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1.
Environ Monit Assess ; 193(11): 699, 2021 Oct 07.
Artículo en Inglés | MEDLINE | ID: mdl-34622348

RESUMEN

In response to the Minamata Convention on Mercury, international organizations, governments, nonprofit organizations, and other institutions as well as individuals have worked to promote the development and implementation of safe and environmentally healthy practices, processes, and products. It is expected that the accumulation of mercury in the natural environment will decrease in volume each year. However, even after Hg ceases to be used, the Hg already accumulated in forests will continue to pose an ecological risk. Forest fires are serious events, partly because they release accumulated Hg from the environment. In this study, the effects of forest fires on the accumulation and chemical species of Hg in soil, related to the mobilization of Hg, were investigated. The research was conducted in secondary forests located near artisanal small-scale gold mining sites, where Hg is used for the amalgamation of gold in Camarines Norte, Philippines. The results showed that the original Hg accumulation level in the burned forest was not as high as that in the control forest, and that burn severity might have affected only the surface soil (0-5 cm). However, the proportion of water-soluble Hg, which was derived from ash, was increased by fire. Therefore, it is suggested that forest fires not only increase the release of Hg into the atmosphere but also increase the outflow risk to the aquatic system through rainfall.


Asunto(s)
Mercurio , Incendios Forestales , Monitoreo del Ambiente , Oro , Humanos , Mercurio/análisis , Minería , Suelo
2.
Anal Sci ; 36(11): 1393-1399, 2020 Nov 10.
Artículo en Inglés | MEDLINE | ID: mdl-32713901

RESUMEN

An ultra-sensitive analytical system that can determine the concentration of N-nitrosamines at the ng/L level without preconcentration was used to investigate the contamination, decomposition, and formation of N-nitrosodimethylamine (NDMA) and other N-nitrosamines in water samples during general analytical procedures. A preliminary experiment was performed to estimate the NDMA concentrations in ambient air. Since the air samples contained NDMA at concentrations in the range of 2.0 - 10.7 ng/m3, ambient air was identified as the source of NDMA contamination in water samples. We directly confirmed that the concentration of aqueous 10-ng/L NDMA samples stored in clear glass bottles decreased upon exposure to sunlight. Thus, to maintain the N-nitrosamine concentration, such samples must always be protected from sunlight during sampling. The existence of N-nitrosamines in experimental reagents, such as ranitidine and sodium hypochlorite solutions, was also confirmed, as was the formation of NDMA on an activated carbon solid-phase extraction cartridge.

3.
Chemosphere ; 247: 125827, 2020 May.
Artículo en Inglés | MEDLINE | ID: mdl-31955040

RESUMEN

Total-Hg (T-Hg) and methylmercury (MeHg) concentrations in rice grains were measured to understand the MeHg accumulation process. Rice plants were cultivated in Hg2+-spiked non-contaminated soils in experimental pots at three different places. Although soil MeHg concentrations in the pots changed significantly and individually during the rice-growing season, T-Hg concentration of brown rice grain was high at high soil MeHg concentration. In addition, there was no significant variation in T-Hg concentration in brown rice grains from individual panicles or among panicles obtained from the same pot, although the period of growth for each panicle was different. The highest T-Hg concentration of brown rice grains recorded for a panicle was 1.4 ± 0.1 mg kg-1 (n = 8), and the corresponding MeHg ratio was 76%. In addition, the T-Hg and MeHg concentrations in various parts of the brown rice grain-white rice (endosperm), bran, and embryo-were measured. Among the parts of the brown rice grain, the embryo had the highest Hg concentration. Furthermore, Hg concentration in the grain was constant during grain filling. These findings suggest that MeHg formed in soil accumulates in the rice plant during growth and is supplied to the rice grains continuously for the entire duration of the grain development period.


