Soil CO2 flux measurements in volcanic and geothermal areas     

《Applied Geochemistry》1998,13(5):543-552

The accumulation chamber methodology allows one to obtain reliable values of the soil CO₂ flux, ϕ_{soil CO2}, in the range 0.2 to over 10 000 g m⁻² d⁻¹, as proven by both laboratory tests and field surveys in geothermal and volcanic areas. A strong negative correlation is observed between Δϕ_{soil CO2}/Δt and ΔP_atm/Δt. Maps of classes of log ϕ_{soil CO2} for the northern sector of Vulcano Island, Solfatara of Pozzuoli, Nea Kameni Islet and Yanbajain geothermal field evidence that active faults and fractures act as uprising channels of deep, CO₂-rich geothermal or magmatic gases. The total diffuse CO₂ output was evaluated for each surveyed area.  相似文献   

Time and temperature dependency of carbon dioxide triggered metal(loid) mobilization in soil     

《Applied Geochemistry》2016

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 kg_soil⁻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 kg_soil⁻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 kg_soil⁻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   

Analysis of the spatial and temporal changes in soil CO<Subscript>2</Subscript> flux in alpine meadow of Qilian Mountain     

Zongqiang Chang  Qi Feng  Jianhua Si  Yonghong Su  Haiyang Xi  Jianlin Li 《Environmental Geology》2009,58(3):483-490

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   

Factors affecting the dissolution kinetics of volcanic ash soils: dependencies on pH,CO2, and oxalate     

《Applied Geochemistry》2004,19(8):1217-1232

Laboratory experiments were conducted with volcanic ash soils from Mammoth Mountain, California to examine the dependence of soil dissolution rates on pH and CO₂ (in batch experiments) and on oxalate (in flow-through experiments). In all experiments, an initial period of rapid dissolution was observed followed by steady-state dissolution. A decrease in the specific surface area of the soil samples, ranging from 50% to 80%, was observed; this decrease occurred during the period of rapid, initial dissolution. Steady-state dissolution rates, normalized to specific surface areas determined at the conclusion of the batch experiments, ranged from 0.03 μmol Si m⁻² h⁻¹ at pH 2.78 in the batch experiments to 0.009 μmol Si m⁻² h⁻¹ at pH 4 in the flow-through experiments. Over the pH range of 2.78–4.0, the dissolution rates exhibited a fractional order dependence on pH of 0.47 for rates determined from H⁺ consumption data and 0.27 for rates determined from Si release data. Experiments at ambient and 1 atm CO₂ demonstrated that dissolution rates were independent of CO₂ within experimental error at both pH 2.78 and 4.0. Dissolution at pH 4.0 was enhanced by addition of 1 mM oxalate. These observations provide insight into how the rates of soil weathering may be changing in areas on the flanks of Mammoth Mountain where concentrations of soil CO₂ have been elevated over the last decade. This release of magmatic CO₂ has depressed the soil pH and killed all vegetation (thus possibly changing the organic acid composition). These indirect effects of CO₂ may be enhancing the weathering of these volcanic ash soils but a strong direct effect of CO₂ can be excluded.  相似文献   

Spatiotemporal changes in CO<Subscript>2</Subscript> emissions during the second ZERT injection,August–September 2008     

James E. Amonette  Jonathan L. Barr  Laura M. Dobeck  Kadie Gullickson  Stephen J. Walsh 《Environmental Earth Sciences》2010,60(2):263-272

This study reports the first field test of a multi-channel, auto-dilution, steady-state, soil–CO₂ flux monitoring system being developed to help understand the pathways by which fugitive CO₂ from a geologic sequestration site migrates to the surface. The test was conducted from late August through mid-October 2008 at the Zero Emissions Research and Technology project site located in Bozeman, MT. Twenty steady-state and five non-steady-state flux chambers were installed in a 10 × 15 m area, one boundary of which was directly above a shallow (2-m depth) horizontal injection well located 0.5 m below the water table. A total flux of 52 kg CO₂ day⁻¹ was injected into the well for 13 days and the efflux from the soil was monitored by the chambers before, during, and for 33 days after the injection. The results showed a rapid increase in soil efflux once injection started, with maximal values reached within 3–7 days in most chambers. Efflux returned to background levels within a similar time period after injection ceased. A radial efflux pattern was observed to at least 2 m from the injection well, and evidence for movement of the CO₂ plume during the injection, presumably due to groundwater flow, was seen. The steady-state chambers yielded very stable data, but threefold to fivefold higher fluxes than the non-steady-state chambers. The higher fluxes were attributed to vacuum induced in the steady-state chambers by narrow vent tubes. High winds resulted in significant decreases in measured soil CO₂ efflux, presumably by enhancing efflux from soil outside the chambers.  相似文献   

