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The effect of oxygen fugacity on the solubility of carbon-oxygen fluids in basaltic melt
Authors:Alison R Pawley  John R Holloway and Paul F McMillan
Institution:

aDepartment of Chemistry, Arizona State University, Tempe, AZ 85287,USA

bDepartment of Geology, Arizona State University, Tempe, AZ 85287,USA

Abstract:The solubility of CO2single bondCO fluids in a mid-ocean ridge basalt (morb) has been measured at 1200°C, 500–1500 bar, and oxygen fugacities between NNO and NNO-4. High oxygen fugacities, and thus CO2-rich fluids, were produced by using a starting material equilibrated at NNO, and Ag2C2O4 as the fluid source. Low oxygen fugacities were achieved by using graphite capsules, and MgCO3 as the fluid source. These graphite-saturated fluids have the lowest possibleC/O2CO ratio for a given pressure and temperature.

Experiments were run in a rapid-quench internally heated pressure vessel. Fluid compositions were measured using a simple vacuum technique and by Raman spectroscopy of fluid inclusions. The two techniques yielded comparable results. Fourier transform micro-infrared spectroscopy was used to identify and measure concentrations of dissolved volatiles in double-polished wafers of the quenched glasses. Carbonate was the only carbon-bearing species identified. Raman spectroscopic analysis of inclusion-free areas of glass confirmed the absence of dissolved molecular CO2, CO and carbon. The measured concentrations of dissolved CO2 in the glasses were proportional to the fugacity of CO2 during the experiments, calculated from the measured fluid compositions. The data were fit to the equationXCO2melt(ppm)= 0.492 fCO2 (bar).

The insolubility of CO, compared to CO2, may be related to the fact that dissolution of CO requires reduction of another species in the melt, whereas dissolution of CO2 does not. Due to the fact that CO will be an important component of natural Csingle bondO fluids at low pressures and low oxygen fugacities, equilibrium dissolved CO2 contents will be less than calculated assuming pure CO2 fluids, but as theC/O2CO ratio in a pure Csingle bondO fluid at fixed pressure and temperature is a direct function of oxygen fugacity, measurement of the oxygen fugacity of quenched glasses or trapped fluids in natural samples should allow saturation concentrations to be calculated. Dissolved CO2 contents of somemorb are less than expected if they were in equilibrium with pure CO2. These samples must, therefore, have been more reduced than average if they were fluid-saturated. Together with results from other studies of CO2 and H2O solubilities in basalt, the results of this study provide a comprehensive framework for modelling CO2 solution inmorb.

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