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1.
Benthic fluxes in two southern California borderland basins have been estimated by modeling water column property gradients, by modeling pore water gradients and by measuring changes in concentration in a benthic chamber. Results have been used to compare the different methods, to establish budgets for biogenic silica and carbon and to estimate rate constants for models of CaCO3 dissolution. In San Pedro Basin, a low oxygen, high sedimentation rate area, fluxes of radon-222 (86 ± 8 atoms m−2 s−1), SiO2 (0.7 ± 0.1 mmol m−2 d−1), alkalinity (1.7 ± 0.3 meq m−2 d−1), TCO2 (1.9 ± 0.3 mmol m−2 d−1) and nitrate (−0.8 ± 0.1 mmol m−2 d−1) measured in a benthic chamber agree within the measurement uncertainty with fluxes estimated from modeling profiles of nutrients and radon obtained in the water column. The diffusive fluxes of radon, SiO2 and TCO2 determined from modeling the sediment and pore water also agree with the other approaches. Approximately 33 ± 13% of the organic carbon and 37 ± 47% of the CaCO3 arriving at the sea floor are recycled. In San Nicolas Basin, which has larger oxygen concentrations and lower sedimentation rates than San Pedro, the fluxes of radon (490 ± 16 atoms m−2 s−1), SiO2 (0.7 ± 0.1 mmol m−2 d−1), alkalinity (1.7 ± 0.3 meq m−2 d−1), TCO2 (1.7 ± 0.2 mmol m−2 d−1), oxygen (−0.7 ± 0.1 mmol m−2 d−1) and nitrate (-0.4 ± 0.1 mmol m−2 d−1) determined from chamber measurements agree with the water column estimates given the uncertainty of the measurements and model estimates. Diffusion from the sediments matches the lander-measured SiO2 and PO43− (0.017 ± 0.002 mmol m−2 d−1) fluxes, but is not sufficient to supply the radon or TCO2 fluxes observed with the lander. In San Nicolas Basin 38 ± 9% of the organic carbon and 43 ± 22% of the CaCO3 are recycled. Approximately 90% of the biogenic silica arriving at the sea floor in each basin is recycled. The rates of CaCO3 dissolution determined from chamber flux measurements and material balances for protons and electrons are compared to those predicted by previously published models of CaCO3 dissolution and this comparison indicates that in situ rates are comparable to those observed in laboratory studies of bulk sediments, but orders of magnitude less than those observed in experiments done with suspended sediments.  相似文献   

2.
Mineralization of organic matter and the subsequent dissolution of calcite were simulated for surface sediments of the upper continental slope off Gabon by using microsensors to measure O2, pH, pCO2 and Ca2+ (in situ), pore-water concentration profiles of NO3−, NH4+, Fe2+, and Mn2+ and SO42− (ex situ), as well as sulfate reduction rates derived from incubation experiments. The transport and reaction model CoTReM was used to simulate the degradation of organic matter by O2, NO3−, Fe(OH)3 and SO42−, reoxidation reactions involving Fe2+ and Mn2+, and precipitation of FeS. Model application revealed an overall rate of organic matter mineralization amounting to 50 μmol C cm−2 yr−1, of which 77% were due to O2, 17% to NO3− and 3% to Fe(OH)3 and 3% to SO42−. The best fit for the pH profile was achieved by adapting three different dissolution rate constants of calcite ranging between 0.01 and 0.5% d−1 and accounting for different calcite phases in the sediment. A reaction order of 4.5 was assumed in the kinetic rate law. A CaCO3 flux to the sediment was estimated to occur at a rate of 42 g m−2 yr−1 in the area of equatorial upwelling. The model predicts a redissolution flux of calcite amounting to 36 g m−2 yr−1, thus indicating that ∼90% of the calcite flux to the sediment is redissolved.  相似文献   