Greenhouse gas emissions from soils—A review     

《Chemie der Erde / Geochemistry》2016,76(3):327-352

Soils act as sources and sinks for greenhouse gases (GHG) such as carbon dioxide (CO₂), methane (CH₄), and nitrous oxide (N₂O). Since both storage and emission capacities may be large, precise quantifications are needed to obtain reliable global budgets that are necessary for land-use management (agriculture, forestry), global change and for climate research. This paper discusses exclusively the soil emission-related processes and their influencing parameters. It reviews soil emission studies involving the most important land-cover types and climate zones and introduces important measuring systems for soil emissions. It addresses current shortcomings and the obvious bias towards northern hemispheric data.When using a conservative average of 300 mg CO₂e m⁻² h⁻¹ (based on our literature review), this leads to global annual net soil emissions of ≥350 Pg CO₂e (CO₂e = CO₂ equivalents = total effect of all GHG normalized to CO₂). This corresponds to roughly 21% of the global soil C and N pools. For comparison, 33.4 Pg CO₂ are being emitted annually by fossil fuel combustion and the cement industry.  相似文献   

Long-term pCO2 dynamics in rivers in the Chesapeake Bay watershed     

《Applied Geochemistry》2013

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   

Dynamics of CO<Subscript>2</Subscript> fluxes and concentrations during a shallow subsurface CO<Subscript>2</Subscript> release     

Jennifer L. Lewicki  George E. Hilley  Laura Dobeck  Lee Spangler 《Environmental Earth Sciences》2010,60(2):285-297

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   

Assessment of soil moisture influence on CO2 flux: a laboratory experiment     

Romina Sanci  Héctor O. Panarello  Héctor A. Ostera 《Environmental Geology》2009,58(3):491-497

Accurate measurements to assess the influence of soil moisture on CO₂ flux requires the absolute estimates of soil CO₂ flux. Thus, it was constructed a calibration system where CO₂ with fixed concentration flowed through the different porous material. Previous to measurement, in order to verify the performance and reliability of a closed dynamic chamber, different discontinuous air-mixing rates and times were tested. The CO₂ flux was estimated through sequential lectures and the best fit for flux measurements was obtained taking short readings every 3 min, during a total time of 12 min (R ² = 0.99). The best mixing rate was attained for 250 mL min⁻¹, allowing 25 s of mixing previous to CO₂ extraction for an infrared gas analyzer. The deviation of the measured values for dry sand from the reference CO₂ flux (0.097 and 0.071 g m⁻² min⁻¹) was 5 and 7%. On dry sandy loam soil (SLS) the deviation was 2%. The measured fluxes decreased 73 and 22% with content moisture of 20 and 10% (sand), and 78% with content moisture of 31% (SLS). This work allowed to estimate how much the measured emission rates deviate from the true ones for the specified chamber and sampling conditions.  相似文献   

Use of mineral/solution equilibrium calculations to assess the potential for carnotite precipitation from groundwater in the Texas Panhandle,USA     

