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1.
C.E. Dunlap C.N. Alpers H.E. Taylor A.R. Flegal 《Geochimica et cosmochimica acta》2008,72(24):5935-5948
Lead concentrations and isotope ratios measured in river water colloids and streambed sediment samples along 426 km of the Sacramento River, California reveal that the influence of lead from the historical mining of massive sulfide deposits in the West Shasta Cu-mining district (at the headwaters of the Sacramento River) is confined to a 60 km stretch of river immediately downstream of that mining region, whereas inputs from past leaded gasoline emissions and historical hydraulic Au-mining in the Sierra Nevadan foothills are the dominant lead sources in the remaining 370 km of the river. Binary mixing calculations suggest that more than 50% of the lead in the Sacramento River outside of the region of influence of the West Shasta Cu-mining district is derived from past depositions of leaded gasoline emissions. This predominance is the first direct documentation of the geographic extent of gasoline lead persistence throughout a large riparian system (>160,000 km2) and corroborates previous observations based on samples taken at the mouth of the Sacramento River. In addition, new analyses of sediment samples from the hydraulic gold mines of the Sierra Nevada foothills confirm the present-day fluxes into the Sacramento River of contaminant metals derived from historical hydraulic Au-mining that occurred during the latter half of the 19th and early part of the 20th centuries. These fluxes occur predominantly during periods of elevated river discharge associated with heavy winter precipitation in northern California. In the broadest context, the study demonstrates the potential for altered precipitation patterns resulting from climate change to affect the mobility and transport of soil-bound contaminants in the surface environment. 相似文献
2.
Trace element concentrations (Pb, Cd, Mn, Fe, and Zn) were measured along four surface water transects across the continental shelf off Baja California, to evaluate the magnitude of heavy metal contamination in the coastal waters along the US-Mexican boundary. These initial measurements of trace elements in Mexican neritic waters revealed offshore concentration gradients, with the highest levels in coastal waters with high salinities and nutrient concentrations. There were also longshore gradients, with lower concentrations in the southern locations. Although the relative enrichment of metals detected at nearshore stations along the US-Mexican border appeared to correspond to wastewater discharges in that area, these trace metal enhancements were found to be primarily associated with physical oceanographic processes (upwelling and advection), rather than anthropogenic inputs. This was demonstrated both by metal-nutrient correlations and multivariate statistical analyses. Mass balance calculations also indicated that about 1% of Cd, 9% of Zn, and 29% of Pb were from urban discharges within the area. 相似文献
3.
Antonio Tovar-Snchez Sergio A. Saudo-Wilhelmy A. Russell Flegal 《Estuarine, Coastal and Shelf Science》2004,60(4):717-728
Despite the fact that Co is an essential trace element for the growth of marine phytoplankton, there is very limited information on the cycling of this trace metal in the marine environment. We report here the distribution of dissolved (<0.4 μm) and particulate (>0.4 μm) Co in surface waters of the Hudson River Estuary (HRE) and San Francisco Bay (SFB). Samples were collected during several cruises (from 1990 to 1995 in SFB and from 1995 to 1997 in the HRE) along the whole salinity gradient. Dissolved Co concentrations (mean±1 standard deviation) were nearly identical in magnitude in both estuaries despite differences in climate, hydrography, riverine-flow conditions and land-usage (HRE=0.91±0.61 nM; SFB=1.12±0.69 nM). Dissolved Co levels in each system showed non-conservative distributions when plotted as a function of salinity, with increasing concentrations downstream from the riverine end-members. Desorption from suspended particulates and sewage inputs, therefore, seems to be the major processes responsible for the non-conservative behavior of Co observed. Mass balance estimates also indicated that most of the estuarine Co is exported out of both estuaries, indicating that they and other estuarine systems are principal sources of this essential trace element to the open ocean. 相似文献
4.
