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1.
Ocean acidification due to anthropogenic CO2 emissions is a dominant driver of long-term changes in pH in the open ocean, raising concern for the future of calcifying organisms, many of which are present in coastal habitats. However, changes in pH in coastal ecosystems result from a multitude of drivers, including impacts from watershed processes, nutrient inputs, and changes in ecosystem structure and metabolism. Interaction between ocean acidification due to anthropogenic CO2 emissions and the dynamic regional to local drivers of coastal ecosystems have resulted in complex regulation of pH in coastal waters. Changes in the watershed can, for example, lead to changes in alkalinity and CO2 fluxes that, together with metabolic processes and oceanic dynamics, yield high-magnitude decadal changes of up to 0.5 units in coastal pH. Metabolism results in strong diel to seasonal fluctuations in pH, with characteristic ranges of 0.3 pH units, with metabolically intense habitats exceeding this range on a daily basis. The intense variability and multiple, complex controls on pH implies that the concept of ocean acidification due to anthropogenic CO2 emissions cannot be transposed to coastal ecosystems directly. Furthermore, in coastal ecosystems, the detection of trends towards acidification is not trivial and the attribution of these changes to anthropogenic CO2 emissions is even more problematic. Coastal ecosystems may show acidification or basification, depending on the balance between the invasion of coastal waters by anthropogenic CO2, watershed export of alkalinity, organic matter and CO2, and changes in the balance between primary production, respiration and calcification rates in response to changes in nutrient inputs and losses of ecosystem components. Hence, we contend that ocean acidification from anthropogenic CO2 is largely an open-ocean syndrome and that a concept of anthropogenic impacts on marine pH, which is applicable across the entire ocean, from coastal to open-ocean environments, provides a superior framework to consider the multiple components of the anthropogenic perturbation of marine pH trajectories. The concept of anthropogenic impacts on seawater pH acknowledges that a regional focus is necessary to predict future trajectories in the pH of coastal waters and points at opportunities to manage these trajectories locally to conserve coastal organisms vulnerable to ocean acidification.  相似文献   

2.
Respiration and calcification rates of the Pacific oyster Crassostrea gigas were measured in a laboratory experiment in the air and underwater, accounting for seasonal variations and individual size, to estimate the effects of this exotic species on annual carbon budgets in the Bay of Brest, France. Respiration and calcification rates changed significantly with season and size. Mean underwater respiration rates, deducted from changes in dissolved inorganic carbon (DIC), were 11.4 μmol DIC g−1 ash-free dry weight (AFDW) h−1 (standard deviation (SD), 4.6) and 32.3 μmol DIC g−1 AFDW h−1 (SD 4.1) for adults (80–110 mm shell length) and juveniles (30–60 mm), respectively. The mean daily contribution of C. gigas underwater respiration (with 14 h per day of immersion on average) to DIC averaged over the Bay of Brest population was 7.0 mmol DIC m−2 day−1 (SD 8.1). Mean aerial CO2 respiration rate, estimated using an infrared gas analyzer, was 0.7 μmol CO2 g−1 AFDW h−1 (SD 0.1) for adults and 1.1 μmol CO2 g−1 AFDW h−1 (SD 0.2) for juveniles, corresponding to a mean daily contribution of 0.4 mmol CO2 m−2 day−1 (SD 0.50) averaged over the Bay of Brest population (with 10 h per day of emersion on average). Mean CaCO3 uptake rates for adults and juveniles were 4.5 μmol CaCO3 g−1 AFDW h−1 (SD 1.7) and 46.9 μmol CaCO3 g−1 AFDW h−1 (SD 29.2), respectively. The mean daily contribution of net calcification in the Bay of Brest C. gigas population to CO2 fluxes during immersion was estimated to be 2.5 mmol CO2 m−2 day−1 (SD 2.9). Total carbon release by this C. gigas population was 39 g C m−2 year−1 and reached 334 g C m−2 year−1 for densely colonized areas with relative contributions by underwater respiration, net calcification, and aerial respiration of 71%, 25%, and 4%, respectively. These observations emphasize the substantial influence of this invasive species on the carbon cycle, including biogenic carbonate production, in coastal ecosystems.  相似文献   