《Applied Geochemistry》2016

This study investigated the potential for the uranium mineral carnotite (K₂(UO₂)₂(VO₄)₂·3H₂O) to precipitate from evaporating groundwater in the Texas Panhandle region of the United States. The evolution of groundwater chemistry during evaporation was modeled with the USGS geochemical code PHREEQC using water-quality data from 100 groundwater wells downloaded from the USGS National Water Information System (NWIS) database. While most modeled groundwater compositions precipitated calcite upon evaporation, not all groundwater became saturated with respect to carnotite with the system open to CO₂. Thus, the formation of calcite is not a necessary condition for carnotite to form. Rather, the determining factor in achieving carnotite saturation was the evolution of groundwater chemistry during evaporation following calcite precipitation. Modeling in this study showed that if the initial major-ion groundwater composition was dominated by calcium-magnesium-sulfate (>70 precent Ca + Mg and >50 percent SO₄ + Cl) or calcium-magnesium-bicarbonate (>70 percent Ca + Mg and <70 percent HCO₃ + CO₃) and following the precipitation of calcite, the concentration of calcium was greater than the carbonate alkalinity (2mCa⁺² > mHCO₃⁻ + 2mCO₃⁻²) carnotite saturation was achieved. If, however, the initial major-ion groundwater composition is sodium-bicarbonate (varying amounts of Na, 40–100 percent Na), calcium-sodium-sulfate, or calcium-magnesium-bicarbonate composition (>70 percent HCO₃ + CO₃) and following the precipitation of calcite, the concentration of calcium was less than the carbonate alkalinity (2mCa⁺² < mHCO₃^- + 2mCO₃⁻²) carnotite saturation was not achieved. In systems open to CO_2, carnotite saturation occurred in most samples in evaporation amounts ranging from 95 percent to 99 percent with the partial pressure of CO₂ ranging from 10^−3.5 to 10^−2.5 atm. Carnotite saturation occurred in a few samples in evaporation amounts ranging from 98 percent to 99 percent with the partial pressure of CO₂ equal to 10^−2.0 atm. Carnotite saturation did not occur in any groundwater with the system closed to CO₂.  相似文献   

The influence of degradation of the swamp and alpine meadows on CH<Subscript>4</Subscript> and CO<Subscript>2</Subscript> fluxes on the Qinghai-Tibetan Plateau     

Junfeng Wang  Genxu Wang  Hongchang Hu  Qingbai Wu 《Environmental Earth Sciences》2010,60(3):537-548

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   

Preliminary estimate of CO2 output from Pantelleria Island volcano (Sicily,Italy): evidence of active mantle degassing     

《Applied Geochemistry》2001,16(7-8):883-894

Total CO₂ output from fumaroles, bubbling and water dissolved gases and soil gases was investigated at Pantelleria Island volcano, Italy. The preliminary results indicate an overall output of 0.39 Mt a⁻¹ of CO₂ from the island. The main contribution to the total output was from diffuse soil degassing (about 0.32 Mt a⁻¹), followed by dissolved CO₂ (0.034 Mt a⁻¹), focussed soil degassing (0.028 Mt a⁻¹) and bubbling CO₂ (0.013 Mt a⁻¹). The contribution of CO₂ from fumarole gases was found to be negligible (1.4×10⁻⁶ Mt a⁻¹). Carbon-13 values for CO₂ coupled with those for associated He in gases from fumaroles and sites of focussed soil degassing clearly rule out any significant organic CO₂ component and suggest a common mantle origin for these gas species. The inferred mantle source beneath Pantelleria would seem to have peculiar geochemical characteristics, quite distinct from those of mantle producing MORB but compatible with those of magmatic sources of central Mediterranean and central European volcanoes. These findings indicate that the Pantelleria volcanic complex is a site of active mantle degassing that is worthy of attention for future geochemical surveillance of the island.  相似文献   

Geochemistry of organic-rich river waters in Amazonia: Insights on weathering processes of intertropical cratonic terrain     

《Applied Geochemistry》2016

In this study, eight organic-rich rivers that flow through the Brazilian craton in the southwestern Amazon rainforest are investigated. This investigation is the first of its type in this area and focuses on the effects of lithology, long-term weathering, thick soils, forest cover and hydrological period on the dissolved load compositions in rivers draining cratonic terrain. The major dissolved ion concentrations, alkalinity (TAlk), SiO₂, trace element concentrations, and Sr isotope contents in the water were determined between April 2009 and January 2010. In addition, the isotopic values of oxygen and hydrogen were determined between 2011 and 2013. Overall, the river water is highly dilute and dominated by the major dissolved elements TAlk, SiO₂ and K⁺ and the major dissolved trace elements Al, Fe, Ba, Mn, P, Zn and Sr, which exhibit large temporal and spatial variability and are closely correlated with the silicatic bedrock and hydrology. Additionally, rainwater and recycled water vapor and the size of the basin contribute to the geochemistry of the waters. The total weathering flux estimated from our results is 2–4 t km⁻².yr⁻¹, which is one of the lowest fluxes in the world. The CO₂ consumption rate is approximately 21–61 10³ mol km⁻² yr⁻¹, which is higher than expected given the stability of the felsic to basic igneous and metamorphic to siliciclastic basement rocks and the thick tropical soil cover. Thus, weathering of the cratonic terrain under intertropical humid conditions is still an important consumer of CO₂.  相似文献   