3.
The effects of fish farm activities on sediment biogeochemistry were investigated in Loch Creran (Western Scotland) from March to October 2006. Sediment oxygen uptake rates (SOU) were estimated along an organic matter gradient generated from an Atlantic salmon farm using a combination of in situ techniques: microelectrodes, planar optode and benthic chamber incubations. Sulphide (H2S) and pH distributions in sediment porewater were also measured using in situ microelectrodes, and dissolved inorganic carbon (DIC) fluxes were measured in situ using benthic chambers. Relationships between benthic fluxes, vertical distribution of oxidants and reduced compounds in the sediment were examined as well as bacterial abundance and biomass. Seasonal variations in SOU were relatively low and mainly driven by seasonal temperature variations. The effect of the fish farm on sediment oxygen uptake rate was clearly identified by higher total and diffusive oxygen uptake rates (TOU and DOU, respectively) on impacted stations (TOU: 70 ± 25 mmol O2 m?2 day?1; DOU: 70 ± 32 mmol O2 m?2 day?1 recalculated at the summer temperature), compared with the reference station (TOU: 28.3 ± 5.5 mmol O2 m?2 day?1; DOU: 21.5 ± 4.5 mmol O2 m?2 day?1). At the impacted stations, planar optode images displayed high centimetre scale heterogeneity in oxygen distribution underlining the control of oxygen dynamics by small-scale processes. The organic carbon enrichment led to enhanced sulphate reduction as demonstrated by large vertical H2S concentration gradients in the porewater (from 0 to 1,000 μM in the top 3 cm) at the most impacted site. The impact on ecosystem functions such as bioirrigation was evidenced by a decreasing TOU/DOU ratio, from 1.7 in the non-impacted sediments to 1 in the impacted zone. This trend was related to a shift in the macrofaunal assemblage and an increase in sediment bacterial population. The turnover time of the organic load of the sediment was estimated to be over 6 years.  相似文献   

4.
Mid-shelf sediments off the Oregon coast are characterized as fine sands that trap and remineralize phytodetritus leading to the consumption of significant quantities of dissolved oxygen. Sediment oxygen consumption (SOC) can be delayed from seasonal organic matter inputs because of a transient buildup of reduced constituents during periods of quiescent physical processes. Between 2009 and 2013, benthic oxygen exchange rates were measured using the noninvasive eddy covariance (EC) method five separate times at a single 80-m station. Ancillary measurements included in situ microprofiles of oxygen at the sediment–water interface, and concentration profiles of pore water nutrients and trace metals, and solid-phase organic C and sulfide minerals from cores. Sediment cores were also incubated to derive anaerobic respiration rates. The EC measurements were made during spring, summer, and fall conditions, and they produced average benthic oxygen flux estimates that varied between ?2 and ?15 mmol m?2 d?1. The EC oxygen fluxes were most highly correlated with bottom-sensed, significant wave heights (H s). The relationship with H s was used with an annual record of deepwater swell heights to predict an integrated oxygen consumption rate for the mid-shelf of 1.5 mol m?2 for the upwelling season (May–September) and 6.8 mol m?2 y?1. The annual prediction requires that SOC rates are enhanced in the winter because of sand filtering and pore water advection under large waves, and it counters budgets that assume a dominance of organic matter export from the shelf. Refined budgets will require winter flux measurements and observations from cross-shelf transects over multiple years.  相似文献   

5.
《Geochimica et cosmochimica acta》1999,63(19-20):3349-3356
The calcium cycle, in particular carbonate dissolution, was analyzed in two deep eutrophic lakes, Lago di Lugano (288 m maximum depth) and Sempachersee (87 m) located in Switzerland. A box model approach was used to calculate calcite dissolution in the water column and at the sediment-water interface based on various lake monitoring data such as sediment traps, sediment cores, water and pore-water analysis. A model for stationary conditions allowing the calculation of calcite dissolution in the water column for a given particle size distribution was developed. The relative values of the simulated flux were consistent with sediment trap observations. The best fit of the dissolution rate constant of sinking calcite in Lago di Lugano was on the same order of magnitude (3 · 10−10 kg1/3 s−1) as published laboratory values for this surface controlled process.Both lakes show a similar specific calcite precipitation rate of 170 g Ca m−2 a−1. The diffusive flux across the sediment-water interface amounts to about 15 and 10% of total calcite precipitation in Sempachersee and Lago di Lugano, respectively. However, 61% of the precipitated calcite is dissolved in the water column of Lago di Lugano compared to only 13% in Sempachersee. These results point towards the importance of grain size distributions and settling times in stratified deep waters as the two most important factors determining calcite retention in sediments of hard water lakes.  相似文献   