3.
The results of an international interlaboratory proficiency test for the determination of carbonic species are presented. Eight laboratories analysed twelve water samples (four synthetic waters, one lake water, four geothermal waters, one seawater and two petroleum waters) by two methods: (a) individual laboratory analytical procedure and (b) acid–base titration curves in tabular form following a standardised protocol. In case (b), the concentrations of carbonic species were calculated by the organiser using the (1) Hydrologists' method, (2) Geochemists' method and/or (3) initial pH and total alkalinity method. For synthetic waters, the averaged % trueness and precision of measurement of the two methods were (trueness = 7.6, precision = 9.4) and (9.0, 3.4) for total alkalinity, and (6.6, 31.0) and (7.8, 6.1) for carbonic alkalinity, respectively. This indicates that the total alkalinity calculation procedure is in general correct in the individual laboratory method, but the carbonic alkalinity calculation procedure has serious problems. The measurements of total alkalinity for lake and seawaters were in agreement in both the methods; however, the individual laboratory measurement method for geothermal and petroleum waters was conceptually incorrect. Thus, the analytical procedures for the determination of carbonic species were reviewed. To apply the Hydrologists' and/or Geochemists' methods, the location of NaHCO3EP and H2CO3EP is necessary, even for samples with pH lower than that of NaHCO3EP, and a backward titration curve after complete removal of CO2 must be performed. The initial pH and total alkalinity method is appropriate where a complete analysis of species that contribute to the alkalinity is known.  相似文献   

4.
Mangrove ecosystems play an important, but understudied, role in the cycling of carbon in tropical and subtropical coastal ocean environments. In the present study, we examined the diel dynamics of seawater carbon dioxide (CO2) and dissolved oxygen (DO) for a mangrove-dominated marine ecosystem (Mangrove Bay) and an adjacent intracoastal waterway (Ferry Reach) on the island of Bermuda. Spatial and temporal trends in seawater carbonate chemistry and associated variables were assessed from direct measurements of dissolved inorganic carbon, total alkalinity, dissolved oxygen (DO), temperature, and salinity. Diel pCO2 variability was interpolated across hourly wind speed measurements to determine variability in daily CO2 fluxes for the month of October 2007 in Bermuda. From these observations, we estimated rates of net sea to air CO2 exchange for these two coastal ecosystems at 59.8 ± 17.3 in Mangrove Bay and 5.5 ± 1.3 mmol m−2 d−1 in Ferry Reach. These results highlight the potential for large differences in carbonate system functioning and sea-air CO2 flux in adjacent coastal environments. In addition, observation of large diel variability in CO2 system parameters (e.g., mean pCO2: 390–2,841 μatm; mean pHT: 8.05–7.34) underscores the need for careful consideration of diel cycles in long-term sampling regimes and flux estimates.  相似文献   

5.
Rising atmospheric pCO2 and ocean acidification originating from human activities could result in increased dissolution of metastable carbonate minerals in shallow-water marine sediments. In the present study, in situ dissolution of carbonate sedimentary particles in Devil’s Hole, Bermuda, was observed during summer when thermally driven density stratification restricted mixing between the bottom water and the surface mixed layer and microbial decomposition of organic matter in the subthermocline layer produced pCO2 levels similar to or higher than those levels anticipated by the end of the 21st century. Trends in both seawater chemistry and the composition of sediments in Devil’s Hole indicate that Mg-calcite minerals are subject to selective dissolution under conditions of elevated pCO2. The derived rates of dissolution based on observed changes in excess alkalinity and estimates of vertical eddy diffusion ranged from 0.2 mmol to 0.8 mmol CaCO3 m−2 h−1. On a yearly basis, this range corresponds to 175–701 g CaCO3 m−2 year−1; the latter rate is close to 50% of the estimate of the current average global coral reef calcification rate of about 1,500 g CaCO3 m−2 year−1. Considering a reduction in marine calcification of 40% by the year 2100, or 90% by 2300, as a result of surface ocean acidification, the combination of high rates of carbonate dissolution and reduced rates of calcification implies that coral reefs and other carbonate sediment environments within the 21st and following centuries could be subject to a net loss in carbonate material as a result of increasing pCO2 arising from burning of fossil fuels.  相似文献   

