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A first principles method to determine speciation of carbonates in supercritical water

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  • Ding Pan

    (Hong Kong University of Science and Technology
    HKUST Fok Ying Tung Research Institute)

  • Giulia Galli

    (Pritzker School of Molecular Engineering, The University of Chicago
    The University of Chicago
    Argonne National Laboratory)

Abstract

The determination of the speciation of ions and molecules in supercritical aqueous fluids under pressure is critical to understanding their mass transport in the Earth’s interior. Unfortunately, there is no experimental technique yet available to directly characterize species dissolved in water at extreme conditions. Here we present a strategy, based on first-principles simulations, to determine ratios of Raman scattering cross-sections of aqueous species under extreme conditions, thus providing a key quantity that can be used, in conjunction with Raman measurements, to predict chemical speciation in aqueous fluids. Due to the importance of the Earth’s carbon cycle, we focus on carbonate and bicarbonate ions. Our calculations up to 11 GPa and 1000 K indicate a higher concentration of bicarbonates in water than previously considered at conditions relevant to the Earth’s upper mantle, with important implications for the transport of carbon in aqueous fluids in the Earth’s interior.

Suggested Citation

  • Ding Pan & Giulia Galli, 2020. "A first principles method to determine speciation of carbonates in supercritical water," Nature Communications, Nature, vol. 11(1), pages 1-6, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-019-14248-1
    DOI: 10.1038/s41467-019-14248-1
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