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W. Shotyk M.E. Goodsite F. Roos-Barraclough R. Frei G. Asmund T.S. Hansen 《Geochimica et cosmochimica acta》2003,67(21):3991-4011
Mercury concentrations are clearly elevated in the surface and sub-surface layers of peat cores collected from a minerotrophic (“groundwater-fed”) fen in southern Greenland (GL) and an ombrotrophic (“rainwater-fed”) bog in Denmark (DK). Using 14C to precisely date samples since ca. AD 1950 using the “atmospheric bomb pulse,” the chronology of Hg accumulation in GL is remarkably similar to the bog in DK where Hg was supplied only by atmospheric deposition: this suggests not only that Hg has been supplied to the surface layers of the minerotrophic core (GL) primarily by atmospheric inputs, but also that the peat cores have preserved a consistent record of the changing rates of atmospheric Hg accumulation. The lowest Hg fluxes in the GL core (0.3 to 0.5 μg/m2/yr) were found in peats dating from AD 550 to AD 975, compared to the maximum of 164 μg/m2/yr in AD 1953. Atmospheric Hg accumulation rates have since declined, with the value for 1995 (14 μg/m2/yr) comparable to the value for 1995 obtained by published studies of atmospheric transport modelling (12 μg/m2/yr).The greatest rates of atmospheric Hg accumulation in the DK core are also found in the sample dating from AD 1953 and are comparable in magnitude (184 μg/m2/yr) to the GL core; again, the fluxes have since gone into strong decline. The accumulation rates recorded by the peat core for AD 1994 (14 μg/m2/yr) are also comparable to the value for 1995 obtained by atmospheric transport modelling (18 μg/m2/yr). Comparing the Pb/Ti and As/Ti ratios of the DK samples with the corresponding crustal ratios (or “natural background values” for preanthropogenic peat) shows that the samples dating from 1953 also contain the maximum concentration of “excess” Pb and As. The synchroneity of the enrichments of all three elements (Hg, Pb, and As) suggests a common source, with coal-burning the most likely candidate. Independent support for this interpretation was obtained from the Pb isotope data (206Pb/207Pb = 1.1481 ± 0.0002 in the leached fraction and 1.1505 ± 0.0002 in the residual fraction) which is too radiogenic to be explained in terms of gasoline lead alone, but compares well with values for U.K. coals. In contrast, the lowest values for 206Pb/207Pb in the DK profile (1.1370 ± 0.0003 in the leached fraction and 1.1408 ± 0.0003 in the residual fraction) are found in the sample dating from AD 1979: this shows that the maximum contribution of leaded gasoline occurred approximately 25 yr after the zenith in total anthropogenic Pb deposition. 相似文献
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W. Shotyk M.E. Goodsite F. Roos-Barraclough N. Givelet G. Le Roux A.K. Cheburkin J. Heinemeier S.A. Norton 《Geochimica et cosmochimica acta》2005,69(1):1-17
A monolith representing 5420 14C yr of peat accumulation was collected from a blanket bog at Myrarnar, Faroe Islands. The maximum Hg concentration (498 ng/g at a depth of 4.5 cm) coincides with the maximum concentration of anthropogenic Pb (111 μg/g). Age dating of recent peat accumulation using 210Pb (CRS model) shows that the maxima in Hg and Pb concentrations occur at AD 1954 ± 2. These results, combined with the isotopic composition of Pb in that sample (206Pb/207Pb = 1.1720 ± 0.0017), suggest that coal burning was the dominant source of both elements. From the onset of peat accumulation (ca. 4286 BC) until AD 1385, the ratios Hg/Br and Hg/Se were constant (2.2 ± 0.5 × 10-4 and 8.5 ± 1.8 × 10-3, respectively). Since then, Hg/Br and Hg/Se values have increased, also reaching their maxima in AD 1954. The age date of the maximum concentrations of anthropogenic Hg and Pb in the Faroe Islands is consistent with a previous study of peat cores from Greenland and Denmark (dated using the atmospheric bomb pulse curve of 14C), which showed maximum concentrations in AD 1953.The average rate of atmospheric Hg accumulation from 1520 BC to AD 1385 was 1.27 ± 0.38 μg/m2/yr. The Br and Se concentrations and the background Hg/Br and Hg/Se ratios were used to calculate the average rate of natural Hg accumulation for the same period, 1.32 ± 0.36 μg/m2/yr and 1.34 ± 0.29 μg/m2/yr, respectively. These fluxes are similar to the preanthropogenic rates obtained using peat cores from Switzerland, southern Greenland, southern Ontario, Canada, and the northeastern United States. Episodic volcanic emissions and the continual supply of marine aerosols to the Faroe Islands, therefore, have not contributed significantly to the Hg inventory or the Hg accumulation rates, relative to these other areas. The maximum rate of Hg accumulation was 34 μg/m2/yr. The greatest fluxes of anthropogenic Hg accumulation calculated using Br and Se, respectively, were 26 and 31 μg/m2/yr. The rate of atmospheric Hg accumulation in 1998 (16 μg/m2/yr) is comparable to the values recently obtained by atmospheric transport modeling for Denmark, the Faroe Islands, and Greenland. 相似文献
