Publications (47)194.72 Total impact
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Article: Climate-related variations in crustal trace elements in Dome C (East Antarctica) ice during the past 672 kyr
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ABSTRACT: Cr, Fe, Rb, Ba and U were determined by inductively coupled plasma sector field mass spectrometry (ICP-SFMS) in various sections of the 3,270m deep ice core recently drilled at Dome C on the high East Antarctic plateau as part of the EPICA program. The sections were dated from 263kyr bp (depth of 2,368m) to 672kyr bp (depth of 3,062m). When combined with the data previously obtained by Gabrielli and co-workers for the upper 2,193m of the core, it gives a detailed record for these elements during a 672-kyr period from the Holocene back to Marine Isotopic Stage (MIS) 16.2. Concentrations and fallout fluxes of all elements are found to be highly variable with low values during the successive interglacial periods and much higher values during the coldest periods of the last eight climatic cycles. Crustal enrichment factors indicates that rock and soil dust is the dominant source for Fe, Rb, Ba and U whatever the period and for Cr during the glacial maxima. The relationship between Cr, Fe, Rb, Ba and U concentrations and the deuterium content of the ice appears to be similar before and after the Mid-Brunhes Event (MBE, around 430kyr bp). Mean concentration values observed during the successive interglacials from the Holocene to MIS 15.5 appear to vary from one interglacial to another at least for part of the elements. Concentrations observed during the successive glacial maxima suggest a decreasing trend from the most recent glacial maxima (MIS 2.2 and 4.2) to the oldest glacial maxima such as MIS 14.2, 14.4 and 16.2, which could be linked with changes in the size distribution of dust particles transported from mid-latitude areas to the East Antarctic ice cap.Climatic Change 04/2012; 92(1):191-211. · 3.38 Impact Factor -
Article: Isotopic signatures for natural versus anthropogenic Pb in high-altitude Mt. Everest ice cores during the past 800 years.
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ABSTRACT: A long-term record, extending back 800 years (1205 to 2002 AD), of the Pb isotopic composition ((206)Pb/(207)Pb and (208)Pb/(207)Pb) as well as Pb concentrations from high altitude Mt. Everest ice cores has the potential to identify sources and source regions affecting natural and anthropogenic Pb deposition in central Asia. The results show that the regional natural background Pb isotope signature (~1.20 for (206)Pb/(207)Pb and ~2.50 for (208)Pb/(207)Pb) in the central Himalayas was dominated by mineral dust over the last ~750 years from 1205 to 1960s, mostly originating from local sources with occasional contributions of long-range transported dust probably from Sahara desert and northwestern India. Since the 1970s, the Pb isotope ratios are characterized by a continuous decline toward less radiogenic ratios with the least mean ratios of 1.178 for (206)Pb/(207)Pb and 2.471 for (208)Pb/(207)Pb in the period 1990-1996. The depression of the (206)Pb/(207)Pb and (208)Pb/(207)Pb values during the corresponding periods is most likely due to an increasing influence of less radiogenic Pb of anthropogenic origin mainly from leaded gasoline used in South Asia (India as well as possibly Bangladesh and Nepal). From 1997 to 2002, isotopic composition tends to show a shift to slightly more radiogenic signature. This is likely attributed to reducing Pb emissions from leaded gasoline in source regions, coinciding with the nationwide reduction of Pb in gasoline and subsequent phase-out of leaded gasoline in South Asia since 1997. An interesting feature is the relatively high levels of Pb concentrations and enrichment factors (EF) between 1997 and 2002. Although the reason for this feature remains uncertain, it would be probably linked with an increasing influence of anthropogenic Pb emitted from other sources such as fossil fuel combustion and non-ferrous metal production.Science of The Total Environment 10/2011; 412-413:194-202. · 3.29 Impact Factor -
Article: An 800-year record of atmospheric As, Mo, Sn, and Sb in central Asia in high-altitude ice cores from Mt. Qomolangma (Everest), Himalayas.