Asunto(s)
Compuestos de Metilmercurio/análisis , Oryza/metabolismo , Contaminantes del Suelo/metabolismo , Suelo/química , Grano Comestible/química , Grano Comestible/metabolismo , Monitoreo del Ambiente , Mercurio/análisis , Mercurio/metabolismo , Compuestos de Metilmercurio/metabolismo , Oryza/química , Contaminantes del Suelo/análisis
4.
Environ Res ; 180: 108668, 2020 01.
Artículo en Inglés | MEDLINE | ID: mdl-31648069

RESUMEN

In the latter half of the 1950s, a large amount of methylmercury (MeHg) was discharged directly into Minamata Bay, Japan by a chemical factory, resulting in the contamination of the fish and shellfish. Ultimately, an outbreak of MeHg intoxication, called Minamata disease, occurred. From 1977 to 1988, the Kumamoto Prefectural Government dredged and transferred sediments exceeding 25 µg/g of total mercury (THg, dry basis) into a strictly segregated area of the bay near the wastewater outlet, then this area was landfilled. We conducted analyses of the mercury speciation in preserved Minamata Bay sludge samples (collected from inside of the bay prior to the termination of the remediation project; n=4) and recent Minamata Bay sediments (collected outside the dredging area of the bay; n=5) to evaluate the potential risk of the sludge/sediment leakage from the reclaimed land to the Minamata Bay. Median THg (dry basis) concentrations were 241 µg/g for the preserved sludge, 6.1 µg/g for the recent Minamata Bay sediments, and 0.18 µg/g for a single control sample; median MeHg concentrations (percentage of MeHg in THg) were 108 ng/g (0.031%), 3.7 ng/g (0.12%), and 0.71 ng/g (0.41%), respectively. In all the samples, the MeHg% decreased exponentially with increasing THg concentration. The extractability of THg from each sample into seawater was shown to be much lower than that of MeHg. The extracted MeHg was 0.86% for the preserved sludge, 4.57% for the recent Minamata Bay sediments, and 7.89% for the control. The predominant chemical form of mercury in the preserved sludge containing the highest THg concentration was found to be stable ß-mercury sulfide (HgS) based on transmission electron microscopy linked with energy-dispersive X-ray spectroscopy (TEM-EDX) and X-ray absorption fine structure (XAFS) analyses.


Asunto(s)
Mercurio , Compuestos de Metilmercurio , Contaminantes Químicos del Agua , Animales , Bahías , Monitoreo del Ambiente , Japón , Aguas del Alcantarillado
5.
Chemistry ; 25(59): 13500-13503, 2019 Oct 22.
Artículo en Inglés | MEDLINE | ID: mdl-31454440

RESUMEN

In order to investigate the proton solvation state in protic ionic liquids (PILs), ten acid dissociation enthalpies and entropies of eight compounds were determined in ethylammonium nitrate (EAN). Regardless of the nature of the compound, 24 kJ mol-1 larger enthalpy and 65 J mol-1 K-1 larger entropy than those in water, respectively, were observed. These values were reasonably explained by the differences in the proton solvation structure in EAN and water. Namely, protons in EAN exist as HNO3 , having a higher reaction energy than that of H3 O+ in water, undergo entropic stabilization as a result of the less-structured solvation. As such, the entropic effect of the proton solvation structure on the acid-base property is possibly applicable to all PILs. In addition, based on these proton thermodynamics, enthalpy and entropy windows were proposed as a novel perspective for the characterization of solvents. Use of this concept enabled the visualization of similarities and differences between EAN and water.