Concentrations of lead were measured in a surface transect and at two vertical profile stations (15°N and 20°S) in the Central Pacific. These measurements complement similar measurements made earlier in the North Pacific at 33°N and in the Northwest Atlantic at 34°N [1,2], as well as recent measurements of eolian lead input fluxes near each of these locations [3]. The new transect of surface water concentrations of lead corroborates previous measurements, which decrease from 13 ng/kg at 30°N to 4 ng/kg at 17°S in the Central Pacific [4]. This transect gradient is shown to overlie a similar geographic gradient of subsurface maximum concentrations of lead in the three Pacific vertical profile stations, decreasing from 14 ng/kg at 33°N to 11 ng/kg at 14°N to 2.5 ng/kg at 20°S. Lead concentrations at each of those locations exhibit maxima at 400 m, decreasing concentrations to 2500 m and approximately concentrations of 0.8–1.1 ng/kg below that depth. The subsurface maximum at the northwest Atlantic profile station (36 ng/kg at 34°N) is also congruent with surface water lead concentrations which decrease from 806 ng/kg to 32 ng/kg in an offshore transect from Rhode Island to 34°N, 66°W [5], and the shape of the Atlantic profile is congruent with those in the Pacific. There is a positive correlation between the magnitudes of eolian lead input fluxes and the magnitudes of the upper water maxima in lead concentration profiles at corresponding locations as follows: South Pacific easterlies 3 ng/cm2 yr vs. 2.5 ng/kg; North Pacific easterlies 6 ng/cm2 yr vs. 11 ng/kg; North Pacific westerlies 50 ng/cm2 yr vs. 14 ng/kg; and North Atlantic westerlies 170 ng/cm2 yr vs. 36 ng/kg.This relationship enables one to view the anthropogenic perturbations of the marine lead cycle on a global scale, since the industrial origin of eolian and seawater lead has been established by correlations between geographic patterns of industrial lead emissions to the atmosphere and isotopic ratios of industrial leads [3] and by geographic patterns of Pb/silicate-dust ratios and lead isotopic ratios in ocean surface waters [3–5]. These new data coupled with earlier biogeochemical data indicate that surface water concentrations of lead in the North Pacific and North Atlantic are now conservatively estimated to be 8 to 20-fold greater and those in the South Pacific are 2-fold greater than natural concentrations because of industrial emissions of lead to the atmosphere. 相似文献
5.
Edward D. Goldberg Minoru Koide Vern Hodge A.Russel Flegal John Martin 《Estuarine, Coastal and Shelf Science》1983,16(1):69-93
The results of the U.S. Mussel Watch Monitoring Program for the period 1976–1978 for trace metals and artificial radionuclides in bivalves are presented. The substances analysed included Ag, Cu, Zn, Cd, Ni, Pb, 238Pu, 239+240Pu and 241Am. The analyses of organic substances will be presented elsewhere. The concentrations of these substances in the bivalves may reflect upwelling processes, anthropogenic inputs or natural levels. Off the California coast, mussels show markedly elevated Pu and Cd concentrations in coastal areas adjacent to the most intensive upwelling zones. Elevated levels of Pb, for example, are found in organisms living adjacent to highly urbanized places. The general patterns of distribution repeat themselves year after year at a given site. Thus, it is concluded that annual monitoring activities may not be necessary and that a frequency of sampling of several or so years may be more appropriate to identify pollution problems. Finally, national or regional baselines for metal concentrations in bivalves from unpolluted waters are proposed. National baselines for Pb in the west coast mussels of 1·0 parts 10?6 and for Ag in east coast mussels of 0·05 parts 10?6 are suggested. 相似文献
6.
The geographic variation in the isotopic composition of lead in surface waters of the central Pacific provides new evidence of the global anthropogenic perturbation of the element's cycle. Ratios of 206Pb/207Pb decrease from 1.196 in the northern hemisphere (19°N, 158°W) to 1.176 in the southern hemisphere (15°S, 150°W). This decrease parallels the geographic variation in surface concentrations of soluble lead which decrease from 13 ng kg?1 at the northern station to 4 ng kg?1 at the southern station. Both the 206Pb/207Pb and the 206Pb/208Pb ratios of those waters fit between the isotopic ratios of Australian (Broken Hill) and North American (Mississippi Valley) leads which are the predominant sources of leads in anthropogenic emissions to the Pacific Ocean basin. 相似文献
7.
