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1.
Subterranean estuaries are characterized by the mixing of terrestrially derived groundwater and seawater in a coastal aquifer. Subterranean estuaries, like their river water-seawater counterparts on the surface of the earth, represent a major, but less visible, hydrological and geochemical interface between the continents and the ocean. This article is the first in a two-part series on the biogeochemistry of the subterranean estuary at the head of Waquoit Bay (Cape Cod, MA, USA). The pore-water distributions of salinity, Fe and Mn establish the salt and redox framework of this subterranean estuary. The biogeochemistry of Fe, Mn, P, Ba, U and Th will be addressed from the perspective of the sediment composition. A second article will focus on the groundwater and pore-water chemistries of Fe, Mn, U and Ba.Three sediment cores were collected from the head of Waquoit Bay where the coastal aquifer consists of permeable sandy sediment. A selective dissolution method was used to measure the concentrations of P, Ba, U and Th that are associated with “amorphous (hydr)oxides of iron and manganese” and “crystalline Fe and Mn (hydr)oxides.” The deeper sections of the cores are characterized by large amounts of iron (hydr)oxides that are precipitated onto organic C-poor quartz sand from high-salinity pore waters rich in dissolved ferrous iron. Unlike Fe (hydr)oxides, which increase with depth, the Mn (hydr)oxides display midcore maxima. This type of vertical stratification is consistent with redox-controlled diagenesis in which Mn (hydr)oxides are formed at shallower depths than iron (hydr)oxides. P and Th are enriched in the deep sections of the cores, consistent with their well-documented affinity for Fe (hydr)oxides. In contrast, the downcore distribution of Ba, especially in core 3, more closely tracks the concentration of Mn (hydr)oxides. Even though Mn (hydr)oxides are 200-300 times less abundant than Fe (hydr)oxides in the cores, Mn (hydr)oxides are known to have an affinity for Ba which is many orders of magnitude greater than iron (hydr)oxides. Hence, the downcore distribution of Ba in Fe (hydr)oxide rich sediments is most probably controlled by the presence of Mn (hydr)oxides. U is enriched in the upper zones of the cores, consistent with the formation of highly reducing near-surface sediments in the intertidal zone at the head of the Bay. Hence, the recirculation of seawater through this type of subterranean estuary, coupled with the abiotic and/or biotic reduction of soluble U(VI) to insoluble U(IV), leads to the sediments acting as a oceanic net sink of U. These results highlight the importance of permeable sediments as hosts to a wide range of biogeochemical reactions, which may be impacting geochemical budgets on scales ranging from coastal aquifers to the continental shelf.  相似文献   

2.
Organic-rich sediment samples collected from a transect within, and below, the Oman Margin oxygen minimum zone (OMZ) were analysed using a sequential leaching technique to characterise the diagenetic behaviour and speciation of Mn and Fe in operationally defined sediment host fractions. Trace metals showed distinct diagenetic behaviour in the two contrasting environments that were sampled. The absence of non-detrital Mn in the cores below the OMZ site is attributed to the lack of easily reducible oxides in surficial sediments and to the reduction and export of any moderately reducible aged oxides. The reactive form of solid phase Mn showed a classic feature of enrichment in the upper layer of the sediments at the abyssal site, reflecting the presence of an oxidising sedimentary layer which acts as a Mn trap during its recycling. The diagenetic Mn enrichment was inferred from typical downcore colour changes and an upward-increasing Mn content in the upper core sections. An easily reducible Fe oxide layer was observed in the abyssal sediments at an identical depth to the Mn enrichment suggesting that Fe associated with Mn oxides also has undergone sub-oxic diagenesis. However, the association of Fe with organic matter did not indicate diagenetic modification; i.e., the binding strength of the metal with organic materials appears to be sufficiently strong to preserve the trace metal. The speciation signature of non-detrital Fe differed from that of Mn. The association of Fe with organic matter suggests that this metal does not undergo diagenetic modification and is preserved in abyssal sediments. The contrasting behaviour of Mn and Fe observed between cores within the OMZ were particularly interesting. Another interesting observation was that, for cores below the OMZ, the iron oxides were associated with the Mn-oxide peak, rather than deeper in the sediments as observed by earlier studies in the Atlantic [Froelich et al. (1979). Geochim. et Cosmochim Acta 43, 1075–1090].This revised version was published online in May 2005 with corrections to the article title.  相似文献   