6.
7.
Environ Sci Pollut Res Int ; 26(24): 25262-25274, 2019 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-31256393

RESUMEN

To estimate the impact of mercury discharged from artisanal and small-scale gold mining (ASGM) activity, variations in the concentrations of elemental mercury (Hg0), mercury ion (Hg2+), particulate mercury (P-Hg), and total mercury in filtered river water (FT-Hg) were investigated from sampling locations extending from 10 km upstream to 30 km downstream of ASGM operations in West Java, Indonesia. The average of the annual concentrations at the ASGM site from 2013 to 2017 were 0.14-0.85 µg L-1, 0.27-12.9 µg L-1, 4.3-49.5 µg L-1, and 1.2-12.5 µg L-1 for Hg0, Hg2+, P-Hg, and FT-Hg, respectively. The concentration of mercury species decreased as the distance from the ASGM site increased, while the ratio of P-Hg increased towards the lower reaches of the river system, with the percentage of P-Hg estimated at 90% of Hg at the sample location furthest downstream. A high mercury concentration of 600 mg kg-1 was observed for suspended particulate matter (SPM) at the ASGM site. The SPM maintained a high concentration of mercury, even in the downstream area. In the annual variations of the mercury species from 2013 to 2017, FT-Hg and P-Hg concentrations tended to decrease from 2016, which suggested a decline of ASGM activity in this area. However, SPM and river sediment showed no apparent changes in their mercury concentrations over this period, indicating that the contamination in the river system is persistent and does not recover quickly.


Asunto(s)
Monitoreo del Ambiente , Mercurio/análisis , Minería , Contaminantes Químicos del Agua/análisis , Oro , Indonesia , Ríos
8.
J Phys Chem B ; 122(46): 10593-10599, 2018 11 21.
Artículo en Inglés | MEDLINE | ID: mdl-30351941

RESUMEN

We selected and validated the pH values of three standard materials that function in the protic ionic liquid, ethylammonium nitrate (EAN). The pH values of 0.05 mol kg-1 phthalate, oxalate, and phosphate buffers were 4.93 (0.04), 2.12 (0.04), and 7.13 (0.06), respectively (the values in the parentheses denote the standard deviation). Because the pH of EAN ranges from 0 to 10, with a neutral pH of 5, these materials are usable as acidic, basic, or neutral standards. The standard electrode potential of silver-silver chloride in EAN was 127.2 (1.7) mV. The activity coefficients of hydrogen and chloride ions remain equal to unity in EAN of a wide concentration range, which indicates that the effective ionic strength is independent of the solute ion concentration. In addition, the estimated value of the transfer activity coefficient of chloride ion suggests a weaker solvation in EAN compared with water in spite of a ubiquitous cation (C2H5NH3+). These behaviors of ions in EAN can be explained by the unique solvation in the ionic liquid through direct ion-ion electrostatic interactions.

9.
J Phys Chem B ; 121(41): 9659-9665, 2017 10 19.
Artículo en Inglés | MEDLINE | ID: mdl-28937759

RESUMEN

Metal ions in ionic liquids are laid under an unprecedented reaction field. In order to assess the reaction thermodynamics of metal ions in such a situation, Cu2+-chloro complex formation was examined with spectroscopic and calorimetric titrations in an ionic liquid, 1-buthyl-3-methylimidazolium trifluoromethanesulfonate (C4mimTfO). In addition, the effect of the structure of the solvated complexes on the complexation mechanism was investigated with the aid of DFT calculations. Chloro complexation successively proceeded and finally provided a [CuCl4]2- species, which is also the final product in conventional molecular solvents. Their stability constants were comparable to those in molecular solvents. Interestingly, in spite of the charged solvent in the ionic liquid, the entropy profile of the complexation resembled that in the conventional molecular liquids. This indicates that the entropy gain of the released solvent species from the complexes is the main driving force of the chloro complexation in the ionic liquid. In contrast, unlike the major molecular solvents, the total coordination number of Cu2+ is saturated to 4 in the ionic liquid, and the Cl- complexation tends to be accompanied by a 1:1 exchange of the solvent TfO- from the complex. In addition, this ligand exchange was almost athermal. This possibly indicates that the coordination number is dominated by the electrostatic hindrance among the ligands including the solvent ions in the primary coordination sphere.