6.
Variation in 13C/12C-isotope ratios of fracture filling calcite was analyzed in situ to investigate carbon sources and cycling in fractured bedrock. The study was conducted by separating sections of fracture fillings, and analyzing the 13C/12C-ratios with secondary ion mass spectrometry (SIMS). Specifically, the study was aimed at fillings where previously published sulfur isotope data indicated the occurrence of bacterial sulfate reduction. The results showed that the δ13C values of calcite were highly variable, ranging from −53.8‰ to +31.6‰ (VPDB). The analysis also showed high variations within single fillings of up to 39‰. The analyzed calcite fillings were mostly associated with two calcite groups, of which Group 3 represents possible Paleozoic fluid circulation, based on comparison with similar dated coatings within the Baltic Shield and the succeeding Group 1–2 fillings represent late-stage, low temperature mineralization and are possibly late Paleozoic to Quaternary in age. Both generations were associated with pyrite with δ34S values indicative of bacterial sulfate reduction. The δ13C values of calcite, however, were indicative of geochemical environments which were distinct for these generations. The δ13C values of Group 3 calcite varied from −22.1‰ to +11‰, with a distinct peak at −16‰ to −12‰. Furthermore, there were no observable depth dependent trends in the δ13C values of Group 3 calcite. The δ13C values of Group 3 calcite were indicative of organic matter degradation and methanogenesis. In contrast to the Group 3 fillings, the δ13C values of Group 1–2 calcite were highly variable, ranging from −53.8‰ to +31.6‰ and they showed systematic variation with depth. The near surface environment of <30 m (bsl) was characterized by δ13C values indicative of degradation of surface derived organic matter, with δ13C values ranging from −30.3‰ to −5.5‰. The intermediate depth of 34–54 m showed evidence of localized methanotrophic activity seen as anomalously 13C depleted calcite, having δ13C values as low as −53.8‰. At depths of ∼60–400 m, positive δ13C values of up to +31.6‰ in late-stage calcite of Group 1–2 indicated methanogenesis. In comparison, high CH4 concentrations in present day groundwaters are found at depths of >300 m. One sample at a depth of 111 m showed a transition from methanogenetic conditions (calcite bearing methanogenetic signature) to sulfate reducing (precipitation of pyrite on calcite surface), however, the timing of this transition is so far unclear. The results from this study gives indications of the complex nature of sulfur and carbon cycling in fractured crystalline environments and highlights the usefulness of in situ stable isotope analysis.  相似文献   

