ENP concentrations in tap water are extremely low and pose low risk during ingestion. However, after leaving drinking water treatment plants, corrosion by-products released from distribution pipes or in-home premise plumbing can release incidental nanoparticles into tap water. The occurrence and toxicity of incidental nanoparticles, rather than ENPs, should therefore be the focus of future research.


Assuntos
Água Potável/análise , Nanopartículas/análise , Poluentes da Água/análise , Purificação da Água/métodos , Lagos/análise , Tamanho da Partícula , Rios/química
5.
Water Res ; 133: 264-271, 2018 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-29407707

RESUMO

Phosphorus (P) is an important and often limiting element in terrestrial and aquatic ecosystem. A lack of understanding of its distribution and structures in the environment limits the design of effective P mitigation and recovery approaches. Here we developed a robust method employing size exclusion chromatography (SEC) coupled to an ICP-MS to determine the molecular weight (MW) distribution of P in environmental samples. The most abundant fraction of P varied widely in different environmental samples: (i) orthophosphate was the dominant fraction (93-100%) in one lake, two aerosols and DOC isolate samples, (ii) species of 400-600 Da range were abundant (74-100%) in two surface waters, and (iii) species of 150-350 Da range were abundant in wastewater effluents. SEC-DOC of the aqueous samples using a similar SEC column showed overlapping peaks for the 400-600 Da species in two surface waters, and for >20 kDa species in the effluents, suggesting that these fractions are likely associated with organic matter. The MW resolution and performance of SEC-ICP-MS agreed well with the time integrated results obtained using conventional ultrafiltration method. Results show that SEC in combination with ICP-MS and DOC has the potential to be a powerful and easy-to-use method in identifying unknown fractions of P in the environment.


Assuntos
Fósforo/análise , Poluentes Químicos da Água/análise , Fracionamento Químico , Cromatografia em Gel , Água Doce/análise , Peso Molecular , Fósforo/química , Análise Espectral/métodos , Ultrafiltração , Águas Residuárias/análise , Poluentes Químicos da Água/química
6.
Bull Environ Contam Toxicol ; 100(1): 120-126, 2018 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-29164274

RESUMO

Single particle inductively coupled plasma mass spectrometry (spICP-MS) was used to detect Ti-containing particles in heavily-used bathing areas of a river (Salt River) and five swimming pools. Ti-containing particle concentrations in swimming pools ranged from 2.8 × 103 to 4.4 × 103 particles/mL and were an order of magnitude lower than those detected in the Salt River. Measurements from the Salt River showed an 80% increase in Ti-containing particle concentration over baseline concentration during peak recreational activity (at 16:00 h) in the river. Cloud point extraction followed by transmission electron microscopy with energy dispersive X-ray analysis confirmed presence of aggregated TiO2 particles in river samples, showing morphological similarity to particles present in an over-the-counter sunscreen product. The maximum particle mass concentration detected in a sample from the Salt River (659 ng/L) is only slightly lower than the predicted no effect concentration for TiO2 to aquatic organisms (< 1 µg/L).


Assuntos
Monitoramento Ambiental/métodos , Titânio/análise , Poluentes Químicos da Água/análise , Espectrometria de Massas/métodos , Microscopia Eletrônica de Transmissão , Rios , Análise Espectral , Protetores Solares/análise
7.
Sci Total Environ ; 584-585: 515-522, 2017 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-28129906