10.
Chemosphere ; 184: 244-252, 2017 Oct.
Artículo en Inglés | MEDLINE | ID: mdl-28601006

RESUMEN

The distributions of the total mercury (T-Hg), methylmercury (MeHg), and ethylmercury (EtHg) concentrations in soil and their relationship to chemical composition of the soil and total organic carbon content (TOC, %) were investigated. Core samples were collected from hill slope on the right and left riverbanks of the Idrija River. Former smelting plant is located on the right bank. The T-Hg average in each of the core samples ranged from 0.25 to 1650 mg kg-1. The vertical T-Hg variations in the samples from the left bank showed no significant change with depth. Conversely, the T-Hg varied with depth, with the surface, or layers several centimeters from the surface, tending to show the highest values in the samples from the right bank. Since the right and left bank soils have different chemical compositions, different pathways of mercury delivery into soils were suggested. The MeHg and EtHg concentrations ranged from n.d. (not detected) to 444 µg kg-1 and n.d. to 17.4 µg kg-1, respectively. The vertical variations of MeHg and EtHg were similar to those of TOC, except for the near-surface layers containing TOC greater than 20%. These results suggest that the decomposition of organic matter is closely related to organic mercury formation.


Asunto(s)
Monitoreo del Ambiente , Mercurio/análisis , Minería , Contaminantes del Suelo/análisis , Compuestos de Metilmercurio/análisis , Ríos/química , Eslovenia , Suelo/química
11.
Chemosphere ; 173: 380-386, 2017 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-28129615

RESUMEN

The separate influences of drying and storage conditions on methylmercury (MeHg) concentrations in soil and sediment samples were investigated. Concentrations of MeHg and total Hg were determined in various soil and sediment samples that had been stored or dried under differing conditions. The influence of drying conditions (oven-drying (40 °C) versus freeze-drying) on MeHg concentrations in marine sediments, river sediments, soils, and paddy field soils was investigated (n = 43). The ratio of the MeHg concentration in oven-dried sub-samples divided by the concentration in freeze-dried sub-samples ranged from 0 to 336%. In order to confirm the production of MeHg during storage in some samples, Hg2+ was added at 15 mg kg-1 to a paddy soil, and the sample was then stored at 30 °C. The concentrations of MeHg at 1-h, 1-day, 4-days and 7-days after Hg2+ spiking were 2.0 ± 0.1, 13.8 ± 1.0, 36.0 ± 5.0, and 24.9 ± 1.6 µg kg-1 (n = 3), respectively. The concentration of MeHg at 4-days after Hg spiking and sterilizing (121 °C, 30 min) was 1.8 µg kg-1, similar to the original value. These results indicate that bacterial Hg methylation and MeHg demethylation occurred within days in the soil. In addition, tests of the stability of MeHg in wet and dry samples during storage were also performed. Overall, our results indicate that the best way to preserve MeHg in soil and sediment samples is to freeze the samples immediately after collection, followed subsequently by freeze-drying, grinding, homogenization, and storage of the dry material in cool, dark conditions until analysis.


Asunto(s)
Monitoreo del Ambiente/métodos , Sedimentos Geológicos/análisis , Compuestos de Metilmercurio/análisis , Contaminantes del Suelo/análisis , Contaminantes Químicos del Agua/análisis , Desecación , Liofilización , Ríos
12.
Environ Sci Pollut Res Int ; 24(3): 2643-2652, 2017 Jan.
Artículo en Inglés | MEDLINE | ID: mdl-27830415

