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  • Copernicus  (4)
  • Mineralogical Society of Great Britain and Ireland  (1)
  • 2010-2014  (5)
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  • 1
    Publication Date: 2014-11-01
    Description: Natural hydromagnesite (Mg5(CO3)4(OH)2·4H2O) dissolution and precipitation experiments were performed in closed-system reactors as a function of temperature from 22.5 to 75ºC and at 8.6 〈 pH 〈 10.7. The equilibrium constants for the reaction Mg5(CO3)4(OH)2·4H2O + 6H+ = 5Mg2+ + 4HCO3– + 6H2O were determined by bracketing the final fluid compositions obtained from the dissolution and precipitation experiments. The resulting constants were found to be 1033.7±0.9, 1030.5±0.5 and 1026.5±0.5 at 22.5, 50 and 75ºC, respectively. Whereas dissolution rates were too fast to be determined from the experiments, precipitation rates were slower and quantified. The resulting BET surface areanormalized hydromagnesite precipitation rates increase by a factor of ~2 with pH decreasing from 10.7 to 8.6. Measured rates are approximately two orders of magnitude faster than corresponding forsterite dissolution rates, suggesting that the overall rates of the low-temperature carbonation of olivine are controlled by the relatively sluggish dissolution of the magnesium silicate mineral.
    Print ISSN: 0026-461X
    Electronic ISSN: 1471-8022
    Topics: Geosciences
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  • 2
    Publication Date: 2012-08-14
    Description: Quantifying how C fluxes will change in the future is a complex task for models because of the coupling between climate, hydrology, and biogeochemical reactions. Here we investigate how pedogenesis of the Peoria loess, which has been weathering for the last 13 kyr, will respond over the next 100 yr of climate change. Using a cascade of numerical models for climate (ARPEGE), vegetation (CARAIB) and weathering (WITCH) we explore the effect of an increase in CO2 of 315 ppmv (1950) to 700 ppmv (2100 projection). The increasing CO2 results in an increase in temperature along the entire transect. In contrast, drainage increases slightly for a focus pedon in the South but decreases strongly in the North. These two variables largely determine the behavior of weathering. In addition, although CO2 production rate increases in the soils in response to global warming, the rate of diffusion back to the atmosphere also increases, maintaining a roughly constant or even decreasing CO2 concentration in the soil gas phase. Our simulations predict that temperature increasing in the next 100 yr causes the weathering rates of the silicates to increase into the future. In contrast, the weathering rate of dolomite – which consumes most of the CO2-decreases due to its retrograde solubility in both end members (South and North) of the transect. We thus infer slower rates of advance of the dolomite reaction front into the subsurface, and faster rates of advance of the silicate reaction front. However, additional simulations for 9 pedons located along the North–South transect show that dolomite weathering will increase in the central part of the Mississippi Valley, owing to a maximum in the response of vertical drainage to the ongoing climate change. The carbonate reaction front can be likened to a terrestrial lysocline because it represents a depth interval over which carbonate dissolution rates increase drastically. However, in contrast to the lower pH and shallower lysocline expected in the oceans with increasing atmospheric CO2, we predict an acceleration of the lysocline deepening in soils in the central area of the Mississippi Valley, but a slowdown of its deepening in the Southern and Northern section. This result illustrates the complex behavior of carbonate weathering facing short term global climate change. Predicting the global response of terrestrial weathering to increased atmospheric CO2 and temperature in the future will mostly depend upon our ability to make precise assessments of which areas of the globe increase or decrease in precipitation and soil drainage.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 3
    Publication Date: 2013-01-28
    Description: CO2 exchange between terrestrial ecosystems and the atmosphere is key to understanding the feedbacks between climate change and the land surface. In regions with carbonaceous parent material, CO2 exchange patterns occur that cannot be explained by biological processes, such as disproportionate outgassing during daytime or nighttime CO2 uptake during periods when all vegetation is senescent. Neither of these phenomena can be attributed to carbonate weathering reactions, since their CO2 exchange rates are too small. Soil ventilation induced by high atmospheric turbulence is found to explain atypical CO2 exchange between carbonaceous systems and the atmosphere. However, by strongly altering subsurface CO2 concentrations, ventilation can be expected to influence carbonate weathering rates. By imposing ventilation-driven CO2 outgassing in a carbonate weathering model, we show here that carbonate geochemistry is accelerated and does play a surprisingly large role in the observed CO2 exchange patterns. We found that by rapidly depleting soil CO2 during daytime, ventilation disturbs soil carbonate equilibria and therefore strongly magnifies daytime carbonate precipitation and associated CO2 production. At night, ventilation ceases and the depleted CO2 concentrations increase steadily. Dissolution of carbonate is now enhanced, which consumes CO2 and largely compensates for the enhanced daytime carbonate precipitation. This is why only a relatively small effect on global carbonate weathering rates is to be expected. On the short term, however, ventilation has a drastic effect on synoptic carbonate weathering rates, resulting in a pronounced diel pattern that exacerbates the non-biological behavior of soil-atmosphere CO2 exchanges in dry regions with carbonate soils.
