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Regnier, P, Friedlingstein P, Ciais P, Mackenzie FT, Gruber N, Janssens IA, Laruelle GG, Lauerwald R, Luyssaert S, Andersson AJ, Arndt S, Arnosti C, Borges AV, Dale AW, Gallego-Sala A, Godderis Y, Goossens N, Hartmann J, Heinze C, Ilyina T, Joos F, LaRowe DE, Leifeld J, Meysman FJR, Munhoven G, Raymond PA, Spahni R, Suntharalingam P, Thullner M.  2013.  Anthropogenic perturbation of the carbon fluxes from land to ocean. Nature Geoscience. 6:597-607.   10.1038/ngeo1830   AbstractWebsite

A substantial amount of the atmospheric carbon taken up on land through photosynthesis and chemical weathering is transported laterally along the aquatic continuum from upland terrestrial ecosystems to the ocean. So far, global carbon budget estimates have implicitly assumed that the transformation and lateral transport of carbon along this aquatic continuum has remained unchanged since pre-industrial times. A synthesis of published work reveals the magnitude of present-day lateral carbon fluxes from land to ocean, and the extent to which human activities have altered these fluxes. We show that anthropogenic perturbation may have increased the flux of carbon to inland waters by as much as 1.0 Pg C yr(-1) since pre-industrial times, mainly owing to enhanced carbon export from soils. Most of this additional carbon input to upstream rivers is either emitted back to the atmosphere as carbon dioxide (similar to 0.4 Pg C yr(-1)) or sequestered in sediments (similar to 0.5 Pg C yr(-1)) along the continuum of freshwater bodies, estuaries and coastal waters, leaving only a perturbation carbon input of similar to 0.1 Pg C yr(-1) to the open ocean. According to our analysis, terrestrial ecosystems store similar to 0.9 Pg C yr(-1) at present, which is in agreement with results from forest inventories but significantly differs from the figure of 1.5 Pg C yr(-1) previously estimated when ignoring changes in lateral carbon fluxes. We suggest that carbon fluxes along the land-ocean aquatic continuum need to be included in global carbon dioxide budgets.

Lerman, A, Guidry M, Andersson AJ, Mackenzie FT.  2011.  Coastal Ocean Last Glacial Maximum to 2100 CO(2)-Carbonic Acid-Carbonate System: A Modeling Approach. Aquatic Geochemistry. 17:749-773.   10.1007/s10498-011-9146-z   AbstractWebsite

Using coupled terrestrial and coastal zone models, we investigated the impacts of deglaciation and anthropogenic inputs on the CO(2)-H(2)O-CaCO(3) system in global coastal ocean waters from the Last Glacial Maximum (LGM: 18,000 year BP) to the year 2100. With rising sea level and atmospheric CO(2), the carbonate system of coastal ocean water changed significantly. We find that 6 x 10(12) metric tons of carbon were emitted from the coastal ocean, growing due to the sea level rise, from the LGM to late preindustrial time (1700 AD) because of net heterotrophy and calcification processes. This carbon came to reside in the atmosphere and in the growing vegetation on land and in uptake of atmospheric CO(2) through the weathering of rocks on land. It appears that carbonate accumulation, mainly, but not exclusively, in coral reefs from the LGM to late preindustrial time could account for about 24 ppmv of the 100 ppmv rise in atmospheric CO(2), lending some support to the "coral reef hypothesis". In addition, the global coastal ocean is now, or soon will be, a sink of atmospheric CO(2). The temperature rise of 4-5A degrees C since the LGM led to increased weathering rates of inorganic and organic materials on land and enhanced riverine fluxes of total C, N, and P to the coastal ocean of 68%, 108%, and 97%, respectively, from the LGM to late preindustrial time. During the Anthropocene, these trends have been exacerbated owing to rising atmospheric CO(2), due to fossil fuel combustion and land-use practices, other human activities, and rising global temperatures. River fluxes of total reactive C, N, and P are projected to increase from late preindustrial time to the year 2100 by 150%, 380%, and 257%, respectively, modifying significantly the behavior of these element cycles in the coastal ocean, particularly in proximal environments. Despite the fact that the global shoal water carbonate mass has grown extensively since the LGM, the pH(T) (pH values on the total proton scale) of global coastal waters has decreased from similar to 8.35 to similar to 8.18 and the carbonate ion concentration declined by similar to 19% from the LGM to late preindustrial time. The latter represents a rate of decline of about 0.028 mu mol CO(3) (2-) per decade. In comparison, the decrease in coastal water pH(T) from the year 1900 to 2000 was about 8.18-8.08 and is projected to decrease further from about 8.08 to 7.85 between 2000 and 2100, according to the IS92a business-as-usual scenario of CO(2) emissions. Over these 200 years, the carbonate ion concentration will fall by similar to 120 mu mol kg(-1) or 6 mu mol kg(-1) per decade. This decadal rate of decline of the carbonate ion concentration in the Anthropocene is 214 times the average rate of decline for the entire Holocene. Hence, when viewed against the millennial to several millennial timescale of geologic change in the coastal ocean marine carbon system, one can easily appreciate why ocean acidification is the "other CO(2) problem".

Mackenzie, FT, Andersson AJ, Arvidson RS, Guidry MW, Lerman A.  2011.  Land-sea carbon and nutrient fluxes and coastal ocean CO(2) exchange and acidification: Past, present, and future. Applied Geochemistry. 26:S298-S302.   10.1016/j.apgeochem.2011.03.087   AbstractWebsite

Epochs of changing atmospheric CO(2) and seawater CO(2)-carbonic acid system chemistry and acidification have occurred during the Phanerozoic at various time scales. On the longer geologic time scale, as sea level rose and fell and continental free board decreased and increased, respectively, the riverine fluxes of Ca, Mg, DIC, and total alkalinity to the coastal ocean varied and helped regulate the C chemistry of seawater, but nevertheless there were major epochs of ocean acidification (OA). On the shorter glacial-interglacial time scale from the Last Glacial Maximum (LGM) to late preindustrial time, riverine fluxes of DIC, total alkalinity, and N and P nutrients increased and along with rising sea level, atmospheric PCO(2) and temperature led, among other changes, to a slightly deceasing pH of coastal and open ocean waters, and to increasing net ecosystem calcification and decreasing net heterotrophy in coastal ocean waters. From late preindustrial time to the present and projected into the 21st century, human activities, such as fossil fuel and land-use emissions of CO(2) to the atmosphere, increasing application of N and P nutrient subsidies and combustion N to the landscape, and sewage discharges of C, N, P have led, and will continue to lead, to significant modifications of coastal ocean waters. The changes include a rapid decline in pH and carbonate saturation state (modern problem of ocean acidification), a shift toward dissolution of carbonate substrates exceeding production, potentially leading to the "demise" of the coral reefs, reversal of the direction of the sea-to-air flux of CO(2) and enhanced biological production and burial of organic C, a small sink of anthropogenic CO(2), accompanied by a continuous trend toward increasing autotrophy in coastal waters. (C) 2011 Elsevier Ltd. All rights reserved.