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ABSTRACT: As, Mo, Sn, and Sb have been determined by inductively coupled plasma sector field mass spectrometry (ICP-SFMS) in 143 depth intervals of high-altitude ice cores from Mt. Everest, covering an 800-year time period from 1205 to 2002 AD. The results clearly demonstrate the long-term historical record of atmospheric transport and deposition of As, Mo, Sn, and Sb that has prevailed at high altitudes in the central Himalayas. Natural contributions, mainly from mineral dust, have dominated the atmospheric cycles of As, Mo, Sn, and to some extent Sb during the 700 years prior to the 20th century. Compared to those of the pre-1900 period, pronounced increases of both concentrations and crustal enrichment factors are observed since the 1970s, with the highest increase factor for Sn and the lowest for As. Such increases are attributed to anthropogenic emissions of these elements, largely from stationary fossil fuel combustion and nonferrous metals production, particularly in India. Our central Himalayan ice core record provides an explicit recognition of rising atmospheric As, Mo, Sn, and Sb pollution in response to rapid economic growth in central Asia.Environmental Science and Technology 11/2009; 43(21):8060-5. · 5.23 Impact Factor -
Article: An ultra-clean technique for accurately analysing Pb isotopes and heavy metals at high spatial resolution in ice cores with sub-pg g(-1) Pb concentrations.
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ABSTRACT: Measurements of Pb isotope ratios in ice containing sub-pg g(-1) concentrations are easily compromised by contamination, particularly where limited sample is available. Improved techniques are essential if Antarctic ice cores are to be analysed with sufficient spatial resolution to reveal seasonal variations due to climate. This was achieved here by using stainless steel chisels and saws and strict protocols in an ultra-clean cold room to decontaminate and section ice cores. Artificial ice cores, prepared from high purity water were used to develop and refine the procedures and quantify blanks. Ba and In, two other important elements present at pg g(-1) and fg g(-1) concentrations in Polar ice, were also measured. The final blank amounted to 0.2+/-0.2 pg of Pb with (206)Pb/(207)Pb and (208)Pb/(207)Pb ratios of 1.16+/-0.12 and 2.35+/-0.16, respectively, 1.5+/-0.4 pg of Ba and 0.6+/-2.0 fg of In, most of which probably originates from abrasion of the steel saws by the ice. The procedure was demonstrated on a Holocene Antarctic ice core section and was shown to contribute blanks of only approximately 5%, approximately 14% and approximately 0.8% to monthly resolved samples with respective Pb, Ba and In concentrations of 0.12 pg g(-1), 0.3 pg g(-1) and 2.3 fg g(-1). Uncertainties in the Pb isotopic ratio measurements were degraded by only approximately 0.2%.Analytica chimica acta 03/2009; 634(2):228-36. · 4.31 Impact Factor -
Article: Atmospheric pollution for trace elements in the remote high-altitude atmosphere in central Asia as recorded in snow from Mt. Qomolangma (Everest) of the Himalayas.
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ABSTRACT: A series of 42 snow samples covering over a one-year period from the fall of 2004 to the summer of 2005 were collected from a 2.1-m snow pit at a high-altitude site on the northeastern slope of Mt. Everest. These samples were analyzed for Al, V, Cr, Mn, Co, Ni, Cu, Zn, As, Rb, Sr, Cd, Sb, Pb, and Bi in order to characterize the relative contributions from anthropogenic and natural sources to the fallout of these elements in central Himalayas. Our data were also considered in the context of monsoon versus non-monsoon seasons. The mean concentrations of the majority of the elements were determined to be at the pg g(-1) level with a strong variation in concentration with snow depth. While the mean concentrations of most of the elements were significantly higher during the non-monsoon season than during the monsoon season, considerable variability in the trace element inputs to the snow was observed during both periods. Cu, Zn, As, Cd, Sb, and Bi displayed high crustal enrichment factors (EFc) in most samples, while Cr, Ni, Rb, and Pb show high EFc values in some of the samples. Our data indicate that anthropogenic inputs are potentially important for these elements in the remote high-altitude atmosphere in the central Himalayas. The relationship between the EFc of each element and the Al concentration indicates that a dominant input of anthropogenic trace elements occurs during both the monsoon and non-monsoon seasons, when crustal contribution is relatively minor. Finally, a comparison of the trace element fallout fluxes calculated in our samples with those recently obtained at Mont Blanc, Greenland, and Antarctica provides direct evidence for a geographical gradient of the atmospheric pollution with trace elements on a global scale.Science of The Total Environment 11/2008; 404(1):171-81. · 3.29 Impact Factor -
Article: Simultaneous determination of picogram per gram concentrations of Ba, Pb and Pb isotopes in Greenland ice by thermal ionisation mass spectrometry.