RESUMO

Increasing application of engineered nanomaterials (ENMs) in industry and consumer products inevitably lead to their release into and impact on aquatic environments. To characterize the NMs efficiently in surface water, a fast and simple method is needed to separate and concentrate nanomaterials from the aqueous matrix without altering their shape and size. Applying cloud-point extraction (CPE) using the surfactant Triton 114 to an array of NMs (titanium dioxide, gold, silver, and silicon dioxide) with different sizes or capping agents in nanopure water resulted in extraction efficiency of 83%-107%. Additional CPE experiments were conducted to extract NMs from surface, potable, and sewage waters, and NMs enriched in the surfactant phase were characterized using transmission electron microscopy coupled with energy dispersive x-ray spectroscopy. The most abundant nanoparticles identified in surface water were silica, titanium dioxide, and iron oxide with 4-99nm diameter. The extraction efficiencies of CPE for silicon, titanium, and iron elements from environmental water samples were 51%, 15%, and 99%, respectively. This study applied CPE with TEM to enrich and analyze popular nanoparticles such as SiO2 and TiO2 from natural waters, which has not been well addressed by previous researches. Overall, CPE coupled with transmission electron microscopy (TEM) can be an effective method to characterize NMs in aqueous water samples, and further optimization will increase the extraction efficiency of NMs in complicated surface water matrix.

8.
Atmos Pollut Res ; 8(5): 873-884, 2017 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-30505154

RESUMO

The Desert Southwest Coarse Particulate Matter Study was undertaken to further our understanding of the spatial and temporal variability and sources of fine and coarse particulate matter (PM) in rural, arid, desert environments. Sampling was conducted between February 2009 and February 2010 in Pinal County, AZ near the town of Casa Grande where PM concentrations routinely exceed the U.S. National Ambient Air Quality Standards (NAAQS) for both PM10 and PM2.5. In this desert region, exceedances of the PM10 NAAQS are dominated by high coarse particle concentrations, a common occurrence in this region of the United States. This work expands on previously published measurements of PM mass and chemistry by examining the sources of fine and coarse particles and the relative contribution of each to ambient PM mass concentrations using the positive matrix factorization receptor model (Clements et al., 2014). Coarse particles within the region were apportioned to nine sources including primary biological aerosol particles (PBAPs - 25%), crustal material (20%), re-entrained road dust (11%), feedlot (11% at the site closest to a cattle feedlot), secondary particles (10%), boron-rich crustal material (9%), and transported soil (6%), with minor contributions from ammonium nitrate, and salt (considered to be NaCl). Fine particles within the region were apportioned to six sources including motor vehicles (37%), road dust (29%), lead-rich (10%), with minor contributions from brake wear, crustal material, and salt. These results can help guide local air pollution improvement strategies designed to reduce levels of PM to below the NAAQS.

9.
J Hazard Mater ; 323(Pt A): 18-25, 2017 Feb 05.
Artigo em Inglês | MEDLINE | ID: mdl-27229910

RESUMO

N-Nitrosodimethylamine (NDMA) is carcinogenic in rodents and occurs in chloraminated drinking water and wastewater effluents. NDMA forms via reactions between chloramines and mostly unidentified, N-containing organic matter. We developed a mass spectrometry technique to identify NDMA precursors by analyzing 25 model compounds with LC/QTOF-MS. We searched isolates of 11 drinking water sources and 1 wastewater using a custom MATLAB® program and extracted ion chromatograms for two fragmentation patterns that were specific to the model compounds. Once a diagnostic fragment was discovered, we conducted MS/MS during a subsequent injection to confirm the precursor ion. Using non-target searches and two diagnostic fragmentation patterns, we discovered 158 potential NDMA precursors. Of these, 16 were identified using accurate mass combined with fragment and retention time matches of analytical standards when available. Five of these sixteen NDMA precursors were previously unidentified in the literature, three of which were metabolites of pharmaceuticals. Except methadone, the newly identified precursors all had NDMA molar yields of less than 5%, indicating that NDMA formation could be additive from multiple compounds, each with low yield. We demonstrate that the method is applicable to other disinfection by-product precursors by predicting and verifying the fragmentation patterns for one nitrosodiethylamine precursor.