3.
The concentrations of authigenic phases of Cd, Re, U, and Mo increase with depth in four 45-cm-long sediment box cores collected along the axis of the Laurentian Trough, Gulf of St. Lawrence. Average authigenic accumulation rates, estimated from element inventories, are similar to rates in other continental margin environments. Strong regional variations in sediment accumulation rate and sulfide concentration have little influence on the accumulation rates of Cd and Re. This suggests that slow precipitation kinetics controls the accumulation of Cd and Re in these sediments. The accumulation rate of authigenic U is more variable; it may be tied to the kinetics of microbially mediated U reduction and be controlled by the availability of reactive organic matter. Authigenic Mo is distinguished by a sharp subsurface concentration minimum, above which Mo cycles with manganese. Mo released to pore water upon reduction of Mn oxides diffuses downward and enriches the subsurface sediment. Mo accumulates most rapidly in the sediment with the highest sulfide content. Slow conversion of molybdate to thiomolybdate may explain the much slower Mo accumulation rate in the less sulfidic sediments. A component of authigenic Mo accumulates with pyrite in an approximately constant Mo:Fe ratio. The accumulation rate of pyrite and associated Mo is insensitive to AVS abundance. Pyrite formation may be limited by the reactivity of iron oxide minerals.  相似文献   

4.
Four sediment cores representing adjacent mudflat and mangrove sub-environments of middle estuary (Shastri) were analyzed for sand, silt, clay, and organic carbon. Total metal concentration of iron (Fe), manganese (Mn), nickel (Ni), zinc (Zn), chromium (Cr), copper (Cu), cobalt (Co), and lead (Pb) and chemical speciation of Fe, Mn, and Co on selected samples was also carried out on mudflat cores. The sediments in the upper middle estuary were found to be deposited under highly varying hydrodynamic energy conditions; whereas lower middle estuary experienced relatively stable hydrodynamic energy conditions with time. The tributary joining the river near the upper middle estuary is found to be responsible for the addition of enhanced organic carbon and metal concentrations. Speciation study indicated Fe and Co are from natural lithogenic origin while Mn is derived from anthropogenic sources. Higher Mn and Co than apparent effects threshold can pose a high risk of toxicity to organisms associated with these sediments.  相似文献   

5.
This research tests the hypothesis that trace metals respond to the extent of reducing conditions in a predictable way. We describe pore water and sediment measurements of iron (Fe), manganese (Mn), vanadium (V), uranium (U), rhenium (Re), and molybdenum (Mo) along a transect off Washington State (USA). Sediments become less reducing away from the continent, and the stations have a range of oxygen penetration depths (depth to unmeasurable O2 concentration) varying from a few millimeters to five centimeters. When oxygen penetrates ∼1 cm or less, Fe is reduced in the pore waters but reoxidized near the sediment-water interface, preventing a flux of Fe2+ to overlying waters, whereas Mn oxides are reduced and Mn2+ diffuses to overlying waters. Both Re and U authigenically accumulate in sediments. Only at the most reducing location, where the oxygen penetrates 0.3 cm below the sediment-water interface, does the surface 30 cm of sediments become reducing enough to authigenically accumulate Mo.Stations in close proximity to the Juan de Fuca Ridge crest are enriched in Mn and Fe from hydrothermal plume processes. Both V and Mo clearly associate with Mn cycling, whereas U may be associating with either Mn oxides and/or Fe oxyhydroxides. Rhenium is uncomplicated by adsorption to Mn oxides and/or Fe oxyhydroxides, and Re accumulation in sediments appears to be due solely to the extent of reducing conditions. Therefore, authigenic sediment Re enrichment appears to be the best indicator for intermediate reducing conditions, where oxygen penetrates less than ∼1 cm below the sediment-water interface, when coupled with negligible authigenic Mo enrichment.  相似文献   