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Karin A. Koinig William Shotyk André F. Lotter Christian Ohlendorf Michael Sturm 《Journal of Paleolimnology》2003,30(3):307-320
A 9000cal. year record of geochemistry was analysed in a sediment core obtained from a Swiss alpine hard-water lake (1937 ma.s.l.) that is located at the present-day tree-line. Geochemical stratigraphies are compared to changes in mineralogy, grain-size, pollen, and macrofossil records. This allows the reconstruction of the effects of changes in vegetation and of 3500 years of land-use in the catchment area on sediment geochemistry. Using principal component analysis, two major geochemical groups are distinguished: (i) Changes in concentrations of Rb, Ti, Zr, Fe, As, and Pb are closely related to corresponding changes in the concentrations of quartz and clay. They are thus considered to represent the silicate fraction which shows an increase from the oldest to the youngest core section. (ii) In contrast, Ca and Sr concentrations are positively correlated with changes in silt, sand, and calcite. They are therefore considered to represent the carbonate fraction which gradually decreased. Based on constrained cluster analysis, the core is divided into two major zones. The oldest zone (A; 9000–6400 cal.BP) is characterised by high concentrations of detrital carbonates. The more open catchment vegetation at that time promoted the physical weathering of these carbonates. The second major zone (B, 6400 cal.BP–1996 AD) is divided into four subsections with boundaries at ca. 3500, 2400, and 160cal. BP. The lower part of this zone, B1, is characterized by a gradual decrease in the carbonate-silt fraction and a pronounced increase in the silicate-clay fraction. This is concurrent with the expansion of Picea in the catchment area, which probably stabilized the soil. The middle part, B2 and B3 (3500–160cal. BP), comprises pronounced fluctuations in all elements, especially Ca, Sr, Mn, and Rb, but also in clay and silt. These changes are related to varying intensities of alpine farming. In the same section, Mn/Fe ratios are highly variable, suggesting changes in the mixing regime of the lake with phases of anoxic bottom water. The uppermost section, B4 (since 160cal. BP), is characterized by a steep decline in the silicate fraction and an increase in Ca and Sr. Despite the decrease in the silicate fraction, Pb increases, due to elevated atmospheric input resulting from early metal pollution, are masked by the high natural variability. Generally, changes in vegetation, which correspond to climate changes in the early Holocene and to human activities since ca. 3700cal. BP, are the controlling factor for variations in the geochemical composition of the sediment of Sägistalsee. 相似文献
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Jeffrey M. McKenzie Donald I. Siegel William Shotyk Philipp Steinmann Gabriele Pfunder 《水文研究》2002,16(5):1047-1064
We report the results of numerical and analytical simulations to test the hypothesis that downward vertical flow of porewater from the crests of domed alpine and kettle bogs controls vertical porewater distributions of major solutes such as Ca and Mg. The domed Etang de la Gruère bog (EGr), Switzerland, characterized by a vertical downward gradient of 0·04 and stratified layers of peat, is chosen as a field site for the model calibration and evaluation. The middle 4‐m section of the 6·5 m thick bog peat is heavily humified and has a hydraulic conductivity of ～10?5·6 cm s?1. Above and below, peat is less humified with a hydraulic conductivity of ～10?3 cm s?1. Heuristic finite difference simulations, using Visual MODFLOW, of the bog hydraulics show that the higher conductivity peat at the bog base is critical to create the observed deep, local flow cells that substantively recharge porewater. Model results and Peclet number calculations show that before ～7000 14C yr BP diffusion of solutes from underlying mineral soils controlled the vertical distribution of porewater chemistry. From 7000 to ～1250 14C BP the porewater chemistry was probably controlled by both upward diffusion and downward advection, and after ～1250 14C yr BP porewater chemistry was probably controlled by downward advection. Concentrations of conservative major solutes in the porewaters of alpine, ombrotrophic bogs are the net effect of both downward vertical porewater movement and upward vertical diffusion, the magnitudes of which are delicately poised to the configuration of the bog water table over time and subsurface peat stratigraphy. Copyright © 2002 John Wiley & Sons, Ltd. 相似文献