Assuntos
Fracionamento Químico/métodos , Dimetilnitrosamina/análise , Água Potável/análise , Poluentes Químicos da Água/análise , Abastecimento de Água/normas , Fracionamento Químico/instrumentação , Cromatografia Líquida , Espectrometria de Massas
10.
J Sep Sci ; 39(14): 2796-805, 2016 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-27184503

RESUMO

#x02010;Nitrosodimethylamine is mutagenic in rodents, a drinking water contaminant, and a byproduct of drinking water disinfection by chloramination. Nitrosodimethylamine precursor identification leads to their control and improved understanding of nitrosodimethylamine formation during chloramination. Mass balances on nitrosodimethylamine precursors were evaluated across solid-phase extraction cartridges and in eluates to select the best combination of solid-phase media and eluent that maximized recovery of nitrosodimethylamine precursors into a solvent amenable to time-of-flight mass spectrometry analysis. After reviewing literature and comparing various solid-phase cartridges and eluent combinations, a method was obtained to efficiently recover nitrosodimethylamine precursors. The approach with the greatest recoveries of nitrosodimethylamine precursors involved cation exchange resin loaded with water samples at pH 3 and eluted with 5% NH4 OH in methanol. This indicated that nitrosodimethylamine precursors are amines that protonate at low pH and deprotonate at high pH. Quaternary amines were irreversibly sorbed to the cation exchange cartridge and did not account for a large fraction of precursors. Overall, a median recovery of 82% for nitrosodimethylamine precursors was achieved from 11 surface waters and one wastewater. Applying this method allowed discovery of methadone as a new nitrosodimethylamine precursor in wastewater effluent and drinking water treatment plant intakes.


Assuntos
Dimetilnitrosamina/análise , Extração em Fase Sólida , Adsorção , Estrutura Molecular , Propriedades de Superfície
11.
Environ Sci Technol ; 50(7): 4018-26, 2016 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-26927927

RESUMO

For textiles containing nanosilver, we assessed benefit (antimicrobial efficacy) in parallel with potential to release nanosilver (impact) during multiple life cycle stages. The silver loading and method of silver attachment to the textile highly influenced the silver release during washing. Multiple sequential simulated household washing experiments for fabric swatches in deionized water with or without detergent showed a range of silver release. The toxicity of washing experiment supernatants to zebrafish (Danio rerio) embryos was negligible, with the exception of the very highest Ag releases (∼1 mg/L Ag). In fact, toxicity tests indicated that residual detergent exhibited greater adverse response than the released silver. Although washing the fabrics did release silver, it did not affect their antimicrobial efficacy, as demonstrated by >99.9% inhibition of E. coli growth on the textiles, even for textiles that retained as little as 2 µg/g Ag after washing. This suggests that very little nanosilver is required to control bacterial growth in textiles. Visible light irradiation of the fabrics reduced the extent of Ag release for textiles during subsequent washings. End-of-life experiments using simulated landfill conditions showed that silver remaining on the textile is likely to continue leaching from textiles after disposal in a landfill.


Assuntos
Anti-Infecciosos/farmacologia , Meio Ambiente , Nanopartículas Metálicas/toxicidade , Prata/farmacologia , Têxteis , Poluentes Químicos da Água/toxicidade , Animais , Detergentes/farmacologia , Embrião não Mamífero/efeitos dos fármacos , Escherichia coli/efeitos dos fármacos , Luz , Fatores de Tempo , Peixe-Zebra/embriologia
12.
Sci Total Environ ; 565: 902-912, 2016 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-26874640

RESUMO

There is increasing recognition of the importance of transformations in nanomaterials across their lifecycle, yet few quantitative examples exist. We examined food-grade silicon dioxide (SiO2) nanomaterials from its source (bulk material providers), occurrence in food products, impacts on human gastrointestinal tract during consumption, and fate at wastewater treatment plants. Based upon XRD, XPS and TEM analysis, pure SiO2 present in multiple food-grade stock SiO2 exhibited consistent morphologies as agglomerates, ranging in size from below 100nm to >500nm, with all primary particle size in the range of 9-26nm and were most likely amorphous SiO2 based upon high resolution TEM. Ten of 14 targeted foods purchased in the USA contained SiO2 of the same morphology and size as the pristine bulk food-grade SiO2, at levels of 2 to 200mg Si per serving size. A dissolution study of pristine SiO2 showed up to 7% of the dissolution of the silica, but the un-dissolved SiO2 maintained the same morphology as the pristine SiO2. Across a realistic exposure range, pristine SiO2 exhibited adverse dose-response relationships on a cell model (microvilli) of the human gastro-intestinal tract, association onto microvilli and evidence that SiO2 lead to production of reactive oxygen species (ROS). We also observed accumulation of amorphous nano-SiO2 on bioflocs in tests using lab-cultured activated sludge and sewage sludges from a full-scale wastewater treatment plant (WWTP). Nano-scale SiO2 of the same size and morphology as pristine food-grade SiO2 was observed in raw sewage at a WWTP, but we identified non-agglomerated individual SiO2 particles with an average diameter of 21.5±4.7nm in treated effluent from the WWTP. This study demonstrates an approach to track nanomaterials from source-to-sink and establishes a baseline occurrence of nano-scale SiO2 in foods and WWTPs.


