A first-principles molecular dynamics study of molecular hydrogen diffusion in Fe-free olivine

Abstract

Molecular hydrogen (H₂) may be an important form of water in nominally anhydrous minerals in the Earth’s mantle and plays a critical role in mantle water cycle, but the transport properties of H₂ remain unclear. Here, the diffusion of H₂ in Fe-free olivine lattice is investigated at pressures of 1–13 GPa and temperatures of 1300–1900 K by first-principles molecular dynamics. The activation energy and activation volume for H₂ diffusion in Fe-free olivine are determined to be 55 ± 8 kJ/mol and 3.6 ± 0.2 cm³/mol, respectively. H₂ diffusion in Fe-free olivine is faster than H⁺ by 1–4 orders of magnitude and therefore it is more favorable for hydrogen transportation under upper mantle conditions. H₂ can be carried to the mantle transition zone by subducting slabs without releasing to the surrounding mantle. The upper mantle may act as a lid, preventing the releasing of H₂ produced in the deep mantle to the surface.

Keywords

First principles calculations / Molecular dynamics / Molecular hydrogen / Diffusion coefficient / Olivine / Upper mantle

CRediT authorship contribution statement

Haibo Liu: Writing – original draft, Visualization, Validation, Software, Methodology, Investigation, Formal analysis, Data curation, Conceptualization. Baohua Zhang: Writing – review & editing, Validation, Supervision, Funding acquisition. Hongzhan Fei: Writing – review & editing, Validation, Conceptualization. Lei Liu: Software, Methodology.

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. Baohua Zhang is a Guest Editor of the special issue in which this article is published. He was not involved in the handling and decision making of this paper.

Acknowledgements

This study was financially supported by the National Natural Science Foundation of China for Distinguished Young Scholars (42325203). The authors thank Dr. Bowen Chen and Dr. Jingjun Zhou for helpful discussions. The data set for this research is given in the online supporting information and the archiving is underway.

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