Decarbonation of subducting slabs: Insight from petrological–thermomechanical modeling     

《Gondwana Research》2016

Subduction of heterogeneous lithologies (sediments and altered basalts) carries a mixture of volatile components (H₂O ± CO₂) into the mantle, which are later mobilized during episodes of devolatilization and flux melting. Several petrologic and thermodynamic studies investigated CO₂ decarbonation to better understand carbon cycling at convergent margins. A paradox arose when investigations showed little to no decarbonation along present day subduction geotherms at subarc depths despite field based observations. Sediment diapirism is invoked as one of several methods for carbon transfer from the subducting slab. We employ high-resolution 2D petrological–thermomechanical modeling to elucidate the role subduction dynamics has with respect to slab decarbonation and the sediment diapirism hypothesis. Our thermodynamic database is modified to account for H₂O–CO₂ binary fluids via the following lithologies: GLOSS average sediments (H₂O: 7.29 wt.% & CO₂: 3.01 wt.%), carbonated altered basalts (H₂O: 2.63 wt.% & CO₂: 2.90 wt.%), and carbonated peridotites (H₂O: 1.98 wt.% & CO₂: 1.50 wt.%). We include a CO₂ solubility P–x[H₂O wt.%] parameterization for sediment melts. We parameterize our model by varying two components: slab age (20, 40, 60, 80 Ma) and convergence velocity (1, 2, 3, 4, 5, 6 cm year^− 1). 59 numerical models were run and show excellent agreement with the original code base. Three geodynamic regimes showed significant decarbonation. 1) Sedimentary diapirism acts as an efficient physical mechanism for CO₂ removal from the slab as it advects into the hotter mantle wedge. 2) If subduction rates are slow, frictional coupling between the subducting and overriding plate occurs. Mafic crust is mechanically incorporated into a section of the lower crust and undergoes decarbonation. 3) During extension and slab rollback, interaction between hot asthenosphere and sediments at shallow depths result in a small window (~ 12.5 Ma) of high integrated CO₂ fluxes (205 kg m^− 3 Ma^− 1).  相似文献   

Climate and human impact during the past 2000 years as recorded in the Lagunas de Yala,Jujuy, northwestern Argentina     

《Quaternary International》2006,142(1):30-43

²¹⁰Pb, ¹³⁷Cs and ¹⁴C dated sediments of two late Holocene landslide lakes in the Provincial Park Lagunas de Yala (Laguna Rodeo, Laguna Comedero, 24°06′S, 65°30′W, 2100 m asl, northwestern Argentina) reveal a high-resolution multi-proxy data set of climate change and human impact for the past ca. 2000 years. Comparison of the lake sediment data set for the 20th century (sediment mass accumulation rates MARs, pollen spectra, nutrient and charcoal fluxes) with independent dendroecological data from the catchment (fire scars, tree growth) and long regional precipitation series (from 1934 onwards) show that (1) the lake sediment data set is internally highly consistent and compares well with independent data sets, (2) the chronology of the sediment is reliable, (3) large fires (1940s, 1983/1984–1989) as documented in the local fire scar frequency are recorded in the charcoal flux to the lake sediments and coincide with low wet-season precipitation rates (e.g., 1940s, 1983/1984) and/or high interannual precipitation variability (late 1940s), and (4) the regional increase in precipitation after 1970 is recorded in an increase in the MARs (L. Rodeo from 100 to 390 mg cm⁻² yr⁻¹) and in an increase in fern spores reflecting wet vegetation. The most significant change in MARs and nutrient fluxes (C_org and P) of the past 2000 years is observed with the transition from the Inca Empire to the Spanish Conquest around 1600 AD. Compared with the pre-17th century conditions, MARs increased by a factor of ca. 5 to >8 (to 800 _{+130, −280} mg cm⁻² yr⁻¹), PO₄ fluxes increased by a factor of 7, and C_org fluxes by a factor of 10.5 for the time between 1640 and 1930 AD. 17th to 19th century MARs and nutrient fluxes also exceed 20th century values. Excess Pb deposition as indicated by a significant increase in Pb/Zr and Pb/Rb ratios in the sediments after the 1950s coincides with a rapid expansion of the regional mining industry. Excess Pb is interpreted as atmospheric deposition and direct human impact due to Pb smelting.  相似文献   