Assuntos
Análise de Alimentos , Trato Gastrointestinal/metabolismo , Produtos Domésticos/análise , Nanoestruturas/análise , Nanoestruturas/química , Dióxido de Silício/análise , Dióxido de Silício/química , Humanos , Pós/química
13.
Environ Sci Technol ; 49(12): 7179-87, 2015 Jun 16.
Artigo em Inglês | MEDLINE | ID: mdl-26000788

RESUMO

Iron is a limiting nutrient in about half of the world's oceans, and its most significant source is atmospheric deposition. To understand the pathways of iron solubilization during atmospheric transport, we exposed size segregated simulated marine aerosols to 5 ppm sulfur dioxide at arid (23 ± 1% relative humidity, RH) and marine (98 ± 1% RH) conditions. Relative iron solubility increased as the particle size decreased for goethite and hematite, while for magnetite, the relative solubility was similar for all of the fine size fractions (2.5-0.25 µm) investigated but higher than the coarse size fraction (10-2.5 µm). Goethite and hematite showed increased solubility at arid RH, but no difference (p > 0.05) was observed between the two humidity levels for magnetite. There was no correlation between iron solubility and exposure to SO2 in any mineral for any size fraction. X-ray absorption near edge structure (XANES) measurements showed no change in iron speciation [Fe(II) and Fe(III)] in any minerals following SO2 exposure. SEM-EDS measurements of SO2-exposed goethite revealed small amounts of sulfur uptake on the samples; however, the incorporated sulfur did not affect iron solubility. Our results show that although sulfur is incorporated into particles via gas-phase processes, changes in iron solubility also depend on other species in the aerosol.


Assuntos
Aerossóis/química , Atmosfera/química , Umidade , Ferro/química , Tamanho da Partícula , Água do Mar/química , Dióxido de Enxofre/química , Compostos Férricos/química , Óxido Ferroso-Férrico/química , Compostos de Ferro/química , Microscopia Eletrônica de Varredura , Minerais/química , Solubilidade , Espectroscopia por Absorção de Raios X
14.
Environ Sci Technol ; 49(16): 9479-88, 2015 Aug 18.
Artigo em Inglês | MEDLINE | ID: mdl-25581264

RESUMO

U.S. sewage sludges were analyzed for 58 regulated and nonregulated elements by ICP-MS and electron microscopy to explore opportunities for removal and recovery. Sludge/water distribution coefficients (KD, L/kg dry weight) spanned 5 orders of magnitude, indicating significant metal accumulation in biosolids. Rare-earth elements and minor metals (Y, La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu) detected in sludges showed enrichment factors (EFs) near unity, suggesting dust or soils as likely dominant sources. In contrast, most platinum group elements (i.e., Ru, Rh, Pd, Pt) showed high EF and KD values, indicating anthropogenic sources. Numerous metallic and metal oxide colloids (<100-500 nm diameter) were detected; the morphology of abundant aggregates of primary particles measuring <100 nm provided clues to their origin. For a community of 1 million people, metals in biosolids were valued at up to US$13 million annually. A model incorporating a parameter (KD × EF × $Value) to capture the relative potential for economic value from biosolids revealed the identity of the 13 most lucrative elements (Ag, Cu, Au, P, Fe, Pd, Mn, Zn, Ir, Al, Cd, Ti, Ga, and Cr) with a combined value of US $280/ton of sludge.