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ABSTRACT: A technique has been developed to simultaneously measure picogram per gram concentrations of Ba and Pb by isotope dilution mass spectrometry, as well as Pb isotopic ratios in polar ice by thermal ionisation mass spectrometry. BaPO2(+) and Pb+ ions were employed for these determinations. A calibrated mixture of enriched 205Pb and 137Ba was added to the samples providing an accuracy of better than approximately 2% for Pb/Ba element ratio determinations. Interference by molecular ions in the Pb mass spectrum occurred only at 204Pb and 205Pb, but these contributions were negligible in terms of precisions expected on picogram-sized Pb samples. The technique is illustrated with measurements on Greenland firn, using a drill-core section that includes the Laki volcanic eruption of 1783-1784. The data show deviations from the element concentrations indicating volatile metal enrichments, but the Pb isotopic signature of the Laki lava could not be identified.Analytical and Bioanalytical Chemistry 02/2008; 390(2):495-501. · 3.78 Impact Factor -
Article: Glacial-interglacial changes in the occurrence of Pb, Cd, Cu and Zn in Vostok Antarctic ice from 240 000 to 410 000 years BP.
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ABSTRACT: Lead (Pb), cadmium (Cd), copper (Cu) and zinc (Zn) have been measured by electrothermal atomic absorption spectrometry in various sections of the 3623 m deep ice core drilled at Vostok, in central East Antarctica. The sections were dated from 240 to 410 kyear BP (Marine Isotopic Stages (MIS) 7.5 to 11.3), which corresponds to the 3rd and 4th glacial-interglacial cycles before present. Concentrations are found to have varied greatly during this 170 kyear time period, with high concentration values during the coldest climatic stages such as MIS 8.4 and 10.2 and much lower concentration values during warmer periods, such as the interglacials MIS 7.5, 9.3 and 11.3. Rock and soil dust were the dominant sources for Pb, whatever the period, and for Zn and Cu and possibly Cd during cold climatic stages. The contribution from volcanic emissions was important for Cd during all periods and might have been significant for Cu and Zn during warm periods.Journal of Environmental Monitoring 01/2006; 7(12):1326-31. · 1.99 Impact Factor -
Article: Atmospheric particle evolution during a nighttime atmospheric mercury depletion event in sub-Arctic at Kuujjuarapik/Whapmagoostui, Québec, Canada.
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ABSTRACT: During a field experiment at Kuujjuarapik/Whapmagoostui (55.31 degrees N, 77.75 degrees W), Quebec, we observed increases of concentrations of particles with diameters larger than 0.3 microm in the ambient air during a nighttime atmospheric mercury depletion event (AMDE). These increases were strongly correlated with decreases of ozone and atmospheric mercury, and we also observed a change in the particle size distribution during this AMDE. Assuming that these phenomena imply either a chemical link or an association through transport, we also studied the nature of this AMDE. We hypothesize that the observed AMDE was a result of an influx of already depleted air masses and that it was not a product of local chemical reactions.Science of The Total Environment 02/2005; 336(1-3):215-24. · 3.29 Impact Factor -
Article: Meteoric smoke fallout over the Holocene epoch revealed by iridium and platinum in Greenland ice.
