Abstract
Understanding carbon speciation in Earth materials is important to unravel the geochemical evolution of the Earth’s atmosphere, the composition of mantle partial melts, and the overall distribution of carbon in the deep mantle. In an effort to provide the systematic protocols to characterize carbon-bearing fluid inclusions and other carbon-bearing species using high-resolution 13C solid-state NMR, one of the element-specific probes of local structure around carbon, we explore the atomic configurations around the carbon species formed during the reaction between 13C-enriched amorphous carbon and MgSiO3 enstatite synthesized at 1.5 GPa and 1400 °C using 13C MAS NMR spectroscopy and Raman spectroscopy. The Raman spectra for the fluid inclusion show the presence of multiple molecular species (e.g., CO2, CO, CH4, H2O, and H2) and reveal heterogeneous distribution of these species within the inclusion. 13C MAS NMR results show that the sharp peak at 125.2 ppm is dominant. While the peak could be assigned to either molecular CO2 in the fluid phase or fourfold-coordinated carbon ([4]C), the peak is likely due to fluid CO2, as revealed by Raman analyses of micrometer-sized fluid inclusions in the sample. The peaks at 161.2, 170.9, and 173.3 ppm in the 13C NMR spectrum correspond to the carbonate ions (
Acknowledgments
This research was supported by National Research Foundation, Korea Laboratory Program to S.K.L. (2014-053-046). We thank I. Lee (SNU), C.S. Yoo (WSU), and G.D. Cody (CIW) for helpful discussions, and B. Phillips (SUNY, Stony Brook) for constructive suggestions, which greatly improved quality and clarify of the manuscript, and three anonymous reviewers and Y. Morizet for helpful comments and suggestions on the original manuscript.
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