Assuntos
Metais/análise , Esgotos/química , Águas Residuárias/química , Purificação da Água/métodos , Arizona , Biomassa , Coloides/química , Microscopia Eletrônica de Varredura , Material Particulado/química , Espectrofotometria Atômica , Estados Unidos , United States Environmental Protection Agency
15.
Environ Sci Technol ; 48(17): 10291-300, 2014 Sep 02.
Artigo em Inglês | MEDLINE | ID: mdl-25122540

RESUMO

The quantification and characterization of natural, engineered, and incidental nano- to micro-size particles are beneficial to assessing a nanomaterial's performance in manufacturing, their fate and transport in the environment, and their potential risk to human health. Single particle inductively coupled plasma mass spectrometry (spICP-MS) can sensitively quantify the amount and size distribution of metallic nanoparticles suspended in aqueous matrices. To accurately obtain the nanoparticle size distribution, it is critical to have knowledge of the size detection limit (denoted as Dmin) using spICP-MS for a wide range of elements (other than a few available assessed ones) that have been or will be synthesized into engineered nanoparticles. Herein is described a method to estimate the size detection limit using spICP-MS and then apply it to nanoparticles composed of 40 different elements. The calculated Dmin values correspond well for a few of the elements with their detectable sizes that are available in the literature. Assuming each nanoparticle sample is composed of one element, Dmin values vary substantially among the 40 elements: Ta, U, Ir, Rh, Th, Ce, and Hf showed the lowest Dmin values, ≤10 nm; Bi, W, In, Pb, Pt, Ag, Au, Tl, Pd, Y, Ru, Cd, and Sb had Dmin in the range of 11-20 nm; Dmin values of Co, Sr, Sn, Zr, Ba, Te, Mo, Ni, V, Cu, Cr, Mg, Zn, Fe, Al, Li, and Ti were located at 21-80 nm; and Se, Ca, and Si showed high Dmin values, greater than 200 nm. A range of parameters that influence the Dmin, such as instrument sensitivity, nanoparticle density, and background noise, is demonstrated. It is observed that, when the background noise is low, the instrument sensitivity and nanoparticle density dominate the Dmin significantly. Approaches for reducing the Dmin, e.g., collision cell technology (CCT) and analyte isotope selection, are also discussed. To validate the Dmin estimation approach, size distributions for three engineered nanoparticle samples were obtained using spICP-MS. The use of this methodology confirms that the observed minimum detectable sizes are consistent with the calculated Dmin values. Overall, this work identifies the elements and nanoparticles to which current spICP-MS approaches can be applied, in order to enable quantification of very small nanoparticles at low concentrations in aqueous media.


Assuntos
Elementos , Limite de Detecção , Nanopartículas/química , Tamanho da Partícula , Espectrofotometria Atômica/métodos , Meio Ambiente , Humanos , Nanotecnologia , Rios/química , Eliminação de Resíduos Líquidos , Águas Residuárias/química , Água/química
16.
Environ Sci Technol ; 48(11): 6391-400, 2014 Jun 03.
Artigo em Inglês | MEDLINE | ID: mdl-24754874

