Oxygen fugacity-mediated carbonate reactions with siliceous fluids in shallow subduction zones

Abstract

Sediments are one of the main carbon sinks in subduction zones, with CaCO₃ and SiO₂ being the main components in sediments. Their chemical stability plays a significant role in the form of carbon in the Earth’s mantle. Here we report the reactions of CaCO₃ with SiO₂ in hydrated sediments at 0.8–2.0 GPa, 400–500 ℃ and redox-buffered conditions relevant to shallow subduction zones. Our results show that the reaction CaCO₃ + SiO₂ = CaSiO₃ + C + O₂(fluid) occurs under CoCoO and IW buffered conditions to generate wollastonite (CaSiO₃) and carbonaceous material (CM). Moreover, wollastonite is formed by the dissolution-crystallization process, which may be significantly affected by oxygen fugacity, leading to distinct crystallization habits (Yui, 1966, Schott et al., 2012). Anhydrous experiments indicate that the reaction proceeds only in the presence of H₂O within the pressure and temperature (P-T) range of this study. The reaction occurs more rapidly with aragonite-structured than calcite-structured CaCO₃. Further, the experiment buffered with natural olivine at 1.0 GPa and 400 ℃ proves that the above reaction can occur during serpentinization processes in shallow subduction zones. More importantly, nanoscale CM may be generated under relatively reducing conditions, exhibiting Raman characteristics of kerogen. These results provide new insights into how deep carbon is distributed in the Earth’s interior.

Keywords

Subduction zone / Sediments / Carbonate stability / Fugacity / Graphite / Wollastonite

CRediT authorship contribution statement

Fengxia Sun: Data curation, Writing – original draft, Investigation, Methodology. Jun Hu: Formal analysis. Weibin Gui: Conceptualization. Ao Deng: Investigation. Penghui Sun: Conceptualization, Software. Fahui Xiong: Writing – review & editing, Methodology. Jin Liu: Conceptualization, Writing – review & editing, Supervision, Resources.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

We thank for Peng Wang and Junfeng Zhang for constructive discussions and technical support. This work is supported by the National Key Research and Development Program of China (Grant No. 2023YFF0804100) and the United Laboratory of High-Pressure Physics and Earthquake Science (Grant No. 2022HPPES01). Some experiments are supported by the Synergic Extreme Condition User Facility (SECUF).

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