RESUMEN

This study investigates the distribution of total mercury (T-Hg) and methylmercury (MeHg) in the soil and water around the artisanal and small-scale gold mining (ASGM) area along the Cikaniki River, West Java, Indonesia. The concentration of T-Hg and MeHg in the forest soil ranged from 0.07 to 16.7 mg kg-1 and from <0.07 to 2.0 µg kg-1, respectively, whereas it ranged from 0.40 to 24.9 mg kg-1 and from <0.07 to 56.3 µg kg-1, respectively, in the paddy field soil. In the vertical variation of the T-Hg of forest soil, the highest values were observed at the soil surface, and these values were found to decrease with increasing depth. A similar variation was observed for MeHg and total organic carbon content (TOC), and a linear relationship was observed between them. Mercury deposited on the soil surface can be trapped and retained by organic matter and subjected to methylation. The slope of the line obtained for the T-Hg vs. TOC plot became larger near the ASGM villages, implying a higher rate of mercury deposition in these areas. In contrast, the plots of MeHg vs. TOC fell along the same trend line regardless of the distance from the ASGM village. Organic carbon content may be a predominant factor in controlling MeHg formation in forest soils. The T-Hg concentration in the river water ranged from 0.40 to 9.6 µg L-1. River water used for irrigation can prove to be a source of mercury for the paddy fields. The concentrations of Hg0 and Hg2+ in river water showed similar variations as that observed for the T-Hg concentration. The highest Hg0 concentration of 3.2 µg L-1 can be attributed to the waste inflow from work sites. The presence of Hg0 in river water can become a source of mercury present in the atmosphere along the river. MeHg concentration in the river water was found to be 0.004-0.14% of T-Hg concentration, which was considerably lower than the concentrations of other Hg species. However, MeHg comprised approximately 0.2% of the T-Hg in paddy field soil. Mercury deposited from the atmosphere and the river water can be subjected to methylation. Paddy fields are very important ecosystems; therefore, the effect of MeHg on these ecosystems and human beings should be further investigated.


Asunto(s)
Mercurio/análisis , Compuestos de Metilmercurio/análisis , Minería , Atmósfera , Ecosistema , Monitoreo del Ambiente , Bosques , Agua Dulce , Oro , Humanos , Indonesia , Ríos , Suelo , Contaminantes del Suelo/análisis , Contaminantes Químicos del Agua/análisis
13.
Chemosphere ; 169: 32-39, 2017 Feb.
Artículo en Inglés | MEDLINE | ID: mdl-27855329

RESUMEN

An inter-laboratory study was conducted to compare results from different analytical methods for monomethylmercury (MeHg) concentrations in 17 soil and sediment samples. The samples were collected from mercury-contaminated areas, including Minamata Bay and Kagoshima Bay in Japan, the Idrija mercury mine in Slovenia, and an artisanal small-scale gold mining area in Indonesia. The Hg in these samples comes from several different sources: industrial waste from an acetaldehyde production facility, volcanic activity, Hg mining activity, and artisanal and small-scale gold mining activity (ASGM). MeHg concentrations in all the samples were measured in four separate laboratories, using three different determination methods: Kagoshima University (Japan), using high-performance liquid chromatography-chemiluminescence detection (HPLC-CL); National Institute for Minamata Disease (Japan), using gas chromatography-electron capture detection; and Metropolitan Council Environmental Services (USA) and Jozef Stefan Institute (Slovenia), both using alkylation-gas chromatography-atomic fluorescence spectrometry detection. The methods gave comparable MeHg results for most of the samples tested, but for some samples, the results exhibited significant variability depending on the method used. The HPLC-CL method performed poorly when applied to samples with elevated sulfur concentrations, producing MeHg concentrations that were much lower than those from the other methods. Additional analytical work demonstrated the elimination of this sulfur interference when the method was modified to bind sulfur prior to the analytical step by using Hg2+ as a masking agent. These results demonstrate the value of laboratory intercomparison exercises in contributing to the improvement of analytical methods.