RESUMO

Titanium dioxide (TiO2) is widely used in food products, which will eventually enter wastewater treatment plants and terrestrial or aquatic environments, yet little is known about the fraction of this TiO2 that is nanoscale, or the physical and chemical properties of TiO2 that influence its human and environmental fate or toxicity. Instead of analyzing TiO2 properties in complex food or environmental samples, we procured samples of food-grade TiO2 obtained from global food suppliers and then, using spectroscopic and other analytical techniques, quantified several parameters (elemental composition, crystal structure, size, and surface composition) that are reported to influence environmental fate and toxicity. Another sample of nano-TiO2 that is generally sold for catalytic applications (P25) and widely used in toxicity studies, was analyzed for comparison. Food-grade and P25 TiO2 are engineered products, frequently synthesized from purified titanium precursors, and not milled from bulk scale minerals. Nanosized materials were present in all of the food-grade TiO2 samples, and transmission electron microscopy showed that samples 1-5 contained 35, 23, 21, 17, and 19% of nanosized primary particles (<100 nm in diameter) by number, respectively (all primary P25 particles were <100 nm in diameter). Both types of TiO2 aggregated in water with an average hydrodynamic diameter of >100 nm. Food-grade samples contained phosphorus (P), with concentrations ranging from 0.5 to 1.8 mg of P/g of TiO2. The phosphorus content of P25 was below inductively coupled plasma mass spectrometry detection limits. Presumably because of a P-based coating detected by X-ray photoelectron spectroscopy, the ζ potential of the food-grade TiO2 suspension in deionized water ranged from -10 to -45 mV around pH 7, and the iso-electric point for food-grade TiO2 (

Assuntos
Poluentes Ambientais/química , Indústria Alimentícia , Nanopartículas Metálicas/química , Titânio/química
17.
Environ Pollut ; 185: 107-15, 2014 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-24246781

RESUMO

Constructed wetlands remove trace organic contaminants via synergistic processes involving plant biomass that include hydrolysis, volatilization, sorption, biodegradation, and photolysis. Wetland design conditions, such as hydraulic loading rates (HLRs) and carbon loading rates (CLRs), influence these processes. Contaminant of emerging concern (CEC) removal by wetland plants was investigated at varying HLRs and CLRs. Rate constants and parameters obtained from batch-scale studies were used in a mechanistic model to evaluate the effect of these two loading rates on CEC removal. CLR significantly influenced CEC removal when wetlands were operated at HLR >5 cm/d. High values of CLR increased removal of estradiol and carbamazepine but lowered that of testosterone and atrazine. Without increasing the cumulative HLR, operating two wetlands in series with varying CLRs could be a way to improve CEC removal.


Assuntos
Carbono/análise , Recuperação e Remediação Ambiental/métodos , Poluentes Químicos da Água/análise , Áreas Alagadas , Biodegradação Ambiental , Biomassa , Hidrodinâmica , Plantas
18.
ACS Nano ; 7(10): 8849-56, 2013 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-23992048

RESUMO

Extraction of carbon nanotubes (CNTs) from biological matrices such as rat lung tissue is integral to developing a quantification method for evaluating the environmental and human health exposure and toxicity of CNTs. The ability of various chemical treatment methods, including Solvable (2.5% sodium hydroxide/surfactant mixture), ammonium hydroxide, nitric acid, sulfuric acid, hydrochloric acid, hydrofluoric acid, hydrogen peroxide, and proteinase K, to extract CNTs from rat lung tissue was evaluated. CNTs were quantified using programmed thermal analysis (PTA). Two CNTs were used to represent the lower (500 °C) and upper (800 °C) PTA limit of CNT thermal stability. The recovery efficiency of each of the eight chemical reagents evaluated was found to depend on the ability to (1) minimize oxidation of CNTs, (2) remove interfering background carbon from the rat lung tissue, and (3) separate the solid-phase CNTs from the liquid-phase dissolved tissue via centrifugation. A two-step extraction method using Solvable and proteinase K emerged as the optimal approach, enabling a recovery of 98 ± 15% of a 2.9 ± 0.19 µg CNT loading that was spiked into whole rat lungs. Due to its high yield and applicability to low organ burdens of nanomaterials, this extraction method is particularly well suited for in vivo studies to quantify clearance rates and retained CNTs in lungs and other organs.