6.
Manganese nodules and manganese carbonate concretions occur in the upper 10–15 cm of the Recent sediments of Loch Fyne, Argyllshire in water depths of 180–200 m. The nodules are spherical, a few mm to 3 cm in diameter, and consist of a black, Mn-rich core and a thin, red, Fe-rich rim. The carbonate occurs as irregular concretions, 0.5–8 cm in size, and as a cement in irregular nodule and shell fragment aggregates. It partially replaces some nodule material and clastic silicate inclusions, but does not affect aragonitic and calcitic shell fragments.The nodules are approximately 75% pure oxides and contain 30% Mn and 4% Fe. In the cores, the principal mineral phase is todorokite, with a Mn/Fe ratio of 17. The rim consists of X-ray amorphous Fe and Mn oxides with a Mn/Fe ratio of 0.66. The cores are enriched, relative to Al, in K, Ba, Co, Mo, Ni and Sr while the rims contain more P, Ti, As, Pb, Y and Zn.The manganese carbonate has the composition (Mn47.7 Ca45.1 Mg7.2) CO3. Apart from Cu, all minor elements are excluded from significant substitution in the carbonate lattice.Manganese nodules and carbonates form diagenetically within the Recent sediments of Loch Fyne. This accounts for the high Mn/Fe ratios in the oxide phases and the abundance of manganese carbonate concretions. Mn concentrations in the interstitial waters of sediment cores are high (ca. 10 ppm) as also, by inference, are the dissolved carbonate concentrations.  相似文献   

7.
Sediment cores from the middle to lower slope of the southern continental margin of Australia between the Great Australian Bight and western Tasmania are compared in terms of marine and terrigenous input signals during the Holocene. The mass accumulation rates of carbonate, organic carbon, biogenic Ba, and Al are corrected for lateral sediment input (focusing), using the inventory of excess 230Th in the sediment normalised to its known production rate in the water column above each site. The biogenic signal is generally higher in the eastern part of the southern margin probably due to enhanced productivity associated with seasonal upwelling off southeastern South Australia and the proximity of the Subtropical Front, which passes just south of Tasmania. The input of Al, representing the terrigenous signal, is also higher in this region reflecting the close proximity of river runoff from the mountainous catchment of southeastern Australia. The distribution pattern of Mn and authigenic U, together with pore‐water profiles of Mn++, indicate diagenetic reactions driven by the oxidation of buried organic carbon in an oxic to suboxic environment. Whereas Mn is reduced at depth and diffuses upwards to become immobilised in a Mn‐rich surface layer, U is derived from seawater and diffuses downward into the sediment, driven by reduction and precipitation at a depth below the reduction zone of Mn. The estimated removal rate of U from seawater by this process is within the range of U removal measured in hemipelagic sediments from other areas, and supports the proposition that hemipelagic sediments are a major sink of U in the global ocean. Unlike Mn, the depth profile of sedimentary Fe appears to be little affected by diagenesis, suggesting that little of the total Fe inventory in the sediment is remobilised and redistributed as soluble Fe.  相似文献   

8.
The technique of diffusive gradients in thin films (DGT) was applied to obtain high-resolution vertical profiles of trace metals in sediment porewater of a eutrophic lake, Lake Chaohu. All sampling sediments were under anaerobic conditions with Eh values below 0, the redox potential profile in M4 was relatively stable, and higher Eh values in M4 than that in M1 were observed due to hydrodynamic effects. Fe, Mn and As exhibited closely corresponding profiles due to the co-release of Fe and Mn oxides and the reduction of As. Higher Fe and Mn concentrations and lower As concentrations were observed in M1 of the western half-lake than those in M4 of the eastern half-lake due to different sources and metal contamination levels in the two regions. Cu and Zn showed increasing concentrations similar to Mn and Fe at 1–2 cm depth of sediments, while DGT measured Co, Ni, Cd and Pb concentrations decreased down to 3–4 cm in the profiles. Co, Ni, Cu, Zn, Cd and Pb showed insignificant regional concentration variances in the western and eastern half-lakes. According to the R(C DGT/C centrifugation) values, the rank order of metal labilities decrease as follows: Fe (>1) > Cu, Pb, Zn (>0.9) > Co, Ni, Cd (>0.3) > Mn, As (>0.1).  相似文献   

