Home Physical Sciences Carbon speciation in silicate-C-O-H melt and fluid as a function of redox conditions: An experimental study, in situ to 1.7 GPa and 900 °C
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Carbon speciation in silicate-C-O-H melt and fluid as a function of redox conditions: An experimental study, in situ to 1.7 GPa and 900 °C

  • Bjorn Mysen EMAIL logo
Published/Copyright: April 3, 2015
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Abstract

Carbon speciation in and partitioning among silicate-saturated C-O-H fluids and (C-O-H)-saturated melts have been determined ∼1.7 GPa and 900 °C under reducing and oxidizing conditions. The measurements were conducted in situ while the samples were at the conditions of interest. The solution equilibria were (1) 2CH4 + Qn = 2CH3 + H2O + Qn+1 and (2) 2CO32- + H2O + 2Qn+1 = HCO3 + 2Qn, under reducing and oxidizing conditions, and where the superscript, n, in the Qn-species denotes number of bridging oxygen in the silicate species (Q-species). The abundance ratios, CH3/CH4 and HCO3/CO32-, increase with temperature. The enthalpy change associated with the species transformation differs for fluids and melts and also for oxidized and reduced carbon [Reducing: ΔH(1)fluid = 16 ± 5 kJ/mol, ΔH(1) melt = 50 ± 5 kJ/mol; oxidizing ΔH(2) fluid = 81 ± 14 kJ/mol]. For the exchange equilibrium of CH4 and CH3 species between fluid and melt, the temperature-dependent equilibrium constant, (XCH₄/XCH₃)fluid/(XCH₄/ XCH₃)melt, yields ΔH = 34 ± 3 kJ/mol. \

Increased abundance ratios, CH₄/CH₃ and HCO3 /CO32-, lead to increased polymerization of silicate+(C-O-H) melt. Because of such relations, melt transport properties (e.g., viscosity) and element partition coefficients between magmatic liquids, C-O-H fluids, and crystalline phases can vary by more than 100% with speciation changes of C-bearing volatiles upper mantle. These structure effects are more pronounced the higher the pressure and the more mafic the magma.

Received: 2014-3-14
Accepted: 2014-9-30
Published Online: 2015-4-3
Published in Print: 2015-4-1

© 2015 by Walter de Gruyter Berlin/Boston

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