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ABSTRACT: An iridium anomaly at the Cretaceous/Tertiary boundary layer has been attributed to an extraterrestrial body that struck the Earth some 65 million years ago. It has been suggested that, during this event, the carrier of iridium was probably a micrometre-sized silicate-enclosed aggregate or the nanophase material of the vaporized impactor. But the fate of platinum-group elements (such as iridium) that regularly enter the atmosphere via ablating meteoroids remains largely unknown. Here we report a record of iridium and platinum fluxes on a climatic-cycle timescale, back to 128,000 years ago, from a Greenland ice core. We find that unexpectedly constant fallout of extraterrestrial matter to Greenland occurred during the Holocene, whereas a greatly enhanced input of terrestrial iridium and platinum masked the cosmic flux in the dust-laden atmosphere of the last glacial age. We suggest that nanometre-sized meteoric smoke particles, formed from the recondensation of ablated meteoroids in the atmosphere at altitudes >70 kilometres, are transported into the winter polar vortices by the mesospheric meridional circulation and are preferentially deposited in the polar ice caps. This implies an average global fallout of 14 +/- 5 kilotons per year of meteoric smoke during the Holocene.Nature 01/2005; 432(7020):1011-4. · 36.28 Impact Factor -
Article: Meteoric smoke fallout over the Holocene epoch revealed by iridium and platinum in Greenland ice
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ABSTRACT: An iridium anomaly at the Cretaceous/Tertiary boundary layer has been attributed to an extraterrestrial body that struck the Earth some 65 million years agoNature 12/2004; 432(7020):1011-1014. · 36.28 Impact Factor -
Article: Elemental indicators of natural and anthropogenic aerosol inputs to Law Dome, Antarctica
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ABSTRACT: A selection of elements (Bi, Ca, Cd, Co, Cu, Mn, Na, Sr, U, V, Zn) were measured by high-resolution inductively coupled plasma sector-field mass spectrometry in firn- and ice-core samples from Law Dome, Antarctica, corresponding to the period 4500 BC to AD 1989. Concentrations of rock dust and sea salts were calculated for each sample and then used to determine concentrations of each element originating from crustal and marine aerosol emissions, respectively. Where calculated contributions from crustal and marine aerosol sources failed to account for the total measured concentration of an element, the remainder was apportioned to volcanic and/or anthropogenic sources and defined as an enrichment. On this basis, it was determined that Bi and Cd concentrations in Law Dome ice are overwhelmingly influenced by volcanic emissions (enrichments 150-250x crustal and marine inputs); Co, Cu, Pb and Zn concentrations in Law Dome ice are largely influenced by volcanic emissions (enrichments 16-36x crustal and marine inputs); and Mn, Sr, U and V concentrations in Law Dome ice are minimally influenced by volcanic emissions (enrichments 1.5-4x crustal and marine inputs). During the 20th century, enrichments of Pb and Cu concentrations were observed to be greater than in earlier centuries, consistent with increasing anthropogenic emissions of Pb and Cu in the Southern Hemisphere over that period.Annals of Glaciology 05/2004; 39(1):169-174. · 1.80 Impact Factor -
Article: Profiles of Mercury in the snow pack at Station Nord, Greenland shortly after polar sunrise
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ABSTRACT: 1] Mercury (Hg) species have been measured in the snow pack at Station Nord, Greenland both in the snow and in the air of snow from February 25 to March 15, 2002, during twilight and low solar irradiation periods. More than 99% of Hg is in the snow itself ($94– 97% as Hg 2+ and $5% as MeHg +) while less than 1% is in the interstitial air of snow as Hg°. Gaseous Elemental Mercury (Hg°) concentrations, decreased exponentially with depth from $1.5 ng/m 3 outside to $0.1 ng/m 3 at 120 cm depth in the snow air. Hg° incorporation flux to the snow pack has been evaluated to $5.8 –7.0 pg/m 2 /h which is weak, indicating that this process does not change significantly the Hg content in the snow. We believe that this decrease in the air of snow is the result of fast oxidation processes of Hg° rather than adsorption of Hg° onto snow surfaces.Geophys. Res. Lett. 01/2004; 31. -
Article: Diurnal cycles of gaseous mercury within the snowpack at Kuujjuarapik/Whapmagoostui, Québec, Canada.