9.
We analyzed 77 surface sediment samples collected in the southwestern East/Japan Sea from the Korea Strait through the Ulleung Basin and the Korea Plateau for grain size, calcium carbonate, organic carbon, and major (Na, Mg, Al, Fe, K, Ca, and Ti) and trace elements (P, Mn, Sr, Li, Sc, V, Cr, Co, Ni, Zn, Cu, and Pb).The chemical composition of the surface sediments was found to be highly variable spatially. Cluster analysis of surface sediment chemical compositions indicated five major geochemical sedimentary environments: basin, lower slope, coast and upper slope, inner shelf, and outer shelf. Continental-shelf sediments were rich in shell fragments and had relict and coarse-grained characteristics. Recent fine-grained sediments were only distributed in coastal, slope, and basin areas. Concentrations of Al, K, Ca, Ti, Cr, and Sc were highest in the coastal and upper slope areas and decreased with water depth. Elemental ratios using major and trace elements indicated that coastal and upper slope detrital sediments were mixtures of sediments derived from the Changjiang (Yangtze) and Nakdong Rivers. Although the concentrations of organic carbon, P, Mn, V, Co, Ni, Cu, and Pb increased with water depth, their distribution patterns indicated authigenic (V, Cu, and Pb) and diagenetic (Fe, P, Mn, Co, and Ni) origins. The distribution pattern with water depth suggested that the chemical composition of surface sediment was determined by sedimentologic and geochemical processes, such as the supply of detrital and biogenic materials, and authigenic and post-depositional diagenetic processes in sediments.  相似文献   

10.
The top thirty centimeters of sediment at two sites in the eastern equatorial Pacific contain evidence of post-depositional remobilization of Mn, Fe, Co, Ni, Cu, and Zn. Remobilization takes place as Mn and Fe oxyhydroxides are released to the pore water during the microbially-mediated decomposition of organic matter. Precipitation of the dissolved metals in near-surface more oxic strata controls the solid-phase distribution of Mn, Fe, and Zn. The solid-phase redistribution of Co and Ni requires only suitable material for readsorption. Comparison of pore water fluxes with solid-phase metal distributions in the solid sediment indicates no loss of dissolved metal to the overlying water column at the present time. Loss of Mn during the Quaternary is indicated by the composition of the sediments, however. Leaching experiments suggest that portions of the mobile Mn, Fe, Co, Ni, and Cu are fixed by incorporation in authigenic smectite in the surficial sediments.  相似文献   

11.
Surficial sediment samples were collected at 47 stations in Little Traverse Bay, Lake Michigan, to determine the geochemical associations between certain rare earth elements (REE's) and trace metals. Each sample was analyzed for carbonate carbon, organic carbon, grain size, and the elements Al, Ca, Ce, Co, Cr, Eu, Fe, Hf, La, and Mn. Two distinct Ce subpopulatins were identified by graphical analysis, and an R-mode factor analysis was applied to data from the “enriched” Ce subpopulation (18 samples). Results show that the REE's and trace metals are primarily enriched in the authigenic phase of these sediments. Partial correlation analyses indicate that the REE's are primarily associated with hydrous Fe oxides relative to organic matter in this phase. The ratio of Ce/La concentrations increased markedly from the bay margins to the central trough of the bay, indicating that Ce, similar to Fe, exhibits a variable oxidation state in the authigenic phase of nearshore fine-grained sediments. The results of the present study suggest that the REE's and trace metals behave coherently in the authigenic phase of recent lacustrine sediments, and the REE's may be useful as geochemical tracers to differentiate between trace metal enrichments in surface sediments as a result of diagenesis and pollution loadings.  相似文献   