6.
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   

7.
The KPB sections at Højerup in Denmark, Agost and Caravaca in Spain and El Kef in Tunisia and (elsewhere in the world) consists of a very thin reddish biogenic calcite-poor smectite-rich “impact” layer overlain by a thicker smectite-rich marl. The massive amount of impact-generated atmospheric CO2 at KPB would have accumulated globally in the ocean surface, leading to acidification and CaCO3 undersaturation. These chemical changes would have induced a low biocalcification of calcareous plankton and a high dissolution of their shells. The biocalcification/dissolution crises may have played a significant role for the low abundance of biogenic calcite in the “impact” layer of the marine boundary clays at Højerup, Agost, Caravaca and El Kef (and elsewhere in the world). Experimental data and observations indicate that the deposition of the “impact” layer probably lasted only a few decades at most.  相似文献   

8.
In Korea, soils adjacent to abandoned mines are commonly contaminated by heavy metals present in mine tailings. Further, the disposal of oyster shell waste by oyster farm industries has been associated with serious environmental problems. In this study, we attempted to remediate cadmium (Cd)- and lead (Pb)-contaminated soils typical of those commonly found adjacent to abandoned mines using oyster shell waste as a soil stabilizer. Natural oyster shell powder (NOSP) and calcined oyster shell powder (COSP) were applied as soil amendments to immobilize Cd and Pb. The primary components of NOSP and COSP are calcium carbonate (CaCO3) and calcium oxide (CaO), respectively. X-ray diffraction, X-ray fluorescence and scanning electron microscope analyses conducted in this study revealed that the calcination of NOSP at 770°C converted the less reactive CaCO3 to the more reactive CaO. The calcination process also decreased the sodium content in COSP, indicating that it was advantageous to use COSP as a liming material in agricultural soil. After 30 days of incubation, we found that the 0.1 N HCl-extractable Cd and Pb contents in soil decreased significantly as a result of an increase in the soil pH and the formation of metal hydroxides. COSP was more effective in immobilizing Cd and Pb in the contaminated soil than NOSP. Overall, the results of this study suggest that oyster shell waste can be recycled into an effective soil ameliorant.  相似文献   

9.
AquaEnv is an integrated software package for aquatic chemical model generation focused on ocean acidification and antropogenic CO2 uptake. However, the package is not restricted to the carbon cycle or the oceans: it calculates, converts, and visualizes information necessary to describe pH, related CO2 air–water exchange, as well as aquatic acid–base chemistry in general for marine, estuarine or freshwater systems. Due to the fact that it includes the relevant acid–base systems, it can also be applied to pore water systems and anoxic waters. AquaEnv is implemented in the open source programming language R , which allows for a flexible and versatile application: AquaEnv ’s functionality can be used stand-alone as well as seamlessly integrated into reactive-transport models in the R modelling environment. Additionally, AquaEnv provides a routine to simulate and investigate titrations of water samples with a strong acid or base, as well as a routine that allows for a determination of total alkalinity and total carbonate values from recorded titration curves using non-linear curve-fitting.  相似文献   

10.
Field experiments on the CO2 flux of alpine meadow soil in the Qilian Mountain were conducted along the elevation gradient during the growing season of 2004 and 2005. The soil CO2 flux was measured using the Li-6400-09 soil respiration chamber attached to the Li-6400 portable photosynthesis system. The effects of water and heat and roots on the soil CO2 flux were statistically analyzed. The results show that soil CO2 flux along the elevation gradient gradually decreases. The soil CO2 flux was low at night, with lowest value occurring between 0200 and 0600 hours, started to rise rapidly during 0700–0830 hours, and then descend during 1600–1830 hours. The peak CO2 efflux appears during 1100–1600 hours. The diurnal average of soil CO2 efflux was between 0.56 ± 0.32 and 2.53 ± 0.76 μmol m−2 s−1. Seasonally, soil CO2 fluxes are relatively high in summer and autumn and low in spring and winter. The soil CO2 efflux, from the highest to the lowest in the ranking order, occurred in July and August (4.736 μmol m−2 s−1), June and September, and May and October, respectively. The soil CO2 efflux during the growing season is positively correlated with soil temperature, root biomass and soil water content.  相似文献   