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ABSTRACT: Mercury is a globally dispersed and toxic pollutant that can be transported far from its emission sources. In polar and subpolar regions, recent research activities have demonstrated its ability to be converted and deposited rapidly onto snow surfaces during the so-known Mercury Depletion Events (MDEs). The fate of mercury once deposited onto snow surfaces is still unclear: a part could be re-emitted to the atmosphere, the other part could contaminate water systems at the snowmelt. Its capacity to transform to more toxic form and to bioaccumulate in the food chain has consequently made mercury a threat for Arctic ecosystems. The snowpack is a medium that greatly interacts with a variety of atmospheric gases. Its role in the understanding of the fate of deposited mercury is crucial though it is poorly understood. In April 2002, we studied an environmental component of mercury, which is interstitial gaseous mercury (IGM) present in the air of the snowpack at Kuujjuarapik/Whapmagoostui (55 degrees N, 77 degrees W), Canada on the east shore of the Hudson Bay. We report here for the first time continuous IGM measurements at various depths inside a seasonal snowpack. IGM concentrations exhibit a well-marked diurnal cycle with uninterrupted events of Hg0 depletion and production within the snowpack. A possible explanation of Hg0 depletion within the snowpack may be Hg0 oxidation processes. Additionally, we assume that the notable production of Hg0 during the daytime may be the results of photoreduction and photoinitiated reduction of Hg(II) complexes. These new observations show that the snowpack plays undoubtedly a role in the global mercury cycle.Environmental Science and Technology 09/2003; 37(15):3289-97. · 5.23 Impact Factor -
Article: The fate of mercury species in a sub-arctic snowpack during snowmelt
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ABSTRACT: An extensive mercury study was conducted in April 2002 prior to and during the annual melting of a snowpack in a sub-arctic site along the Hudson Bay (Canada). Gas-phase measurements show that the snowmelt coincides with an elemental mercury (Hg°) pulse in the snowpack air far above ambient levels. Additional measurements of inorganic mercury (Hg 2+) and methylmercury (MeHg +) in snow pits, in surface snow and in a meltwater sample clearly reveal that most of Hg is removed from the snow during the first days of snowmelt. We estimate that gas-phase exchanges contribute poorly to remove Hg from the snowpack; consequently during a snowmelt day more than 90% of Hg present in the snow surface is likely released with the meltwater. In arctic areas, where Hg accumulates at an accelerated rate in the snow surfaces [Lu et al., 2001] during mercury depletion events (MDE), the 2 discharge of this toxic and bio-accumulating pollutant in water systems could be a threat to ecosystems and local indigenous populations.Geophysical Research Letters 06/2003; 30(12):1621-1625. · 3.79 Impact Factor -
Article: First investigation of an original device dedicated to the determination of gaseous mercury in interstitial air in snow.
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ABSTRACT: The GAMAS (gaseous mercury in interstitial air in snow) instrument developed in our laboratory is a new device devoted to sampling and determination of gaseous mercury concentration in interstitial air in snow. Sampling probes inserted in the snowpack, coupled with a Gardis mercury vapour analyser, provide reliable and original data of vertical profiles of both snow temperature and gaseous mercury concentration at several depths in a snow mantle. This instrument has been tested successfully in Station Nord in Greenland in February-March 2002. A description of this instrument, of the sampling area and its setting up is presented with precise details. Illustrations of the first investigations are given showing a rapid decrease of gaseous mercury concentration simultaneously with depth. A concentration of 0.10 ng/m(3) is reached at 120 cm depth. It may be the result of fast oxidation processes occurring within the snowpack. Gaseous mercury behaviour in the snowpack is a central parameter to elucidate the fate of deposited mercury after mercury depletion events in polar regions. With our new device, we have now the opportunity to determine this key parameter.Analytical and Bioanalytical Chemistry 02/2003; 375(1):106-11. · 3.78 Impact Factor -
Article: Influence of anthropogenic sources on total gaseous mercury variability in Grenoble suburban air (France).
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ABSTRACT: Total gaseous mercury (TGM) has been monitored at Champ sur Drac, a suburban site of Grenoble in southern east France. TGM measurements have been made over 4 periods of approximately 10 days throughout 1999-2000 using cold vapour atomic fluorescence absorption technique. The first monitoring campaign was initiated on November 4, 1999, followed by three other campaigns respectively on January 12, 2000, April 10, 2000 and July 17, 2000. Concurrent monitoring of O3, NO, NO2, SO2 and of meteorological parameters have also been performed. The mean TGM concentration was 3.4 ng m(-3) with maximum hourly mean concentration of 37.1 ng m(-3). Although mean TGM concentration was not greatly different from those previously measured in the troposphere, the greater TGM variability as well as the occurrence of high TGM concentration linked to particular wind conditions suggested the strong influence of anthropogenic sources. The chlor-alkali plant located nearby, the others chemical industries using fuel combustion and the municipal waste incinerator were thought to contribute to mercury pollution events.Science of The Total Environment 11/2002; 297(1-3):203-13. · 3.29 Impact Factor -
Article: Speciation analysis of organolead compounds in Greenland snow at the femtogram-per-gram level by capillary gas chromatography/atomic emission spectrometry
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Article: Mercury speciation in the French seasonal snow cover.