    Print ISSN: 1810-6277
    Electronic ISSN: 1810-6285
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 4
    Publication Date: 2013-01-09
    Description: Quantifying how C fluxes will change in the future is a complex task for models because of the coupling between climate, hydrology, and biogeochemical reactions. Here we investigate how pedogenesis of the Peoria loess, which has been weathering for the last 13 kyr, will respond over the next 100 yr of climate change. Using a cascade of numerical models for climate (ARPEGE), vegetation (CARAIB) and weathering (WITCH), we explore the effect of an increase in CO2 of 315 ppmv (1950) to 700 ppmv (2100 projection). The increasing CO2 results in an increase in temperature along the entire transect. In contrast, drainage increases slightly for a focus pedon in the south but decreases strongly in the north. These two variables largely determine the behavior of weathering. In addition, although CO2 production rate increases in the soils in response to global warming, the rate of diffusion back to the atmosphere also increases, maintaining a roughly constant or even decreasing CO2 concentration in the soil gas phase. Our simulations predict that temperature increasing in the next 100 yr causes the weathering rates of the silicates to increase into the future. In contrast, the weathering rate of dolomite – which consumes most of the CO2 – decreases in both end members (south and north) of the transect due to its retrograde solubility. We thus infer slower rates of advance of the dolomite reaction front into the subsurface, and faster rates of advance of the silicate reaction front. However, additional simulations for 9 pedons located along the north–south transect show that the dolomite weathering advance rate will increase in the central part of the Mississippi Valley, owing to a maximum in the response of vertical drainage to the ongoing climate change. The carbonate reaction front can be likened to a terrestrial lysocline because it represents a depth interval over which carbonate dissolution rates increase drastically. However, in contrast to the lower pH and shallower lysocline expected in the oceans with increasing atmospheric CO2, we predict a deeper lysocline in future soils. Furthermore, in the central Mississippi Valley, soil lysocline deepening accelerates but in the south and north the deepening rate slows. This result illustrates the complex behavior of carbonate weathering facing short term global climate change. Predicting the global response of terrestrial weathering to increased atmospheric CO2 and temperature in the future will mostly depend upon our ability to make precise assessments of which areas of the globe increase or decrease in precipitation and soil drainage.
    Print ISSN: 1726-4170
    Electronic ISSN: 1726-4189
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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  • 5
    Publication Date: 2013-07-24
    Description: CO2 exchange between terrestrial ecosystems and the atmosphere is key to understanding the feedbacks between climate change and the land surface. In regions with carbonaceous parent material, CO2 exchange patterns occur that cannot be explained by biological processes, such as disproportionate outgassing during the daytime or nighttime CO2 uptake during periods when all vegetation is senescent. Neither of these phenomena can be attributed to carbonate weathering reactions, since their CO2 exchange rates are too small. Soil ventilation induced by high atmospheric turbulence is found to explain atypical CO2 exchange between carbonaceous systems and the atmosphere. However, by strongly altering subsurface CO2 concentrations, ventilation can be expected to influence carbonate weathering rates. By imposing ventilation-driven CO2 outgassing in a carbonate weathering model, we show here that carbonate geochemistry is accelerated and does play a surprisingly large role in the observed CO2 exchange pattern of a semi-arid ecosystem. We found that by rapidly depleting soil CO2 during the daytime, ventilation disturbs soil carbonate equilibria and therefore strongly magnifies daytime carbonate precipitation and associated CO2 production. At night, ventilation ceases and the depleted CO2 concentrations increase steadily. Dissolution of carbonate is now enhanced, which consumes CO2 and largely compensates for the enhanced daytime carbonate precipitation. This is why only a relatively small effect on global carbonate weathering rates is to be expected. On the short term, however, ventilation has a drastic effect on synoptic carbonate weathering rates, resulting in a pronounced diel pattern that exacerbates the non-biological behavior of soil–atmosphere CO2 exchanges in dry regions mbox{with carbonate soils}.
    Print ISSN: 1726-4170
    Electronic ISSN: 1726-4189
    Topics: Biology , Geosciences
    Published by Copernicus on behalf of European Geosciences Union.
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