12.
Oxygen profiles were measured in the sediments of the Gulf of Aqaba (Red Sea), an oligotrophic marine system affected by episodic seasonal flash floods and intense aeolian dry deposition. Sediment cores were retrieved from shallow (15–45 m), intermediate (250–561 m) and deep (700 m) water sites of south–north and east–west transects. Dissolved oxygen concentrations were measured simultaneously by using microelectrodes and microoptodes immediately after sampling and after transportation. Oxygen penetration depths were found to increase from 2 to 5 mm at the shallow water sites with sandy permeable sediments to 10–21 mm at the deeper sites with cohesive muddy sediments. This increase corresponds to decrease in oxygen diffusive fluxes at the sediment–water interface and oxygen consumption rates with depth. Oxygen consumption rates exhibit local maxima at the oxic–anoxic sediment boundary, which may be attributed to oxygen reduction coupled to oxidation of dissolved Fe(II) and Mn(II) at deep and intermediate water sites and of hydrogen sulfide at shallow water sites. Microelectrodes and microoptodes measurements of cohesive sediments from deep and intermediate water sites yielded similar results. By comparison, the microoptodes displayed more robust measurements than microelectrodes in sandy near-shore sediments. This was attributed to their flexible fiber structure that is less likely to break or to abruptly displace sand particles. After transportation of sediment cores from Eilat to Beer Sheva followed by ≤?24-h storage, no changes in oxygen fluxes and consumption rates were detected.  相似文献   

13.
We present inorganic geochemical analyses of pore waters and sediments of two Late Quaternary sediment cores from the western Arctic Ocean (southern Mendeleev Ridge, RV Polarstern Expedition ARK-XXIII/3), focussing on the composition and origin of distinct, brown-colored, Mn-rich sediment layers. Carbonate enrichments occur in association with these layers as peaks in Ca/Al, Mg/Al, Sr/Al and Sr/Mg, suggesting enhanced input of both ice-rafted and biogenic carbonate. For the first time, we show that the Mn-rich layers layers are also consistently enriched in the scavenged trace metals Co, Cu, Mo and Ni. Distinct bioturbation patterns, specifically well-defined brown burrows into the underlying sediments, suggest these metal enrichments formed close to the sediment-water interface. The geochemical signature of these metal- and carbonate-rich layers most probably documents formation under warmer climate conditions with an intensified continental hydrological cycle and only seasonal sea ice cover. Both rivers and sea ice delivered trace metals to the Arctic Ocean, while enhanced seasonal productivity exported reactive organic matter to the sea floor. The coeval deposition of organic matter, Mn (oxyhydr)oxides and trace metals triggered intense diagenetic Mn cycling at the sediment-water interface. These processes resulted in the formation of Mn and trace metal enrichments, and the degradation of labile organic matter. With the onset of cooler conditions, reduced riverine runoff and/or a solid sea ice cover terminated the input of riverine trace metal and fresh organic matter, resulting in deposition of grayish-yellowish, metal-poor sediments. Oxygen depletion of Arctic bottom waters under these cooler conditions is not supported by our data, and did not cause the sedimentary Mn distribution. While the original composition and texture of the brown layers resulted from specific climatic conditions and corresponding diagenetic processes, pore water data show that diagenetic Mn redistribution is still affecting the organic-poor deeper sediments. Given persistent steady state conditions, purely authigenic Mn-rich brown layers may form, while others may be partly or completely dissolved. The degree of diagenetic Mn redistribution largely depends on the depositional environment, the Mn and organic matter availability, and apparently affected the Co/Mo ratios of Mn-rich layers. Thus, brown Arctic layers are not necessarily synchronous features, and should not be correlated across the Arctic Ocean without additional age control.  相似文献   