Assuntos
Pulmão/metabolismo , Nanotubos de Carbono , Animais , Ratos , Análise Espectral Raman
19.
J Air Waste Manag Assoc ; 63(7): 764-72, 2013 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-23926846

RESUMO

UNLABELLED: A year-long study was conducted in Pinal County, AZ, to characterize coarse (2.5 - 10 microm aerodynamic diameter, AD) and fine (< 2.5 microm AD) particulate matter (PMc and PMf, respectively) to further understand spatial and temporal variations in ambient PM concentrations and composition in rural, arid environments. Measurements of PMc and PMf mass, ions, elements, and carbon concentrations at one-in-six day resolution were obtained at three sites within the region. Results from the summer of 2009 and specifically the local monsoon period are presented. The summer monsoon season (July - September) and associated rain and/or high wind events, has historically had the largest number of PM10 NAAQS exceedances within a year. Rain events served to clean the atmosphere, decreasing PMc concentrations resulting in a more uniform spatial gradient among the sites. The monsoon period also is characterized by high wind events, increasing PMc mass concentrations, possibly due to increased local wind-driven soil erosion or transport. Two PM10 NAAQS exceedances at the urban monitoring site were explained by high wind events and can likely be excluded from PM10 compliance calculations as exceptional events. At the more rural Cowtown site, PM10 NAAQS exceedances were more frequent, likely due to the impact from local dust sources. PM mass concentrations at the Cowtown site were typically higher than at the Pinal County Housing and Casa Grande sites. Crustal material was equal to 52-63% of the PMc mass concentration on average. High concentrations of phosphate and organic carbon found at the rural Cowtown were associated with local cattle feeding operations. A relatively high correlation between PMc and PMf (R2 = 0.63) indicated that the lower tail of the coarse particle fraction often impacts the fine particle fraction, increasing the PMf concentrations. Therefore, reductions in PMc sources will likely also reduce PMf concentrations, which also are near the value of the 24-hr PM2.5 NAAQS. IMPLICATIONS: In the desert southwest, summer monsoons are often associated with above average PM10 (< 10 microm AD) mass concentrations. Competing influences of monsoon rain and wind events showed that rain suppresses ambient concentrations while high wind increase them. In this region, the PMc fraction dominates PM10 and crustal sources contribute 52-63% to local PMc mass concentrations on average. Cattle feedlot emissions are also an important source and a unique chemical signature was identified for this source. Observations suggest monsoon wind events alone cannot explain PM10 NAAQS exceedances, thus requiring these values to remain in compliance calculations rather than being removed as exceptional wind events.


Assuntos
Poluentes Atmosféricos/análise , Material Particulado/análise , Arizona , Cromatografia por Troca Iônica , Monitoramento Ambiental , Espectrometria de Massas , Tamanho da Partícula , Chuva , Estações do Ano , Tempo (Meteorologia) , Vento
20.
J Air Waste Manag Assoc ; 63(1): 20-6, 2013 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-23447861

RESUMO

UNLABELLED: The emission of particulate matter (PM10 and PM2.5) and ammonia (NH3) by aeration processes at wastewater treatment plants (WWTPs) with and without odor control units was examined. Local concentrations of PM2.5, PM10, and NH3 at the aeration basins were within urban ranges. Emission fluxes of NH3 and PM2.5 for a medium-sized WWTP were determined to be 136 g day(-1) and 43 g day(-1), respectively, which are not substantial emission fluxes for urban environments. Odor control treatment using a granulated activated carbon bed reduced aerosol and NH3 emissions substantially. Detection of sterols, in particular the fecal sterol campesterol, in the PM clearly demonstrates aerosolization of wastewater components in the aeration process. The presence of campesterol in PM2.5 at a remote fenceline location in a WWTP facility illustrates that wastewater components are aerosolized in the fine PM fraction and transported beyond the facilities. IMPLICATIONS: Wastewater treatment plants are potential emission sources of particulate matter and gases. This study characterized particulate matter emissions from aeration basins and quantified emissions fluxes of particulate matter and NH3. While fine and coarse particles as well as NH3 are being emitted, the overall emissions are small compared to other urban sources. However, fecal steroid presence in particles at the fence of a treatment plant demonstrates that wastewater material is getting aerosolized and transported beyond the facilities.


Assuntos
Aerossóis/análise , Amônia/análise , Material Particulado/análise , Esgotos , Carvão Vegetal , Odorantes/prevenção & controle , Compostos Orgânicos/análise , Esteróis/análise
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