Asunto(s)
Monitoreo del Ambiente/métodos , Compuestos de Metilmercurio/análisis , Contaminantes del Suelo/análisis , Fraccionamiento Químico/métodos , Oro/análisis , Indonesia , Residuos Industriales/análisis , Japón , Mercurio/análisis , Compuestos de Metilmercurio/química , Minería , Eslovenia , Suelo/química , Contaminantes del Suelo/química
14.
Anal Chim Acta ; 952: 50-58, 2017 Feb 01.
Artículo en Inglés | MEDLINE | ID: mdl-28010842

RESUMEN

A novel method for the determination of secondary amines at the nanomolar level was developed. The method is based on the nitrosation reaction of secondary amines, with the generated N-nitrosamines being measured using an HPLC separation, photochemical reaction, and chemiluminescence detection system. The efficient nitrosation of secondary amines was performed using sodium nitrite (200 mM) and acetic acid (0.8 M) at 80 °C over 60 min. Although compounds bearing OH and SH functional groups also underwent the nitrosation reaction, the sensitivity of these compounds was 1000 times lower than that of the secondary amines. Our method was applied to the determination of low molecular weight secondary amines, including dimethylamine, morpholine, pyrrolidine, diethylamine, and piperidine, giving method detection limits of 0.7 nM, 0.2 nM, 0.4 nM, 0.7 nM, and 1.5 nM, respectively. The calibration curves were linear in the range of 5-100 nM. We then applied this method for the detection and quantification of these secondary amines in samples of tap water, river water, treated wastewater, and sea water. Dimethylamine was detected at concentrations up to 15.4 nM, <0.7 nM, and 48.5 nM in tap water, river water, and treated wastewater samples, respectively, with recoveries ranging from 94 to 103%. Other amines were also detected at nanomolar levels. These results indicate that our proposed method can be applied to the analysis of secondary amines in various environmental water samples. To the best of our knowledge, the proposed method is one of the most sensitive and selective methods for the determination of secondary amines without pre-concentration steps.

15.
J Chromatogr A ; 1460: 202-6, 2016 Aug 19.
Artículo en Inglés | MEDLINE | ID: mdl-27443252

RESUMEN

As a contaminant in drinking water, N-nitrosodimethylamine (NDMA) is of great concern because of its carcinogenicity; it has been limited to levels of ng/L by regulatory bodies worldwide. Consequently, a rapid and sensitive method for monitoring NDMA in drinking water is urgently required. In this study, we report an improvement of our previously proposed HPLC-based system for NDMA determination. The approach consists of the HPLC separation of NDMA, followed by NDMA photolysis to form peroxynitrite and detection with a luminol chemiluminescence reaction. The detection limit for the improved HPLC method was 0.2ng/L, which is 10 times more sensitive than our previously reported system. For tap water measurements, only the addition of an ascorbic acid solution to eliminate residual chlorine and passage through an Oasis MAX solid-phase extraction cartridge are needed. The proposed NDMA determination method requires a sample volume of less than 2mL and a complete analysis time of less than 15min per sample. The method was utilized for the long-term monitoring of NDMA in tap water. The NDMA level measured in the municipal water survey was 4.9ng/L, and a seasonal change of the NDMA concentration in tap water was confirmed. The proposed method should constitute a useful NDMA monitoring method for protecting drinking water quality.


Asunto(s)
Cromatografía Líquida de Alta Presión , Dimetilnitrosamina/análisis , Agua Potable/análisis , Mediciones Luminiscentes , Contaminantes Químicos del Agua/análisis , Ácido Ascórbico/química , Cloruros/química , Dimetilnitrosamina/aislamiento & purificación , Monitoreo del Ambiente , Límite de Detección , Estaciones del Año , Extracción en Fase Sólida , Contaminantes Químicos del Agua/aislamiento & purificación
16.
Angew Chem Int Ed Engl ; 55(21): 6266-9, 2016 05 17.
Artículo en Inglés | MEDLINE | ID: mdl-27071502

RESUMEN

To quantify the properties of protic ionic liquids (PILs) as acid-base reaction media, potentiometric titrations were carried out in a neat PIL, ethylammonium nitrate (EAN). A linear relationship was found between the 14 pKa  values of 12 compounds in EAN and in water. In other words, the pKa  value in EAN was found to be roughly one unit greater than that in water regardless of the charge and hydrophobicity of the compounds. It is possible that this could be explained by the stronger acidity of HNO3 in EAN than that of H3 O(+) in water and not by the difference in the solvation state of the ions. The pH value in EAN ranges from -1 to 9 on the pH scale based on the pH value in water.