14.
We used a combination of porewater and solid phase analysis, as well as a series of sediment incubations, to quantify organic carbon oxidation by dissimilatory Fe reduction, Mn reduction, and sulfate reduction, in sediments from the Skagerrak (located off the northeast coast of Jutland, Denmark). In the deep portion of the basin, surface Mn enrichments reached 3.5 wt%, and Mn reduction was the only important anaerobic carbon oxidation process in the upper 10 cm of the sediment. In the less Mn-rich sediments from intermediate depths in the basin, Fe reduction ranged from somewhat less, to far more important than sulfate reduction. Most of the Mn reduction in these sediments may have been coupled to the oxidation of acid volatile sulfides (AVS), rather than to dissimilatory reduction. High rates of metal oxide reduction at all sites were driven by active recycling of both Fe and Mn, encouraged by bioturbation. Recycling was so rapid that the residence time of Fe and Mn oxides, with respect to reduction, ranged from 70-250 days. These results require that, on average, an atom of Fe or Mn is oxidized and reduced between 100-300 times before ultimate burial into the sediment. We observed that dissolved Mn2+ was completely removed onto fully oxidized Mn oxides until the oxidation level of the oxides was reduced to about 3.8, presumably reflecting the saturation by Mn2+ of highly reactive surface adsorption sites. Fully oxidized Mn oxides in sediments, then, may act as a cap preventing Mn2+ escape. We speculate that in shallow sediments of the Skagerrak, surface Mn oxides are present in a somewhat reduced oxidation level (< 3.8) allowing Mn2+ to escape, and perhaps providing the Mn2+ which enriches sediments of the deep basin.  相似文献   

15.
The islands of New Caledonia are largely composed of ultrabasic rocks (peridotites). severily weathered, rich in Fe, Mn and Co, and where several ore deposits of Ni and Cr are extensively mined. Sediment cores from the bay of Dumbea, in the south of the main island, and from the northern part of the lagoon (Belep Islands), less affected by the mining activities, were analyzed for their mineral composition and metal concentrations. In the surficial sediments, oxides and silicates, including Fe serpentine and smectites, undergo rapid transformation or neoformation in a short time, in particular in the confined bay of Dumbea. Fe is largely present as goethite, and in deeper layers (60–100 cm) as hematite and magnetite. Chromite can be identified at each horizon. The metal concentrations decrease from the near shore areas, in particular the vicinity of the Dumbea river mouth to the open part of the lagoon. This trend is more important for Ni than for Fe or Cr. Fe ranges from 3.5 to 9% (dry weight), Ni from 200 to 2000 μg/g, Cr from 700 to 2000 μg/g, Co from 20 to 150 μg/g and Mn from 130 to 900 μg/g; yet the concentrations are lower than concentrations found in the ultrabasic rocks or laterites of the watershed. To try to understand the behavior of metals during the sedimentation-diagenesis events, we evaluated the sediment accumulation rate, and used different sequential leaching procedures. Fe, Mn, Ni, Cr and Co are mainly present as, or bound to, oxides or oxyhydroxides, even in the deeper layers ( > 100 cm) where the organic content is relatively high (about 6% of organic C). Metals are mainly transported from the land to the lagoon as oxides and dispersed in the lagoon sediments, where they are diluted with a large amount of carbonaceous sediment. During diagenesis, a significant part of Mn, Co and Ni are dissolved; but, unlike Mn and Co, which seem to coprecipitate with carbonate, most of the Ni is released into the waters of the lagoon. Apparently no horizon of the sediment has undergone significant in-situ metal enrichment.  相似文献   