P.B. Kozelka S. Sañudo-Wilhelmy A.R. Flegal K.W. Bruland 《Estuarine, Coastal and Shelf Science》1997,44(6):649-658
The speciation of lead at a site in the South San Francisco Bay was determined using a combination of physical size fractionation and electrochemical analyses. The ‘ total dissolvable ’ Pb was 8·1 nM from analysis of an acidified unfiltered sample. The ‘ dissolved ’ Pb was equal to 0·20 nM (41 ng l−1), only 2·5% of the ‘ total dissolvable ’ Pb. The difference yielded the ‘ particulate ’ Pb equal to 7·9 nM (1·6 μg l−1). Results from crossflow ultrafiltration indicated that almost all (0·19 nM) of the dissolved Pb was ‘ in solution ’ [<10K nominal molecular weight (MW)] and that colloidal Pb (10K MW to 0·2 μm)accounted for onlyc. 1% of the dissolved Pb at this station. This small concentration (0·01 nM) of colloidal Pb may be attributed to the low amount of organic carbon associated with colloid size fraction as determined by dissolved organic carbon analyses.The chemical speciation of lead was determined in the dissolved sample and ultrafiltered sub-sample. Differential pulse anodic stripping voltammetry (DPASV) on a thin mercury film (TMF) rotating glassy carbon disk electrode (RGCDE) was used to distinguish the kinetically labile inorganic species (Pb′) from the Pb-chelated by organic ligands (PbLi). Lead titration results were similar for both samples revealing that Pb′, PbLiand excess unbound ligands were present primarily in the ultrafiltrate, rather than in the colloidal phase. The titration data can be interpreted as dissolved Pb being influenced by two classes of Pb-binding ligands. In the dissolved sample, the concentration of the stronger class of ligands was [L1]=0·89±0·35 nM, with a conditional stability constant ofKcondL1,Pb′=3±1×1010M−1. The weaker class was [L2]=12·8±1·9 nM, withKcondL1,Pb′=4±1×108 M−1. The presence of these ligands, in excess of the dissolved Pb, resulted in [Pb′]=7±2 pM and [Pb2+]=0·3 pM (62 pg l−1). While less than 2·4% of the ambient Pb was ‘ in solution ’, it existed chiefly in the form of organic complexes with [PbL1]=0·15 nM and [PbL2]=0·03 nM. More significantly, there were large concentrations of unchelated Pb-binding ligands, (Li′), available to buffer the free Pb2+concentration in the event of perturbations in dissolved Pb. 相似文献
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9.
Widespread Plio-Pleistocene (2.43-0.06 Ma) tephra zones recognised in deep-sea cores from high latitudes (>60°) in the Southern Pacific Ocean were thought to have originated from calc-alkaline rhyolitic eruptions in New Zealand, some 5000 km distant. Electron microprobe analyses of the glasses reveal a wide diversity of alkalic felsic compositions, as well as minor components of basic and intermediate glasses, incompatible with a New Zealand Neogene source but similar to contemporaneous eruptives from the Antarctic region. Most tephra zones are trachytic; seven zones are peralkaline rhyolite. The rhyolitic zones represent a deep-sea record of widespread silicic eruptions from continental Antarctica, possibly Marie Byrd Land. The extent of these rhyolitic zones suggest a greater frequency of large explosive eruptions in Antarctica than previously documented. The coarse grain size of some of the shards (up to 3 mm), their great distance from the closest sources (>1600 km for some cores), and the presence of nonvolcanic ice-rafted debris indicate some of the glasses, especially the more basic compositions, may have been ice-rafted, contrary to previous suggestions of a fallout origin. 相似文献
10.
Dissolved trace element (copper, nickel, cadmium, zinc, cobalt, and iron) concentrations were measured in surface water samples collected from 27 stations in the San Francisco Bay and Sacramento—San Joaquin Delta during April, August and December of 1989. The trace element distributions were relatively similar for all three sampling periods, and evidenced two distinct biogeochemical regimes within the estuarine system. The two regimes were comprised of relatively typical trace element gradients in the northern reach and anthropogenically perturbed gradients in the southern reach of the estuary. These dichotomous trace element distributions were consistent with previous reports on the distributions of nutrients and some other constituents within the estuary.In the northern reach, trace element and dissolved phosphate concentrations were non-conservative. Simple estuarine mixing models indicated substantial internal sources of dissolved copper (46–150%), nickel (250–500%) and cadmium (630–780%) relative to riverine inputs in April and August, and sizable internal sinks for dissolved cobalt (> 99%) and iron (> 70%) during the same periods. Dissolved zinc fluxes varied temporally, with a relatively large (135%) internal source in April and a relatively small (29%) internal sink in August.Concentrations of many trace elements (copper, nickel, cadmium, zinc, and cobalt) in the southern reach were anomalously high relative to concentrations at comparable salinities in the northern reach. Mass balance calculations indicated that those excesses were primarily due to anthropogenic inputs (waste-water discharges and urban runoff) and diagenetic remobilization from benthic sediments. The magnitude of these excesses was amplified by the long hydraulic residence time of dissolved constituents within the South Bay.The influence of other factors was evident throughout the system. Notably, upwelling appeared to elevate substantially dissolved cadmium concentrations at the mouth of the estuary and authigenic flocculation appeared to dominate the cycling of dissolved iron in both the northern and southern reaches of the system. Biological scavenging, geochemical scavenging and diagenic remobilization were also found to be important in different parts of the estuary. Additional complementary information is required to quantify accurately these processes. 相似文献