Abstract
Abstract. High-pressure COH fluids have a fundamental role in a variety of geological processes. Their composition in terms of volatile species can control the solidus temperature and carbonation/decarbonation reactions, as well as influence the amount of solutes generated during fluid–rock interaction at depth. Over the last decades, several systems have been experimentally investigated to unravel the effect of COH fluids at upper-mantle conditions. However, fluid composition is rarely tackled as a quantitative issue, and rather infrequently fluids are analyzed in the same way as the associated solid phases in the experimental assemblage. A comprehensive characterization of carbon-bearing aqueous fluids in terms of composition is hampered by experimental difficulties in synthetizing and analyzing high-pressure fluids without altering their composition upon quenching. Recently, improved techniques have been proposed for the analyses of experimental carbon-saturated COH fluids, leading to a significant advancement in synthetic fluid characterization. Here, we present a review of carbon-bearing aqueous fluid experiments conducted at lower-crust and upper-mantle P–T (pressure and temperature) conditions, in which fluids have been characterized quantitatively through ex situ techniques. We review the experimental background of the most commonly employed thermodynamic models for COH fluids, together with the techniques to synthetize them and analyze their composition when the fluid coexists with solid phases. We highlight how a quantitative approach to COH fluid analyses is a fundamental step to understand the effect of these fluids at upper-mantle conditions and to provide a strong experimental foundation to thermodynamic models to ultimately unravel the deep cycling of elements.
Highlights
Aqueous fluids are involved in many geological processes, from controlling the location and extent of melting to hydrothermal ore genesis, earthquake generation, arc volcanism, and rock-forming processes in general (e.g., Green, 1973; Tatsumi et al, 1986; Taylor and McLennan, 1995; Poli and Schmidt, 2002)
The results summarized in this contribution emphasize how pivotal it is to quantitatively assess the volatile speciation in carbon-saturated COH fluid experiments
Even though conventional thermodynamic modeling represents a valuable tool to predict the volatile speciation at certain P, T, and f O2 conditions, care must be taken to extend the calculation to more complex systems
Summary
Aqueous fluids are involved in many geological processes, from controlling the location and extent of melting to hydrothermal ore genesis, earthquake generation, arc volcanism, and rock-forming processes in general (e.g., Green, 1973; Tatsumi et al, 1986; Taylor and McLennan, 1995; Poli and Schmidt, 2002). Conventional thermodynamic modeling (e.g., PERPLE_X: Connolly and Cesare, 1993; COH: Huizenga, 2001; Gfluid: Zhang and Duan, 2009) allows for the retrieval of the volatile speciation of the COH fluid associated with graphite or diamond as a function of P (pressure), T (temperature), and f O2 These models rely on equations of state (EoS) that only consider pure molecular species (e.g., H2O, CO2, CH4, CO). This approach relies on some concepts which have to be considered when the COH volatile speciation is calculated (French, 1966): i. For a comprehensive characterization of COH fluids, these issues must be considered, especially in more complex chemical systems where the combined effect of these factors could significantly affect the volatile speciation
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