16.
We present a detailed study of the co-diagenesis of Fe and P in hydrothermal plume fallout sediments from ∼19°S on the southern East Pacific Rise. Three distal sediment cores from 340-1130 km from the ridge crest, collected during DSDP Leg 92, were analysed for solid phase Fe and P associations using sequential chemical extraction techniques. The sediments at all sites are enriched in hydrothermal Fe (oxyhydr)oxides, but during diagenesis a large proportion of the primary ferrihydrite precipitates are transformed to the more stable mineral form of goethite and to a lesser extent to clay minerals, resulting in the release to solution of scavenged P. However, a significant proportion of this P is retained within the sediment, by incorporation into secondary goethite, by precipitation as authigenic apatite, and by readsorption to Fe (oxyhydr)oxides. Molar P/Fe ratios for these sediments are significantly lower than those measured in plume particles from more northern localities along the southern East Pacific Rise, and show a distinct downcore decrease to a depth of ∼12 m. Molar P/Fe ratios are then relatively constant to a depth of ∼35 m. The Fe and P speciation data indicate that diagenetic modification of the sediments is largely complete by a depth of 2.5 m, and thus depth trends in molar P/Fe ratios can not solely be explained by losses of P from the sediment by diffusion to the overlying water column during early diagenesis. Instead, these sediments are likely recording changes in dissolved P concentrations off the SEPR, possibly as a result of redistribution of nutrients in response to changes in oceanic circulation over the last 10 million years. Furthermore, the relatively low molar P/Fe ratios observed throughout these sediments are not necessarily solely due to losses of scavenged P by diffusion to the overlying water column during diagenesis, but may also reflect post-depositional oxidation of pyrite originating from the volatile-rich vents of the southern East Pacific Rise. This study suggests that the molar P/Fe ratio of oxic Fe-rich sediments may serve as a proxy of relative changes in paleoseawater phosphate concentrations, particularly if Fe sulfide minerals are not an important component during transport and deposition.  相似文献   

17.
Subterranean estuary occupies the transition zone between hypoxic fresh groundwater and oxic seawater, and between terrestrial and marine sediment deposits. Consequently, we hypothesize, in a subterranean estuary, biogeochemical reactions of Fe respond to submarine groundwater discharge (SGD) and sea level rise. Porewater and sediment samples were collected across a 30-m wide freshwater discharge zone of the Indian River Lagoon (Florida, USA) subterranean estuary, and at a site 250 m offshore. Porewater Fe concentrations range from 0.5 μM at the shoreline and 250 m offshore to about 286 μM at the freshwater-saltwater boundary. Sediment sulfur and porewater sulfide maxima occur in near-surface OC-rich black sediments of marine origin, and dissolved Fe maxima occur in underlying OC-poor orange sediments of terrestrial origin. Freshwater SGD flow rates decrease offshore from around 1 to 0.1 cm/day, while bioirrigation exchange deepens with distance from about 10 cm at the shoreline to about 40 cm at the freshwater-saltwater boundary. DOC concentrations increase from around 75 μM at the shoreline to as much as 700 μM at the freshwater-saltwater boundary as a result of labile marine carbon inputs from marine SGD. This labile DOC reduces Fe-oxides, which in conjunction with slow discharge of SGD at the boundary, allows dissolved Fe to accumulate. Upward advection of fresh SGD carries dissolved Fe from the Fe-oxide reduction zone to the sulfate reduction zone, where dissolved Fe precipitates as Fe-sulfides. Saturation models of Fe-sulfides indicate some fractions of these Fe-sulfides get dissolved near the sediment-water interface, where bioirrigation exchanges oxic surface water. The estimated dissolved Fe flux is approximately 0.84 μM Fe/day per meter of shoreline to lagoon surface waters. Accelerated sea level rise predictions are thus likely to increase the Fe flux to surface waters and local primary productivity, particularly along coastlines where groundwater discharges through sediments.  相似文献   

18.
福建沿岸晚更新世地层中微体古生物化石较为缺乏,极大限制了对该区晚第四纪海侵过程的深入研究。针对这一问题,本研究以闽北2个海湾内的第四纪钻孔为研究对象,通过有孔虫化石以及沉积成因的地球化学元素(Sr/Ba、Mn/Fe)分析,结合三沙湾表层沉积物相应指标,探讨沉积成因的地球化学元素指示海侵地层的可行性。结果显示,2个海湾钻孔的晚第四纪地层中均发育3套疑似海相深灰色黏土层,其中开放海湾霞浦湾钻孔底部黏土层中缺失有孔虫,半封闭海湾三沙湾钻孔中有孔虫仅出现于顶部黏土层中。这3层黏土层的Sr/ Ba值远大于1,和现代潮滩—河口湾体系相近,且出现的海相沟鞭藻和自生黄铁矿为典型的海相地层特征。基于已有的OSL和AMS14C年龄框架,这3层海侵层分别对应于MIS5、MIS3和MIS1期,Sr/Ba和Mn/Fe均值从MIS5到MIS1期不断增大,结合现代潮滩-河口湾体系指标,表明从MIS5到MIS1期海侵强度的增加。由此可见,沉积成因地球化学元素指标可以有效辨识闽北海湾晚更新世海侵地层,这将有助于进一步了解该区晚第四纪海侵过程及其控制因素。  相似文献   