7.
We present a numerical model to quantify calcite dissolution in the guts of deposit feeding invertebrates. Deposit feeder guts were modeled as constantly stirred reactors (CSTRs) following terminology from digestion theory. Saturation state and dissolution of calcium carbonate were calculated from changes in total dissolved carbon dioxide and alkalinity resulting from sediment passage through the digestive tract, while accounting for dissolution of calcite and respiration of organic carbon. Typical dissolution rates for a gut volume of 1 ml ranged between 0.5-4 mg calcite d−1. Sensitivity analysis revealed gut pH, sediment organic matter (OM) content and OM reactivity to be the critical parameters determining calcite dissolution rate. Carbonate dissolution rate was inversely related to gut pH. However, calcite dissolution was found to be possible even at alkaline gut pH due to respiration by intestinal microbes. The kinetics of calcite dissolution had only marginal influence on daily calcite dissolution rates: Varying the calcite dissolution rate constant κ by six orders of magnitude affected calcite dissolution rates by less than a factor of 10. Calcite dissolution rates were calculated for 4 different hydrographic regimes that differed in their content of sedimentary calcite and OM and furthermore in their OM reactivity. Highest dissolution rates were calculated for the shallow water setting, where relatively high OM content facilitated high microbial respiration rates depressing gut pH. However, dissolution rates for the deep sea setting were only slightly lower, due to greatly elevated ingestion rates resulting from low OM content. As a consequence of much higher faunal abundances, shallow-water benthos is likely to contribute the vast majority of gut-mediated carbonate dissolution. Nevertheless, the fraction of sedimentary calcite that dissolves during one gut passage is probably too small to be observable by simple gravimetric analysis. This may explain the notable scarcity of evidence for gut-mediated carbonate dissolution in the literature to date. Assuming depth-dependent calcite dissolution rates and deposit feeder abundances, we estimate gut-mediated carbonate dissolution to contribute approximately 5% of the annual global sedimentary carbonate dissolution rate, which corresponds to an average calcite dissolution rate of approximately 0.5 mg m−2 d−1 for the entire ocean floor.  相似文献   

8.
The hydrogeochemical and carbon isotope characteristics of the Krka River, Slovenia, were investigated to estimate the carbon transfer from the land ecosystem in the watershed. During the 3-year sampling period (2008–2010), temperature, pH, electrical conductivity, major ion content, dissolved inorganic carbon (DIC) and dissolved organic carbon content, and the isotopic composition of DIC (δ13CDIC) were monitored in the main stream of the Krka River and its tributaries. The major solute composition of analysed waters is dominated by an input of HCO3 ?, Ca2+ and Mg2+ originating from carbonate dissolution. The Mg2+/Ca2+ and Mg2+/HCO3 ? molar ratio values ranging from 0.24 to 0.71 and 0.05 to 0.30, respectively, indicate a high degree of dolomite dissolution relative to calcite. Dissolved CO2 concentrations in the river were up to tenfold supersaturated relative to the atmosphere, resulting in supersaturation with respect to calcite and degassing of CO2 downstream. The δ13C values in river water range from ?15.6 to ?9.4 ‰ and are controlled by the input of tributaries, exchange with atmospheric CO2, degradation of organic matter, and dissolution of carbonates. The mass balance calculations for riverine DIC suggest that the contribution from carbonate dissolution and degradation of organic matter have major influence, whereas the exchange with atmospheric CO2 has minor influence on the inorganic carbon pool in the Krka River.  相似文献   

9.
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10.
《Applied Geochemistry》1997,12(3):291-303
The geochemical effects of microbially mediated degradation of aromatic hydrocarbons were observed as changes in solution composition of an artificial groundwater in packed-sand laboratory columns. Benzene, toluene, and xylene, both individually and in a combined fashion, were used as substrates in biodegradation experiments conducted under oxygenated and anoxic conditions in columns filled with quartz, calcite, or Fe3+-coated quartz sand. Typically, column effluent had increased concentrations of dissolved inorganic C, decreased pH, and decreased concentrations of NO3 and dissolved O2 relative to column influent. Efficiency of CO2 generation was similar for the three different substrates, ranging from 22.5 to 26.6% organic C converted to CO2. When all three substrates were combined, the percentage of CO2 produced fell within the range observed in the single substrate experiments. Nitrate disappearance was more varied as a function of substrate identity, with greatest amounts lost when toluene was the substrate. Calcite dissolved as a result of CO2 generated during the biodegradation reactions, and empirically calculated dissolution rates varied between 1.9 and 4.0 x 10−9 mmol cm−2 s−1. The calcite dissolution rate was slower than the biodegradation rate, as evidenced by excess generation of CO2 relative to Ca2+ production. The decrease in pH was less in experiments with calcite present than in those with quartz sand present due to buffering by calcite dissolution. Dissolution of Fe oxyhydroxides was not observed under any experimental conditions.  相似文献   