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A peat core from an ombrotrophic bog documents the isotopic evolution of atmospheric Pb in central Ontario since AD 1804 ± 53 (210Pb dating). Despite the introduction of unleaded gasoline in the mid-1970’s, the ratio 206Pb/207Pb in atmospheric deposition has not increased as expected, but rather continues to decline. In fact, snowpack sampling (2005 and 2009) and rainwater samples (2008) show that the isotopic composition of atmospheric Pb today is often far less radiogenic than the gasoline lead that had been used in Canada in the past. The peat, snow, and rainwater data presented here are consistent with the Pb isotope data for aerosols collected in Dorset in 1984 and 1986 which were traced by Sturges and Barrie (1989) to emissions from the Noranda smelter in northern Quèbec, Canada’s largest single source of atmospheric Pb. Understanding atmospheric Pb deposition in central Ontario, therefore, requires not only consideration of natural sources and past contributions from leaded gasoline, but also emissions from metal smelting and refining.Lead in the streams which enter Kawagama Lake today (206Pb/207Pb = 1.16 − 1.19) represents a mixture between the natural values (1.191 − 1.201 estimated using pre-industrial lake sediments) and the values found in the humus layer of the surrounding forest soils (206Pb/207Pb = 1.15 − 1.19). In the lake itself, however, Pb is much less radiogenic (206Pb/207Pb as low as 1.09) than in the streams, with the dissolved fraction less radiogenic than particulate material. The evolution of Pb isotope ratios within the watershed apparently reflects preferential removal by sedimentation of comparatively dense, radiogenic, terrestrial particles (derived from the mineral fraction of soils) from the humus particles with lower ratios of 206Pb/207Pb (because of atmospheric Pb contamination). Despite the contemporary enrichments of Pb in rain and snow, concentrations of dissolved Pb in the lake are extremely low (sometimes below 10 ng/l), with Pb concentrations and Pb/Sc ratios approaching “natural” values because of efficient binding to particles, and their subsequent removal in the watershed. 相似文献
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L. Ukonmaanaho T.M. Nieminen N. Rausch A. Cheburkin G. Le Roux W. Shotyk 《Global and Planetary Change》2006,53(4):259
Accumulation of organic matter (OM) was studied in four ombrotrophic peat bogs in Finland: Harjavalta (vicinity of a Cu–Ni smelter), Outokumpu (near a closed Cu–Ni mine), Alkkia (Ni-treated site) and Hietajärvi (a pristine site). At each sampling site, two peat cores (15 × 15 × 100 cm) were taken. Age-dating of peat was determined using 210Pb method (CRS model). The local annual temperature sum and precipitation for the past 125 years were modeled. The objective was to compare recent net accumulation rates of heavy metal polluted ombrotrophic peat bogs with those of a pristine bog, and to study the relationship between weather and net accumulation rates. Based on 210Pb age-dating, the upper 16-cm peat layer at Harjavalta, 35 cm at Outokumpu and 25 cm at Hietajärvi represents 125 years of peat formation, yielding the following average peat accumulation rates: Harjavalta 1.3 mm year− 1, Outokumpu 2.8 mm year− 1 and Hietajärvi 2.0 mm year− 1. At the Alkkia site, the Ni treatment in 1962 had completely stopped the peat accumulation. Net accumulation rates were related to precipitation at Outokumpu, Harjavalta and Hietajärvi sites. In addition, emissions released from the nearby located Cu–Ni smelter could have affected negatively net OM accumulation rate at Harjavalta site. 相似文献
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Ombrotrophic bogs are useful records of the impact of historical human activity on heavy metal contamination. Several studies concerning the trace element record (mainly Pb and Hg) in these particular environments have been carried out in recent years, although the role of humic substances has often not been considered. In particular, of the components of peat organic matter, fulvic acids and low molecular weight compounds are generally responsible for the mobility of trace elements through the profile, while humic acids (HAs) are involved in the formation of more stable organo-mineral complexes. In order to study the parallel distribution of As, Cr, Ni, Rb, Ti and Zr in bulk peat and the corresponding HAs, a peat core (10 × 10 × 81 cm) was collected from Etang de la Gruère (Switzerland) and cut into 27 slices of 3 cm. The samples were freeze-dried and milled very finely, and HAs extracted from each sample. Both peat and HAs were analyzed using an energy-dispersive miniprobe X-ray fluorescence multielement analyser (EMMA-XRF). Of the considered elements, Ni showed a great affinity for the humic acid component, while Cr was concentrated mainly into humic material from the deeper layers. On the other hand, Ti, Zr and Rb seemed to reflect the variation in mineral material both in peat and HA samples, while the As content of both materials reflected the environmental conditions characterizing the bog. 相似文献
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