17.
Environ Res ; 125: 12-9, 2013 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-23890827

RESUMEN

The distribution of mercury in the soil, sediment and river water around the artisanal small-scale gold mining (ASGM) area along the Cikaniki River, West Java, Indonesia, was investigated. The total mercury concentration (T-Hg) in the forest soil ranged from 0.11 to 7.0mgkg(-1), and the highest value was observed at the ASGM village. In the vertical T-Hg profile around the villages, the highest value was observed at the soil surface, and the concentration decreased with depth. This result suggested that the mercury released by mining activity was dispersed through the atmosphere and deposited on the surface. The total organic carbon content (TOC) showed a similar vertical profile as the T-Hg, and a linear relationship was found between T-Hg and TOC. Mercury deposited on the surface can be absorbed by organic matter. The slope of the line was larger near the ASGM village, implying a higher rate of deposition of mercury. The T-Hg in the sediment ranged from 10 to 70mgkg(-1), decreasing gradually toward the lower reaches of the river. Mining waste can be transported with the river flow and deposited along the river. The distribution of the mining waste can be determined using the mineralogical composition measured by X-ray fluorescence spectrometry.


Asunto(s)
Contaminantes Ambientales/análisis , Mercurio/análisis , Minería , Ríos/química , Suelo/química , Atmósfera/análisis , Oro , Indonesia , Espectrofotometría Atómica
18.
J Chromatogr A ; 1288: 155-9, 2013 May 03.
Artículo en Inglés | MEDLINE | ID: mdl-23522263

RESUMEN

A method for the simultaneous determination of monomethylmercury (MeHg(+)) and monoethylmercury (EtHg(+)) in soil/sediment samples was developed. The method involves eluting mercury species from the soil/sediment samples using 5M HCl containing 5mM Pd(2+) and 0.1M Cu(2+) and then extracting MeHg(+) and EtHg(+) into toluene as chlorides. These alkylmercury chlorides are then back-extracted into an aqueous EDTA solution, creating EDTA complexes. Finally, an emetine-dithiocarbamate (emetineCS2) solution is added to the EDTA solution to form emetineCS2-alkylmercury complexes. EmetineCS2-MeHg and emetineCS2-EtHg were separated using reverse-phase HPLC and then detected by the chemiluminescence reaction with tris(2,2'-bipyridine)ruthenium(III). The MeHg(+) and EtHg(+) calibration curves, using the peak height, were linear from 0.5 to 20ng (as Hg). The detection limit was 0.16ng/g (analyzing 1g soil or sediment). The procedure was validated by analyzing a certified reference material (ERM CC580, estuarine sediment). The MeHg(+) concentration determined using the proposed method was in good agreement with the certified value, and EtHg(+) was detected in the reference material. A preliminary study of the relationship between environmental mercury concentrations and MeHg(+) production was performed.


Asunto(s)
Cromatografía Líquida de Alta Presión/métodos , Compuestos de Etilmercurio/análisis , Compuestos de Metilmercurio/análisis , Contaminantes del Suelo/análisis , Fraccionamiento Químico , Cromatografía de Fase Inversa/métodos , Compuestos de Etilmercurio/química , Compuestos de Etilmercurio/aislamiento & purificación , Sedimentos Geológicos/química , Mediciones Luminiscentes , Compuestos de Metilmercurio/química , Compuestos de Metilmercurio/aislamiento & purificación , Reproducibilidad de los Resultados , Suelo/química , Contaminantes del Suelo/química , Contaminantes del Suelo/aislamiento & purificación
19.
Anal Sci ; 28(10): 959-65, 2012.
Artículo en Inglés | MEDLINE | ID: mdl-23059991