11.
Assessing the influence of CO2 on soil and aquifer geochemistry is a task of increasing interest when considering risk assessment for geologic carbon sequestration. Leakage and CO2 ascent can lead to soil acidification and mobilization of potentially toxic metals and metalloids due to desorption or dissolution reactions. We studied the CO2 influence on an Fe(III) (oxyhydr)oxide rich, gleyic Fluvisol sampled in close vicinity to a Czech mofette site and compared the short-term CO2 influence in laboratory experiments with observations on long-term influence at the natural site. Six week batch experiments with/without CO2 gas flow at 3 different temperatures and monitoring of liquid phase metal(loid) concentrations revealed two main short-term mobilization processes. Within 1 h to 1 d after CO2 addition, mobilization of weakly adsorbed metal cations occurred due to surface protonation, most pronounced for Mn (2.5–3.3 fold concentration increase, mobilization rates up to 278 ± 18 μg Mn kgsoil−1 d−1) and strongest at low temperatures. However, total metal(loid) mobilization by abiotic desorption was low. After 1–3 d significant Fe mobilization due to microbially-triggered Fe(III) (oxyhydr)oxide dissolution began and continued throughout the experiment (up to 111 ± 24 fold increase or up to 1.9 ± 0.6 mg Fe kgsoil−1 d−1). Rates increased at higher temperature and with a higher content of organic matter. The Fe(III) mineral dissolution was coupled to co-release of incorporated metal(loid)s, shown for As (up to 16 ± 7 fold, 11 ± 8 μg As kgsoil−1 d−1). At high organic matter content, re-immobilization due to resorption reactions could be observed for Cu. The already low pH (4.5–5.0) did not change significantly during Fe(III) reduction due to buffering from sorption and dissolution reactions, but a drop in redox potential (from > +500 mV to minimum +340 ± 20 mV) occurred due to oxygen depletion. We conclude that microbial processes following CO2 induction into a soil can contribute significantly to metal(loid) mobilization, especially at optimal microbial growth conditions (moderate temperature, high organic carbon content) and should be considered for carbon sequestration monitoring and risk assessment.  相似文献   

12.
Biogeochemical processes occurring near the sediment-water interface of shallow (≈20 m) water sediments lying beneath the Mississippi River plume on the Louisiana shelf were studied using benthic chambers and sediment cores. Three sites were chosen with distinctly different characteristics. One was overlain by oxic water where aerobic respiration dominated organic matter remineralization. The second site was overlain by oxic water but organic matter remineralization was dominated by sulfate reduction. The third site was overlain by hypoxic water and aerobic remineralization was of minor significance. Major differences were observed in the fluxes of CO2(17–56 mmol m−2 d−1), O2(2–56 mmol m−2 d−1) and nutrients (e.g., NH4 +, 2.6–4.2 mmol m−2 d−1) across the sediment-water interface, and the relative importance of different electron acceptors, even though the sites were in close proximity and at nearly the same water depth. Large variations in the efficiency of organic-C burial (3%–51%) were also calculated based on a simplified model of the relationships between the fraction of organic matter remineralized by sulfate reduction and the fraction of sulfide produced that is buried as pyrite. These observations demonstrate the high degree of spatial heterogeneity of benthic biogeochemistry in this important near-deltaic environment.  相似文献   

13.
Streams and rivers are major exporters of C and other dissolved materials from watersheds to coastal waters. In streams and rivers, substantial amounts of terrigenous organic C is metabolized and degassed as CO2 to the atmosphere. A long-term evaluation of CO2 dynamics in streams is essential for understanding factors controlling CO2 dynamics in streams in response to changes in climate and land-use. Long-term changes in the partial pressure of CO2 (pCO2) were computed in the Anacostia River and the lower Potomac River in the Chesapeake Bay watershed. Long-term estimates were made using routine monitoring data of pH, total alkalinity, and dissolved nutrients from 1985 to 2006 at 14 stations. Longitudinal variability in pCO2 dynamics was also investigated along these rivers downstream of the urban Washington D.C. metropolitan area. Both rivers were supersaturated with CO2 with respect to atmospheric CO2 levels (392 μatm) and the highly urbanized Anacostia waters (202–9694 μatm) were more supersaturated than the Potomac waters (557–3800 μatm). Long-term variability in pCO2 values may be due to changes in river metabolism and organic matter and nutrient loadings. Both rivers exchange significant amounts of CO2 with the atmosphere (i.e., Anacostia at 0.2–72 mmol m−2 d−1 and Potomac at 0.12–24 mmol m−2 d−1), implying that waterways receiving organic matter and nutrient subsidies from urbanized landscapes have the potential to increase river metabolism and atmospheric CO2 fluxes along the freshwater–estuarine continuum.  相似文献   

