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$Diagenetic fractionation of Ge and Si in reducing sediments$

Title: Diagenetic fractionation of Ge and Si in reducing sediments,
Description: The average Ge/Si ratio in the ocean is determined by the budgets for each of these elements. Previous budget formulations have assumed that the only important sink for both elements is burial as opal, based on studies of the Si cycle and the close oceanic coupling observed between inorganic Ge and Si distributions. However, these budgets implied two paradoxes: (1) hydrothermal flow through ocean ridges is smaller than predicted by other tracers, and (2) the lower Ge/Si ratio of opal deposited during glacial times compared to that deposited during interglacial times required enhanced weathering during cooler, drier climates. Both paradoxes could be resolved if a significant sedimentary sink for Ge other than opal burial could be identified, and the objective of this study was to search for one. Two pore water profiles collected in Equatorial Pacific sediments show that Ge and Si behave similarly in the upper 10 cm of sediment, indicating no evidence for a significant non-opal sink for Ge in oxic sediments. By contrast, profiles in several cores from the California Margin demonstrate that in reducing sediments, Ge diagenesis is poorly coupled to Si diagenesis: significant Ge removal is evident, both downcore and sometimes in the near-surface. Benthic flux chamber measurements at three continental slope stations, all with an oxic layer less than 1 cm thick and large iron gradients in near-surface pore waters, showed that 55 ± 9% of the Ge released by opal dissolution is sequestered. However, at two locations with anoxic sediments but little pore water Fe+2 in the upper 2 cm, flux measurements indicated little fractionation from the oceanic ratio during diagnesis, implicating the importance of iron for fractionating Ge from Si during diagenesis. If the Ge sequestration observed in the iron-rich CA margin sediments is typical of all slope sediments (using a depth range of 200-1000 m), then the Ge sink is sufficient to bring the hydrothermal budget based on Ge into concurrence with that based on other tracers. The temporal variation in oceanic Ge/Si could be explained if Ge and Si inputs remain constant and the effective diagenetic fractionation of Ge increases by a factor of 2-3 during glacial times. Increased fractionation would require that glacial periods are characterized by increased opal dissolution in iron-rich reducing sediments; this could be caused by (1) thinning of the oxygenated sediment layer in response to decreased bottom water oxygen concentrations or increased rain of organics to the sea floor, (2) increased rain of iron-rich detrital sediments in areas receiving high opal rain, (3) increased rain of opal to sediments in margin areas. If the oceanic Ge/Si ratio reflects increased rain of diatom opal or organic carbon in margin areas during glacial periods, it may indicate an increase in the efficiency of the biological pump for CO2 during glacial times. Copyright (C) 2000 Elsevier Science Ltd., Cited By (since 1996):38, Oceanography, ,
Author: Hammond, McManus, Berelson, Meredith, Klinkhammer, Coale
Date: 2000-01-01T00:00:00Z

Title: Biogenic matter diagenesis on the sea floor,
Description: Benthic chamber measurements of the reactants and products involved with biogenic matter diagenesis (oxygen, ammonium, nitrate, silicate, phosphate, TCO2, alkalinity) were used to define fluxes of these solutes into and out of the sediments off southern and central California. Onshore to offshore transects indicate many similarities in benthic fluxes between these regions. The pattern of benthic organic carbon oxidation as a function of water depth, combined with published sediment trap records, suggest that the supply of organic carbon from vertical rain can just meet the sedimentary carbon oxidation + burial demand for the central California region between the depths 100-3500 m. However, there is not enough organic carbon raining through the upper water column to support its oxidation and burial in the basins off southern California. Lateral transport and focusing of refractory carbon within these basins is proposed to account for the carbon buried. The organic carbon burial efficiency is greater off southern California (40-60%) compared to central California (2-20%), even though carbon rain rates are comparable. Oxygen uptake rates are not sensitive to bottom water oxygen concentrations nor to the bulk wt. % organic carbon in surficial sediments. Nitrate uptake rates are well defined by the depth of oxygen penetration into the sediments and the overlying water column nitrate concentration. Nitrate uptake accounts for about 50% of the total denitrification taking place in shelf sediments and denitrification (0.1-1.0 mmolN/m2d) occurs throughout the entire study region. The ratio of carbon oxidized to opal dissolved on the sea floor is constant (0.8 ± 0.2) through a wide range of depths, supporting the hypothesis that opal dissolution kinetics may be dominated by a highly reactive phase. Sea floor carbonate dissolution is negligible within the oxygen minimum zone and reaches maximal rates just above and below this zone (0.2-2.0 mmol/m2d)., Cited By (since 1996):72, Oceanography, ,
Author: Berelson, McManus, Coale, Johnson, Kilgore, Burdige, Pilskaln
Date: 1996-01-01T00:00:00Z