CO2 solubility in aqueous solutions containing Na+, Ca2+, Cl−, SO42− and HCO3-: The effects of electrostricted water and ion hydration thermodynamics     

《Applied Geochemistry》2016

Dissolution of CO₂ into deep subsurface brines for carbon sequestration is regarded as one of the few viable means of reducing the amount of CO₂ entering the atmosphere. Ions in solution partially control the amount of CO₂ that dissolves, but the mechanisms of the ion's influence are not clearly understood and thus CO₂ solubility is difficult to predict. In this study, CO₂ solubility was experimentally determined in water, NaCl, CaCl₂, Na₂SO_4, and NaHCO₃ solutions and a mixed brine similar to the Bravo Dome natural CO₂ reservoir; ionic strengths ranged up to 3.4 molal, temperatures to 140 °C, and CO₂ pressures to 35.5 MPa. Increasing ionic strength decreased CO₂ solubility for all solutions when the salt type remained unchanged, but ionic strength was a poor predictor of CO₂ solubility in solutions with different salts. A new equation was developed to use ion hydration number to calculate the concentration of electrostricted water molecules in solution. Dissolved CO₂ was strongly correlated (R² = 0.96) to electrostricted water concentration. Strong correlations were also identified between CO₂ solubility and hydration enthalpy and hydration entropy. These linear correlation equations predicted CO₂ solubility within 1% of the Bravo Dome brine and within 10% of two mixed brines from literature (a 10 wt % NaCl + KCl + CaCl₂ brine and a natural Na⁺, Ca²⁺, Cl⁻ type brine with minor amounts of Mg²⁺, K⁺, Sr²⁺ and Br⁻).  相似文献   

Accumulation of mantle gases in a permanently stratified volcanic lake (Lac Pavin,France)     

《Geochimica et cosmochimica acta》1999,63(19-20):3357-3372

Lac Pavin is a volcanic crater lake in the Massif Central (France), characterized by a permanent vertical density stratification resulting from a strong and persistent chemocline between about 60 and 70 m depth. The deep water below the chemocline forms the monimolimnion, in which most dissolved ions as well as helium, carbon dioxide, and methane are strongly enriched. The ³He/⁴He isotope ratio of the excess helium is (9.09 ± 0.01) · 10⁻⁶, or (6.57 ± 0.01) R_a. These findings clearly indicate a flux of mantle-derived magmatic gases into the monimolimnion.In order to derive the fluxes of magmatic volatiles into Lac Pavin, it is essential to understand the hydrologic characteristics of the lake. Previously published two-box models have assumed groundwater input at the lake bottom, a short residence time in the monimolimnion, and biogenic origin of the CO₂. We propose an alternative model with a flux of magmatic gases, but not of water, into the monimolimnion, and a weak diffusive coupling between the monimolimnion and the overlying mixolimnion which leads to a long deep-water residence time (≈ 70 yr). We reassess the carbon budget of the lake and conclude that the major part of the accumulated CO₂ in the monimolimnion is of magmatic origin. From the model-derived water exchange rates, we calculated a mantle ⁴He flux of (6 ± 2) · 10¹¹ atoms m⁻² s⁻¹. This value lies near the lower end of the range found in comparable volcanic lakes. The flux of magmatic CO₂ is estimated as (1.2 ± 0.4) · 10⁻⁷ mol m⁻² s⁻¹, which is also comparatively low. The monimolimnion appears to be in steady state with respect to these fluxes, therefore no further, potentially hazardous, accumulation of CO₂ takes place.  相似文献   