14.
Benthic fluxes of soluble reactive phosphorus (SRP) and dissolved inorganic carbon (DIC) were measured in situ using autonomous landers in the Gulf of Finland in the Baltic Sea, on four expeditions between 2002 and 2005. These measurements together with model estimates of bottom water oxygen conditions were used to compute the magnitude of the yearly integrated benthic SRP flux (also called internal phosphorus load). The yearly integrated benthic SRP flux was found to be almost 10 times larger than the external (river and land sources) phosphorus load. The average SRP flux was 1.25?±?0.56?mmol?m?2?d?1 on anoxic bottoms, and ?0.01?±?0.08?mmol?m?2?d?1 on oxic bottoms. The bottom water oxygen conditions determined whether the SRP flux was in a high or low regime, and degradation of organic matter (as estimated from benthic DIC fluxes) correlated positively with SRP fluxes on anoxic bottoms. From this correlation, we estimated a potential increase in phosphorus flux of 0.69?±?0.26?mmol?m?2?d?1 from presently oxic bottoms, if they would turn anoxic. An almost full annual data set of in situ bottom water oxygen measurements showed high variability of oxygen concentration. Because of this, an estimate of the time which the sediments were exposed to oxygenated overlying bottom water was computed using a coupled thermohydrodynamic ocean?Csea and ecosystem model. Total phosphorus burial rates were calculated from vertical profiles of total phosphorus in sediment and sediment accumulation rates. Recycling and burial efficiencies for phosphorus of 97 and 3%, respectively, were estimated for anoxic accumulation bottoms from a benthic mass balance, which was based on the measured effluxes and burial rates.  相似文献   

15.
《Applied Geochemistry》2004,19(3):323-334
In the present study the distribution of TBT between solid and water phase as a function of several parameters was determined. Two types of clay minerals (Na-montmorillonite SWy and kaolinite KGa) and quartz sand were used as sorbents in conventional batch experiments. Sorption coefficients (Kd) followed the order montmorillonite (89 l/kg) > kaolinite (51 l/kg) > quartz (25 l/kg), while for sorption coefficients normalized to the surface area (Kd′) an opposite trend was observed, with the lowest value determined for montmorillonite (2.79 × 10−3 l/m2) and the highest for quartz sand (8.04 × 10−2 l/m2). The results demonstrate that numerous environmental parameters influence the adsorption process of TBT, such as solid/solution ratio, clay content and salinity. Another important factor governing TBT adsorption is pH, because it affects both the TBT species in the water phase as well as the surface properties of the mineral phase. The maximum of TBT adsorption onto clays was always around pH 6–7. According to the data, it is evident that the content of organic matter in the solid phase plays an important role on TBT adsorption, either as particulate organic matter (POM) or organic matter adsorbed to mineral particles (AOM). Experiments were carried out with well characterized organic matter and the results showed a linear increase of Kd from 51 up to 2700 l/kg upon the addition of 5% of particulate organic matter to pure phased kaolinite. TBT adsorption onto mineral surfaces, which were previously enriched with adsorbed organic matter, was investigated at different pH. The present study points to the importance of identifying and characterizing sorbents and envrionmental conditions, in order to predict and model TBT distribution in natural systems.  相似文献   