RESUMEN

A sensitive determination method for mercury speciation analysis was developed. Four mercury species, mercury ion, methylmercury, ethylmercury, and phenylmercury, were complexed with emetine-dithiocarbamate (emetine-CS(2)), and then injected onto a HPLC instrument coupled with a tris(2,2'-bipyridine)ruthenium(III) chemiluminescence detection system. The emetine-CS(2) complexing agent was effectively used to measure the concentration in addition to serving as a separation and detection reagent. The calibration curves for these mercury complexes were linear in the range of 0.050 - 10 µg L(-1) (as Hg). The limit of detection for (emetine-CS(2))(2)Hg, emetine-CS(2)-methylmercury, emetine-CS(2)-ethylmercury, and emetine-CS(2)-phenylmercury were 30, 17, 21, and 22 ng L(-1), respectively. The sensitivity of this method enables the determination of mercury species in water samples at sub-ppb levels. Furthermore, the method was applied to biological samples in combination with acid leaching and liquid-liquid extraction using emetine-CS(2) as an extraction reagent. The determination results were in good agreement with the values of the certified reference materials.


Asunto(s)
Cromatografía Líquida de Alta Presión/métodos , Contaminantes Ambientales/análisis , Mediciones Luminiscentes/métodos , Mercurio/análisis , Compuestos Organomercuriales/análisis , Agua/química , Animales , Contaminantes Ambientales/aislamiento & purificación , Compuestos de Etilmercurio/análisis , Compuestos de Etilmercurio/aislamiento & purificación , Peces , Cabello/química , Humanos , Mercurio/aislamiento & purificación , Compuestos de Metilmercurio/análisis , Compuestos de Metilmercurio/aislamiento & purificación , Compuestos Organomercuriales/aislamiento & purificación , Compuestos de Fenilmercurio/análisis , Compuestos de Fenilmercurio/aislamiento & purificación
20.
Chemosphere ; 89(3): 241-8, 2012 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-22595529

RESUMEN

Mercury pollution is caused by artisanal and small-scale gold mining (ASGM) operations along the Cikaniki River (West Java, Indonesia). The atmosphere is one of the primary media through which mercury can disperse. In this study, atmospheric mercury levels are estimated using the native epiphytic fern Asplenium nidus complex (A. nidus) as a biomonitor; these estimates shed light on the atmospheric dispersion of mercury released during mining. Samples were collected from 8 sites along the Cikaniki Basin during September-November, 2008 and September-November, 2009. The A. nidus fronds that were attached to tree trunks 1-3m above the ground were collected and measured for total mercury concentration using cold vapor atomic absorption spectrometry (CVAAS) after acid-digestion. The atmospheric mercury was collected using porous gold collectors, and the concentrations were determined using double-amalgam CVAAS. The highest atmospheric mercury concentration, 1.8 × 10(3) ± 1.6 × 10(3) ngm(-3), was observed at the mining hot spot, and the lowest concentration of mercury, 5.6 ± 2.0 ngm(-3), was observed at the remote site from the Cikaniki River in 2009. The mercury concentrations in A. nidus were higher at the mining village (5.4 × 10(3) ± 1.6 × 10(3) ngg(-1)) than at the remote site (70 ± 30 ngg(-1)). The distribution of mercury in A. nidus was similar to that in the atmosphere; a significant correlation was observed between the mercury concentrations in the air and in A. nidus (r=0.895, P<0.001, n=14). The mercury levels in the atmosphere can be estimated from the mercury concentration in A. nidus using a regression equation: log (Hg(A.nidu)/ngg(-1))=0.740 log (Hg(Air)/ngm (-3)) - 1.324.


Asunto(s)
Contaminantes Atmosféricos/análisis , Helechos/química , Mercurio/análisis , Monitoreo del Ambiente/métodos , Helechos/metabolismo , Oro , Indonesia , Minería
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