Title: Cobalt and copper distributions in the waters of Santa Monica Basin, California,
Description: The trace metals cobalt and copper are removed from the oceans interior by scavenging on to particle surfaces, but the mechanisms for removal of these two metals are probably quite different. Cobalt appears to be scavenged by manganese oxide particles, whereas organic compounds are the main carrier phase for copper. Remobilization of these metals in marine sediments therefore proceeds by different pathways. The differences in the pathways of remobilization are accentuated in oxygen-deficient environments: manganese oxide reduction is accelerated at low oxygen levels and organic carbon is preserved. Cobalt fluxes from sediments underlying oxygen-deficient waters should be enhanced and copper fluxes reduced. We report here measurements of the cobalt and copper distributions in the waters of an oxygen-deficient marine basin in the Southern California Bight. Cobalt concentrations near the bottom are raised four times above the background level, whereas copper concentrations show no increase. These measurements confirm features of existing models for the oceanic cycles of these metals., Cited By (since 1996):18, Oceanography, CODEN: NATUA, ,
Author: Johnson, Stout, Berelson, Sakamoto-Arnold
Date: 1988-01-01T00:00:00Z

Title: Benthic manganese fluxes along the Oregon-California continental shelf and slope
Description: Here we examine the factors that influence the manganese (Mn) benthic flux from eastern North Pacific marine sediments, with a primary emphasis on continental shelf locations off Oregon and California and studies that involve the use of in situ benthic chambers. Typical shelf-to-shallow margin (<~350m) sites have benthic Mn efflux rates that average ~8±5μmolm-2d-1. In contrast, for the Eel River continental shelf region the benthic Mn efflux can be an order of magnitude higher than other shelf settings with benthic effluxes exceeding ~50μmolm-2d-1. Based on prior work and some new results, continental margin and slope sites (350-~4000m) have benthic Mn efflux rates that average ~1±1μmolm-2d-1. The combination of the benthic flux and Mn solid-phase data, indicate that for the continental shelf off the Umpqua and Eel Rivers, approximately 15±10% of the total Mn that is delivered to the seafloor is remobilized. The compiled data set shows that the benthic Mn efflux co-varies with the organic carbon oxidation rate with a Mn to organic carbon oxidation (Cox) ratio of ~0.8mmol Mn mol-1. Although this ratio can be as high as ~5 for some Eel River sites, the generally close correspondence between Mn and organic carbon implies that the organic carbon oxidation rate exerts some primary control over the rate of the Mn efflux. The amount of organic carbon oxidized by Mn-oxides, however, represents a small fraction (i.e., generally <1%) of the total organic carbon oxidized in these seafloor sediments. © 2012 Elsevier Ltd., Cited By (since 1996):5, Oceanography, CODEN: CSHRD
Author: McManus, Berelson, Severmann, Johnson, Hammond, Roy, Coale
Date: 2012-01-01T00:00:00Z

Title: A time series of benthic flux measurements from Monterey Bay, CA,
Description: In situ incubation chamber measurements of benthic nutrient recycling rates were made on the Monterey Bay shelf at 100m during various years and seasons. Variability in nutrient (Si, PO 4 2+, NH 3, NO 3 -) and trace metal (Mn, Fe (II), Cu) fluxes correlate with variability in the amount of organic carbon oxidized on the sea floor. Patterns of primary productivity show a mid-year maxima, consistent with the timing of increased rates of benthic C org and opal recycling. High rates of C org rain to the shelf promote nitrate consumption at a rate that equals or exceeds ammonia efflux. Low rates of C org rain promote greater efflux of DIN; thus these margin sediments provide a negative feedback to local productivity cycles. The efflux of iron (II) from shelf sediments is sufficient to support > 100% of new production, yet Fe flux is positively correlated with C org recycling which lags the maximum in new production. On account of this time lag, diagenetically recycled Fe is not likely a micro-nutrient trigger of new production, but could serve as a positive feedback. Bio-irrigation rates are seasonally variable by 30% but maximal during the maximum productivity months. © 2003 Elsevier Science Ltd. All rights reserved., Cited By (since 1996):65, CODEN: CSHRD, , , Oceanography
Author: Berelson, McManus, Coale, Johnson, Burdige, Kilgore, Colodner, Chavez, Kudela, Boucher
Date: 2003-01-01T00:00:00Z

Title: Cadmium flux in Los Angeles/Long Beach harbours and at sites along the California continental margin,
Description: Fluxes of dissolved cadmium were measured in situ using benthic flux chambers at stations in Los Angeles/Long Beach harbour and at sites on the California continental margin. Cadmium fluxes ranged from -0.212 to 0.118 μmol m-2 d-1 indicating that Cd flux may either be into or out of sediments. Correlations between Cd flux and carbon oxidation rate and between carbon oxidation rate and sulfate reduction indicate that anaerobic microbial degradation was the major process controlling both the sign and the magnitude of cadmium fluxes at stations in Los Angeles and Long Beach harbours. A simple box model based on sediment fluxes and water column concentrations indicates cadmium has a residence time of 47 days within the Los Angeles/Long Beach harbour system, similar to the hydraulic residence time. Sedimentary flux is, therefore, sufficient to account for water column cadmium concentration in inner harbour areas, suggesting that the sediments are the dominant source and sink of cadmium in these areas of the harbour. Comparison of the cadmium: phosphate ratio for the Los Angeles/Long Beach harbour water column with those reported for the northeast Pacific suggests that distributions of Cd in the study area were elevated over expected values but appear to be dominated by natural physical and biogeochemical processes. © 2001 Academic Press., Cited By (since 1996):9, Oceanography, CODEN: ECSSD, ,
Author: Colbert, Coale, Berelson, Johnson
Date: 2001-01-01T00:00:00Z