16.
Biogeochemical processes were investigated in alpine river—Kamni?ka Bistrica River (North Slovenia), which represents an ideal natural laboratory for studying anthropogenic impacts in catchments with high weathering capacity. The Kamni?ka Bistrica River water chemistry is dominated by HCO3 ?, Ca2+ and Mg2+, and Ca2+/Mg2+ molar ratios indicate that calcite weathering is the major source of solutes to the river system. The Kamni?ka Bistrica River and its tributaries are oversaturated with respect to calcite and dolomite. pCO2 concentrations were on average up to 25 times over atmospheric values. δ13CDIC values ranged from ?12.7 to ?2.7 ‰, controlled by biogeochemical processes in the catchment and within the stream; carbonate dissolution is the most important biogeochemical process affecting carbon isotopes in the upstream portions of the catchment, while carbonate dissolution and organic matter degradation control carbon isotope signatures downstream. Contributions of DIC from various biogeochemical processes were determined using steady state equations for different sampling seasons at the mouth of the Kamni?ka Bistrica River; results indicate that: (1) 1.9–2.2 % of DIC came from exchange with atmospheric CO2, (2) 0–27.5 % of DIC came from degradation of organic matter, (3) 25.4–41.5 % of DIC came from dissolution of carbonates and (4) 33–85 % of DIC came from tributaries. δ15N values of nitrate ranged from ?5.2 ‰ at the headwater spring to 9.8 ‰ in the lower reaches. Higher δ15N values in the lower reaches of the river suggest anthropogenic pollution from agricultural activity. Based on seasonal and longitudinal changes of chemical and isotopic indicators of carbon and nitrogen in Kamni?ka Bistrica River, it can be concluded that seasonal changes are observed (higher concentrations are detected at low discharge conditions) and it turns from pristine alpine river to anthropogenic influenced river in central flow.  相似文献   

17.
《Applied Geochemistry》1998,13(2):177-184
Calcium carbonate is one of the most common and important scale-forming minerals in oilfield produced water, but the kinetics of CaCO3 precipitation has been ignored in most scale prediction models because of the lack of reliable precipitation rate model. There are none in the open literature for oilfield conditions (temperature > 100°C, pressure > 200 bar and salinity > 0.5 mol kg− 1). In this work the kinetics of calcite (CaCO3) precipitation from high salinity waters (up to 2 mol kg−1) have been studied by a pH-free-drift method in a closed water system. This method. is much easier to operate than the often used steady-state method. The experimental results indicate that the calcite precipitation rate is not only affected by the solution CaCO3 saturation level, but also by the solution pH, ionic strength and the concentration ratios of Ca to HCO3− ions (CCa2+/CHCO3−). When the concentration ratios of Ca to HCO3− ions are close to their chemical stoichiometric ratio of 0.5, the calcite growth from a supersaturated solution is believed to be surface reaction controlled. However, at higher CCa2+CHCO3− ratios, the transportation of the lattice ions to calcite crystal surface has to be considered.  相似文献   

18.
《Applied Geochemistry》1999,14(7):927-938
The tunnel excavation at the Äspö Hard Rock Laboratory opened several fracture zones at various depths in the crystalline bedrock. One of these zones is the `Redox zone', a vertical fracture zone penetrated at 70 m depth. Except for the tunnel intersection, several boreholes were drilled to intersect the zone at various depths (ranging from 5 to 70 m) and distances from the tunnel. The response in groundwater chemistry to the opening of the zone has been monitored in these boreholes during 3 a, starting in 1991 and for the boreholes at 70 m depth the monitoring is still ongoing. The water chemistry during this monitoring can be largely explained by mixing between fresh water and native saline groundwater (4900 ppm Cl−). An increase in HCO−3 was recorded, which was interpreted as due to anaerobic respiration. This was supported by 14C-contents in dissolved organic Carbon and HCO−3, indicating that recent organic C is transported into the zone and oxidised to CO2. This study exemplifies the use of 14C-analyses of HCO−3 in order to trace different C sources contributing to the HCO−3 in the groundwater. Three sources were identified: (1) dissolved CO2, dominantly soil-CO2 possibly with some contribution of atmospheric CO2; (2) dissolution of calcite, with low 14C content, which dominantly occurs in the near-surface recharge area; and (3) oxidation of organic material through anaerobic respiration. Corrections for 14C and HCO−3 in the native saline water made it possible to determine 2 different fresh water components corresponding to different flow paths. The C isotope data are in accordance with the results from the tracer test and the groundwater flow model, and support that the extensive build up of HCO3− does not mainly takes place locally within the zone but is transported into the zone by dominantly lateral flow. The results from the monitoring showed that new hydrochemical stability is established, which also comprises the interaction between the organic and inorganic C cycles.  相似文献   