11.
A field facility located in Bozeman, Montana provides the opportunity to test methods to detect, locate, and quantify potential CO2 leakage from geologic storage sites. From 9 July to 7 August 2008, 0.3 t CO2 day−1 were injected from a 100-m long, ~2.5-m deep horizontal well. Repeated measurements of soil CO2 fluxes on a grid characterized the spatio-temporal evolution of the surface leakage signal and quantified the surface leakage rate. Infrared CO2 concentration sensors installed in the soil at 30 cm depth at 0–10 m from the well and at 4 cm above the ground at 0 and 5 m from the well recorded surface breakthrough of CO2 leakage and migration of CO2 leakage through the soil. Temporal variations in CO2 concentrations were correlated with atmospheric and soil temperature, wind speed, atmospheric pressure, rainfall, and CO2 injection rate.  相似文献   

12.
Willapa Bay has received a great deal of attention in the context of rising atmospheric CO2 and the concomitant effects of changes in bay carbonate chemistry, referred to as ocean acidification, and the potential effects on the bay’s naturalized Pacific oyster (Crassostrea gigas) population and iconic oyster farming industry. Competing environmental stressors, historical variability in the oyster settlement record, and the absence of adequate historical observations of bay-water carbonate chemistry all conspire to cast confusion regarding ocean acidification as the culprit for recent failures in oyster larval settlement. We present the first measurements of the aqueous CO2 partial pressure (PCO2) and the total dissolved carbonic acid (TCO2) at the “fattening line,” a location in the bay that has been previously identified as optimal for both larval oyster retention and growth, and collocated with a long historical time series of larval settlement. Samples were collected from early 2011 through late 2014. These measurements allow the first rigorous characterization of Willapa Bay aragonite mineral saturation state (Ωar), which has been shown to be of leading importance in determining the initial shell formation and growth of larval Crassostrea gigas. Observations show that the bay is usually below Ωar levels that have been associated with poor oyster hatchery production and with chronic effects noted in experimental work. Bay water only briefly rises to favorable Ωar levels and does so out of phase with optimal thermal conditions for spawning. Thermal and carbonate conditions are thus coincidentally favorable for early larval development for only a few weeks at a time each year. The limited concurrent exceedance of thermal and Ωar thresholds suggests the likelihood of high variability in settlement success, as seen in the historical record; however, estimates of the impact of elevated atmospheric CO2 suggest that pre-industrial Ωar conditions were more persistently favorable for larval development and more broadly coincident with thermal optima.  相似文献   

13.
CH4 and CO2 fluxes from a high-cold swamp meadow and an alpine meadow on the Qinghai-Tibetan Plateau, subject to different degrees of degradation, were measured over a 12-month period. Air temperature, soil temperature and moisture, and the depths of the water table and thawing-freezing layer were determined. For swamp meadows, the greater the degradation, the lesser the carbon efflux. CH4 emissions at the nondegraded swamp meadow site were 1.09–3.5 and 2.5–11.27 times greater, and CO2 emissions 1.08–1.69 and 1.41–4.43 times greater, respectively, than those from moderately and severely degraded sites. For alpine meadows, the greater the degradation, the greater the CH4 consumption and CO2 emissions. CH4 consumption at the severely degraded alpine meadow site was 6.6–21 and 1.1–5.25 times greater, and CO2 emissions 1.05–78.5 and 1.04–6.28 times greater, respectively, than those from the nondegraded and moderately degraded sites. The CH4 and CO2 fluxes at both sites were significantly correlated (R 2 > 0.59, P < 0.05) with air temperature, soil temperature, and topsoil (0–5 cm depth) moisture, indicating these to be the main environmental factors affecting such fluxes.  相似文献   

14.
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   

15.
In a natural analog study of risks associated with carbon sequestration, impacts of CO2 on shallow groundwater quality have been measured in a sandstone aquifer in New Mexico, USA. Despite relatively high levels of dissolved CO2, originating from depth and producing geysering at one well, pH depression and consequent trace element mobility are relatively minor effects due to the buffering capacity of the aquifer. However, local contamination due to influx of brackish waters in a subset of wells is significant. Geochemical modeling of major ion concentrations suggests that high alkalinity and carbonate mineral dissolution buffers pH changes due to CO2 influx. Analysis of trends in dissolved trace elements, chloride, and CO2 reveal no evidence of in situ trace element mobilization. There is clear evidence, however, that As, U, and Pb are locally co-transported into the aquifer with CO2-rich brackish water. This study illustrates the role that local geochemical conditions will play in determining the effectiveness of monitoring strategies for CO2 leakage. For example, if buffering is significant, pH monitoring may not effectively detect CO2 leakage. This study also highlights potential complications that CO2 carrier fluids, such as brackish waters, pose in monitoring impacts of geologic sequestration.  相似文献   