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ABSTRACT: Snow samples have been collected in the French Alps in 1998, 1999 and 2000 in order to measure both total Hg (HgT) and reactive Hg (HgR). Concentrations of HgT were between 13 and 130 pg g(-1) and HgR concentrations were below the detection limit (approximately 0.8 pg g(-1)). Hg speciation in snow was evaluated on the basis of ionic complexation equilibrium with chloride, hydroxide, oxalate. The pH of the snow was found to be an important parameter for Hg speciation. For pH values near 3, HgC2O4 is predominant in snow samples except for snow strongly influenced by anthropogenic sources (in which case HgCl2 predominates). When pH > 4, Hg(OH)2 and HgOHCl are predominant. These latter pH values are observed for precipitation not influenced by anthropogenic sources but more by soil erosion, e.g. Saharan dusts. The knowledge of Hgr speciation in snow is a key question for understanding the mechanisms of transformation of these complexes in snow after precipitation.Science of The Total Environment 03/2002; 287(1-2):61-9. · 3.29 Impact Factor -
Article: Present Century Record of Organolead Pollution in High Altitude Alpine Snow
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ABSTRACT: Organolead compounds are tracers of lead additives used as anti-knocking agents in leaded gasoline, and snow/ice cores are useful archives of environmental pollution. Determination of these species in those archives provides information on their influence on the Pb pollution by monitoring the changes of organolead concentrations during the years. Organolead compounds have been analyzed by gas chromatography coupled to microwave-induced plasma atomic emission spectrometry (GC−MIP-AES) in a series of snow pit and snow/ice core samples deposited in a high altitude site in the Mont Blanc area between 1956 and 1994. Measured concentrations ranged from 0.1 to 3 pg/g for dimethyllead, from 0.08 to 3.4 pg/g for trimethyllead, from 0.01 to 0.57 pg/g for diethyllead, and from 0.01 to 0.13 pg/g for triethyllead. No organolead compounds were detected in ice deposited before 1962. Concentrations of total alkyllead increased from 1962 till the late 1980s but then declined significantly during the 1990s. Changes in consumption of these species in France were compared with the obtained data. A delay of several years was observed between the restricted consumption of these additives and the subsequent decrease in concentrations observed in the ice. Furthermore, the data were compared with two records for organolead pollution obtained for the Northern Hemisphere: one for Central Greenland snow and the other for vintages originating from the Rhône Valley in southeast France.11/1999; -
Article: Determination of Rh, Pd, and Pt in Polar and Alpine Snow and Ice by Double-Focusing ICPMS with Microconcentric Nebulization
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ABSTRACT: The performance of a double-focusing inductively coupled plasma mass spectrometer equipped with a microconcentric nebulizer was investigated for the direct simultaneous determination of Rh, Pd, and Pt in less than 1 mL of melted snow and ice samples originating from remote sites. Ultraclean procedures were adopted in the laboratories and during the pretreatment steps, to avoid possible contamination problems. Spectroscopic and nonspectroscopic interferences affecting the determination of Rh, Pd, and Pt were carefully considered. Detection limits of 0.02, 0.08, and 0.008 pg g-1 for Rh, Pd, and Pt, respectively, were obtained using the following isotopes: 103Rh, 106Pd, and 195Pt. Repeatability of measurements, as RSD, was 27, 28, and 29%, for Rh, Pd, and Pt, respectively. The new method was applied to the analysis of samples coming from Greenland, Antarctica, and the Alps in order to assess the past natural background concentrations and to determine the present level of these polluting substances. The extremely low detection limits allowed the direct analysis of all samples except for two Greenland ice core sections dating from 7260 and 7760 years ago for which a preconcentration step was necessary. Concentration ranges for all snow samples were (in pg g-1) as follows: Rh (0.0005−0.39), Pd (0.01−16.9), and Pt (0.008−2.7). The lowest concentrations were measured in the enriched Greenland ancient ice samples.Analytical Chemistry 08/1999; 71(19). · 5.86 Impact Factor
Top co-authors
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Institutions
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2008–2009
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Curtin University Australia
- Department of Applied Physics
Bentley, Western Australia, Australia -
Korea Polar Research Institute
Seoul, Seoul, South Korea
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2002–2005
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Université Joseph Fourier - Grenoble 1
- Laboratoire de Glaciologie et Géophysique de l'Environnement
Grenoble, Rhone-Alpes, France
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