19.
The characteristics and formation mechanism of calcite cements in the tight sandstone of the Jurassic Lianggaoshan Formation in the northeastern Central Sichuan Basin were analysed using petrographic and isotopic techniques. In the tight sandstone of the Lianggaoshan Formation, cements are mostly calcite and occur as poikilitic, pore-filling, fracture-filling and replacement of clastic particles. Contents of Al, Si, Fe and Mn in the poikilitic calcites are significantly less than that in the dissolution pore-filling and metasomatic calcites. Three stages (early, middle and late) of authigenic calcites correspond to temperature ranges of <60, 60–100 and ≥100?°C, respectively, with most calcite cements formed under lower temperature (<100?°C) conditions. The δ18O values of the early–middle authigenic calcites are in equilibrium with connate water, and the δ18O values of late calcites are depleted in 18O indicating equilibrium at higher temperatures. The early authigenic calcites precipitated in a relatively open system associated with CO2 from bacterial fermentation at an immature to low-mature stage, and a Ca2+- and alkaline-rich environment owing to hydration–hydrolysis and dissolution of silicate minerals during phase A of eodiagenesis. The middle–late authigenic calcites precipitated in a relatively closed system with CO2 from decarboxylation of organic acids and Ca2+ from dissolution of silicate minerals and transformation of clay minerals during phase B of eodiagenesis to mesodiagenesis. Calcite cements mainly occur in the medium and fine sandstones of sand flats and beach bars. Authigenic calcite dissolution is extremely weak, and calcite cementation is pore-space destructive.  相似文献   

20.
The variation of major and rare earth elements and yttrium (REY) in the monomictic hardwater Lake Tiberias during the wet and dry seasons of the hydrological year was studied in two profiles. The average volume and Cl concentration of the known and unknown saline inflows of 1.6 × 107 m3 and 1.2 × 109 mol are derived by closing both balances. This brine corresponds to a mixture of 83% of groundwater from Cretaceous aquifers and 17% of very saline deep brine. Taking cycling of calcite in the hypolimnion into account, the settling rate of authigenic calcite is estimated to be 3.3 mol m−2 a−1.In the stratified lake of the dry season dissolved inorganic carbon increases by 490 μM at the thermo-/chemocline due to microbial reduction of SO42−, NO3−, chemical reduction of Fe(III) and MnO2 colloids, and cycling of calcite in the hypolimnion. REY distribution in the stratified water column is dominantly controlled by coprecipitation with calcite, hydrous ferric oxides and MnO2 in the epilimnion and cycling of these compounds in the hypolimnion. The positive Ce anomaly in the hypolimnetic water is produced by cycling of MnO2. The simulation of the increase of REY in the hypolimnion reveals that hydrous ferric and manganese oxides only play a negligible role except Ce. Only about 10% of REY from cycled matter enhance REY in solution. Most of the released REY are adsorbed by particular matter and thus settling on the floor of the lake.Different from Na, U, SO42− and SiO2, the other elements, in particular REY, increase in the mixed water column from the top to the lower third and mostly decrease thereafter toward the bottom in the mixed lake during the wet season. The behavior of REY is caused by some cycling of calcite and pH-dependent re-equilibration of REY bound to hydrous ferric and manganese oxides adsorbed by particular matter.  相似文献   

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