16.
Evidence for ocean acidification in the Great Barrier Reef of Australia   总被引：1，自引：0，他引：1  
Geochemical records preserved in the long-lived carbonate skeleton of corals provide one of the few means to reconstruct changes in seawater pH since the commencement of the industrial era. This information is important in not only determining the response of the surface oceans to ocean acidification from enhanced uptake of CO2, but also to better understand the effects of ocean acidification on carbonate secreting organisms such as corals, whose ability to calcify is highly pH dependent. Here we report an ∼200 year δ11B isotopic record, extracted from a long-lived Porites coral from the central Great Barrier Reef of Australia. This record covering the period from 1800 to 2004 was sampled at yearly increments from 1940 to the present and 5-year increments prior to 1940. The δ11B isotopic compositions reflect variations in seawater pH, and the δ13C changes in the carbon composition of surface water due to fossil fuel burning over this period. In addition complementary Ba/Ca, δ18O and Mg/Ca data was obtained providing proxies for terrestrial runoff, salinity and temperature changes over the past 200 years in this region. Positive thermal ionization mass spectrometry (PTIMS) method was utilized in order to enable the highest precision and most accurate measurements of δ11B values. The internal precision and reproducibility for δ11B of our measurements are better than ±0.2‰ (2σ), which translates to a precision of better than ±0.02 pH units. Our results indicate that the long-term pre-industrial variation of seawater pH in this region is partially related to the decadal-interdecadal variability of atmospheric and oceanic anomalies in the Pacific. In the periods around 1940 and 1998 there are also rapid oscillations in δ11B compositions equivalent changes in pH of almost 0.5 U. The 1998 oscillation is co-incident with a major coral bleaching event indicating the sensitivity of skeletal δ11B compositions to loss of zooxanthellate symbionts. Importantly, from the 1940s to the present-day, there is a general overall trend of ocean acidification with pH decreasing by about 0.2-0.3 U, the range being dependent on the value assumed for the fractionation factor α(B3-B4) of the boric acid and borate species in seawater. Correlations of δ11B with δ13C during this interval indicate that the increasing trend towards ocean acidification over the past 60 years in this region is the result of enhanced dissolution of CO2 in surface waters from the rapidly increasing levels of atmospheric CO2, mainly from fossil fuel burning. This suggests that the increased levels of anthropogenic CO2 in atmosphere has already caused a significant trend towards acidification in the oceans during the past decades. Observations of surprisingly large decreases in pH across important carbonate producing regions, such as the Great Barrier Reef of Australia, raise serious concerns about the impact of Greenhouse gas emissions on coral calcification.  相似文献   

17.
An important ecological role ascribed to oysters is the transfer of materials from the water column to the benthos as they feed on suspended particles (seston). This ecosystem service has been often touted as a major reason for many oyster restoration efforts, but empirical characterization and quantification of seston removal rates in the field have been lacking. Changes in chlorophyll a (chl a) concentrations in the water column were measured in May 2005 and June 2006 in South Carolina using in situ fluorometry and laboratory analysis of pumped water samples taken upstream and downstream as water flowed over natural and constructed intertidal oyster reefs. Both methods gave similar results overall, but with wide variability within individual reef datasets. In situ fluorometer data logged at 10 to 30-s intervals for up to 1.3 h over eight different reefs (three natural and five constructed) showed total removal (or uptake) expressed as % removal of chl a ranging from −9.8% to 27.9%, with a mean of 12.9%. Our data indicate that restored shellfish reefs should provide water-quality improvements soon after construction, and the overall impact is probably determined by the size and density of the resident filter feeder populations relative to water flow characteristics over the reef. The measured population-level chl a removal was converted to mean individual clearance rates to allow comparison with previous laboratory studies. Although direct comparisons could not be made due to the small size of oysters on the study reefs (mean shell height, 36.1 mm), our calculated rates (mean, 1.21 L h−1) were similar to published laboratory measured rates for oysters of this size. However, the wide variability in measured removal by the oyster reefs suggests that individual oyster feeding rates in nature may be much more variable than in the laboratory. The proliferation of ecosystem-level models that simulate the impacts of bivalves on water quality based only on laboratory-feeding measurements underscores the importance of further research aimed at determining ecologically realistic feeding rates for oysters in the field. Because in situ methods provide many replicate measurements quickly, they represent a potentially powerful tool for quantifying the effects of oyster reefs, including all suspension-feeding taxa present, on water quality.  相似文献   