19.
Processes of authigenic manganese ore formation in sediments of the northern equatorial Pacific are considered on the basis of study of the surface layer (<2 mm) of ferromanganese nodule and four micronodule size fractions from the associated surface sediment (0–7 cm). Inhomogeneity of the nodule composition is shown. The Mn/Fe ratio is maximal in samples taken from the lateral sectors of nodule at the water-sediment interface. Compositional differences of nodules are related to the preferential accumulation of microelements in iron oxyhydroxides (P, Sr, Pb, U, Bi, Th, Y, and REE), manganese hydroxides (Co, Ni, Cu, Zn, Cd, Mo, Tl, W), and lithogenous component trapped during nodule growth (Ga, Rb, Ba, and Cs). The Ce accumulation in the REE composition is maximal in the upper and lower parts of the nodule characterized by the minimal Mn/Fe values. The compositional comparison of manganese micronodules and surface layers of the nodule demonstrated that the micronodule material was subjected to a more intense reworking during the diagenesis of sediments. The micronodules are characterized by higher Mn/Fe and P/Fe ratios but lower Ni/Cu and Co/Ni ratios. The micronodules and nodules do not differ in terms of contents of Ce and Th that are least mobile elements during the diagenesis of elements. Differences in the chemical composition of micronodules and nodules are related not only to the additional input of Mn in the process of diagenesis, but also to the transformation of iron oxyhydroxides after the removal of Mn from the close association with Fe formed in the suspended matter at the stage of sedimentation.  相似文献   

20.
Vertical profiles from the water column, including the maximum turbidity zone (MTZ) to the consolidated sediment were sampled in September 2000 in the freshwater reaches of the Gironde Estuary during a complete neap tide-spring tide cycle. The vertical distributions of dissolved major redox parameters and metals (Mn, Fe, Cd, Cu, V, Co, Ni, Mo, and U) were determined. Reactive particulate metal fractions were also determined from selective leaching. The studied system is characterized by density layers functioning at different time-scales, consisting of two mobile layers, i.e., the liquid (LM) and the soft mud (SM), overlying consolidated sediments (CS). This results in a three-zone diagenetic regime where (1) O2 dynamics are fast enough to show depletion in the rapidly mixed LM sequence (tidal time-scale), (2) denitrification occurs on the weekly time-scale mixing SM sequence, and (3) the Mn, Fe, and sulfate cycling occurs in the CS layer (annual time-scale). The studied trace metals show differential behavior during early diagenesis: (1) Cd, Cu, and V are released into pore water preferentially from organic matter in the SM, (2) Co, Ni, and U are released in the CS from Mn and Fe oxides during reductive dissolution, and (3) Mo from both processes. Transient conditions (i.e., oscillations of redox fronts and reoxidation processes), due to the dynamics of the mobile layers, strongly influence the trace metal distributions as inducing resolubilization (Cd, Cu, and Mo). In the CS, authigenic metal phases accumulate, either by direct precipitation with sulfides (Cu, Cd) or co-precipitation with Fe-sulfides (Mo). Microbially mediated reduction of Fe oxides is proposed to control U removal from pore water by reduction of U(VI) to U(IV) at depth. However, a significant fraction of the trace metals is trapped in the sediment in exchangeable forms, and therefore is susceptible to be mobilized due to resuspension of estuarine sediment during strong river flood periods and/or dredging activities.  相似文献   

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