CO<Subscript>2</Subscript> emissions from a municipal site for final disposal of solid waste in Gualeguaychu,Entre Rios Province,Argentina     

Romina Sanci  Héctor O. Panarello  Héctor A. Ostera 《Environmental Earth Sciences》2012,66(2):519-528

This paper estimates CO₂ fluxes in a municipal site for final disposal of solid waste, located in Gualeguaychu, Argentina. Estimations were made using the accumulation chamber methods, which had been calibrated previously in laboratory. CO₂ fluxes ranged from 31 to 331 g m⁻² day⁻¹. Three different populations were identified: background soil gases averaging 46 g m⁻² day⁻¹, intermediate anomalous values averaging 110 g m⁻² day⁻¹ and high anomalous values averaging 270 g m⁻² day⁻¹. Gas samples to a depth of 20 cm were also taken. Gas fractions, XCO₂ < 0.1, XCH₄ < 0.01, XN₂ ~0.71 and XO₂ ~0.21, δ¹³C of CO₂ (−34 to −18‰), as well as age of waste emplacement, suggest that the study site may be at the final stage of aerobic biodegradation. In a first approach, and following the downstream direction of groundwater flow, alkalinity and δ¹³C of dissolved inorganic carbon (−15 to 4‰) were observed to increase when groundwater passed through the disposal site. This suggests that the CO₂ generated by waste biodegradation dissolves or that dissolved organic matter appears as a result of leachate degradation.  相似文献   

Benthic fluxes and the cycling of biogenic silica and carbon in two southern California borderland basins     

《Geochimica et cosmochimica acta》1987,51(6):1345-1363

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   

The effect of Si and Al concentrations on the removal of U(VI) in the alkaline conditions created by NH3 gas     

《Applied Geochemistry》2016

Remediation of uranium in the deep unsaturated zone is a challenging task, especially in the presence of oxygenated, high-carbonate alkalinity soil and pore water composition typical for arid and semi-arid environments of the western regions of the U.S. This study evaluates the effect of various pore water constituencies on changes of uranium concentrations in alkaline conditions, created in the presence of reactive gases such as NH₃ to effectively mitigate uranium contamination in the vadose zone sediments. This contaminant is a potential source for groundwater pollution through slow infiltration of soluble and highly mobile uranium species towards the water table. The objective of this research was to evaluate uranium sequestration efficiencies in the alkaline synthetic pore water solutions prepared in a broad range of Si, Al, and bicarbonate concentrations typically present in field systems of the western U.S. regions and identify solid uranium-bearing phases that result from ammonia gas treatment. In previous studies (Szecsody et al. 2012; Zhong et al. 2015), although uranium mobility was greatly decreased, solid phases could not be identified at the low uranium concentrations in field-contaminated sediments. The chemical composition of the synthetic pore water used in the experiments varied for silica (5–250 mM), Al³⁺ (2.8 or 5 mM), HCO₃⁻ (0–100 mM) and U(VI) (0.0021–0.0084 mM) in the solution mixture. Experiment results suggested that solutions with Si concentrations higher than 50 mM exhibited greater removal efficiencies of U(VI). Solutions with higher concentrations of bicarbonate also exhibited greater removal efficiencies for Si, Al, and U(VI). Overall, the silica polymerization reaction leading to the formation of Si gel correlated with the removal of U(VI), Si, and Al from the solution. If no Si polymerization was observed, there was no U removal from the supernatant solution. Speciation modeling indicated that the dominant uranium species in the presence of bicarbonate were anionic uranyl carbonate complexes (UO₂(CO₃)₂⁻² and UO₂(CO₃)₃⁻⁴) and in the absence of bicarbonate in the solution, U(VI) major species appeared as uranyl-hydroxide (UO₂(OH)₃⁻ and UO₂(OH)₄⁻²) species. The model also predicted the formation of uranium solid phases. Uranyl carbonates as rutherfordine [UO₂CO₃], cejkaite [Na₄(UO2)(CO₃)₃] and hydrated uranyl silicate phases as Na-boltwoodite [Na(UO₂)(SiO₄)·1.5H₂O] were anticipated for most of the synthetic pore water compositions amended from medium (2.9 mM) to high (100 mM) bicarbonate concentrations.  相似文献