18.
Karen A. Merritt  Aria Amirbahman   《Earth》2009,96(1-2):54-66
Considerable recent research has focused on methylmercury (MeHg) cycling within estuarine and coastal marine environments. Because MeHg represents a potent neurotoxin that may magnify in marine foodwebs, it is important to understand the mechanisms and environmental variables that drive or constrain methylation dynamics in these environments. This critical review article explores the mechanisms hypothesized to influence aqueous phase and sediment solid phase MeHg concentrations and depth-specific inorganic Hg (II) (Hgi) methylation rates (MMR) within estuarine and coastal marine environments, and discusses issues of terminology or methodology that complicate mechanism-oriented interpretation of field and laboratory data. Mechanisms discussed in this review article include: 1) the metabolic activity of sulfate reducing bacteria (SRB), the microbial group thought to dominate mercury methylation in these environments; 2) the role that Hgi concentration and/or speciation play in defining depth-specific Hgi methylation rates; and 3) the depth-dependent balance between MeHg production and consumption within the sedimentary environment. As discussed in this critical review article, the hypothesis of SRB community control on the Hgi methylation rate in estuarine and coastal marine environments is broadly supported by the literature. Although Hgi speciation, as a function of porewater inorganic sulfide and/or dissolved organic matter concentration and/or pH, may also play a role in observed variations in MMR, the nature and function of the controlling ligand(s) has not yet been adequately defined. Furthermore, although it is generally recognized that the processes responsible for MeHg production and consumption overlap spatially and/or kinetically in the sedimentary environment, and likely dictate the extent to which MeHg accumulates in the aqueous and/or sediment solid phase, this conceptual interpretation requires refinement, and would benefit greatly from the application of kinetic modeling.  相似文献   

19.
Oysters from paired sites of high and low spatfall at three mid-Chesapeake Bay locations were analyzed for tissue copper and tissue zinc as well as copper in aufwuchs scraped from the upper (right valve) shell surface. Paired sites had no significant differences in oyster tissue copper, aufwuchs copper or oyster tissue copper-zinc ratio. In the laboratory, natural aufwuchs material on oyster shell rapidly concentrated copper up to 10× from copper-enriched estuarine water, with a partition coefficient (Ka) of 0.640 I kg?1. Aufwuchs-sorbed copper resisted depuration, suggesting a strong metal-binding substance in aufwuchs material. Eyed veliger oyster larvae (setting stage) exposed to oyster shell fragments having copper-enriched aufwuchs showed normal setting preference for bottoms and edges of shell surfaces but a slight decrease in total set with increasing aufwuchs copper concentration. Settled oyster spat died or failed metamorphosis with LD50=534 μg Cu g?1 aufwuchs. Since mid-Bay aufwuchs copper concentrations averaged 35.5 μg?1, ranging up to 103 μg g?1, oyster spatfall probably is not affected solely by present natural aufwuchs copper concentrations, but the potential for problems exists.  相似文献   

20.
Miller field of the North Sea has had high concentrations of natural CO2 for ~70 Ma. It is an ideal analog for the long-term fate of CO2 during engineered storage, particularly for formation of carbonate minerals that permanently lock up CO2 in solid form. The Brae Formation reservoir sandstone contains an unusually high quantity of calcite concretions; however, C and O stable isotopic signatures suggest that these are not related to the present-day CO2 charge. Margins of the concretions are corroded, probably because of reduced pH due to CO2 influx. Dispersed calcite cements are also present, some of which postdate the CO2 charge and, therefore, are the products of mineral trapping. It is calculated that only a minority of the reservoired CO2 in Miller (6–24%) has been sequestrated in carbonates, even after 70 Ma of CO2 emplacement. Most of the CO2 accumulation is dissolved in pore fluids. Therefore, in a reservoir similar to the Brae Formation, engineered CO2 storage must rely on physical retention mechanisms because mineral trapping is both incomplete and slow.  相似文献   

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