Liquid CO₂ jet breakup and rapid hydrate formation in the deep-water positive-buoyancy zone: Implications for marine CO₂ sequestration

Abstract

Marine CO₂ hydrate sequestration has emerged as a promising strategy for large-scale and long-term carbon storage. Rapid conversion of liquid CO₂ into negatively buoyant hydrates is a key challenge, especially in the positive-buoyancy zone. Jet injection of liquid CO₂ offers a feasible route to accelerate hydrate formation and aligns with the technical pathway toward large-scale CO₂ storage. In this study, the jet characteristics and hydrate formation behavior of liquid CO₂ in high-pressure water were investigated under non-hydrate-forming conditions (6.5 MPa, 10 °C) and hydrate-forming conditions (6.5 MPa, 3 °C), respectively. Panoramic and close-up imaging captured the initial breakup morphology and temporal evolution across five jet instability regimes, confirming their correspondence with the We. Droplet size distributions across these regimes were also characterized, showing an overall decrease with increasing Weber number (We), while the transitional range (We ≈ 22‒669) exhibited significant droplet enlargement and reduced uniformity, with the coefficient of variation (CV) exceeding 75%. Additionally, hydrate nucleation within the jet system remained strongly probabilistic. Atomized jets could induce nucleation on timescales of seconds or even milliseconds, yet high jet velocity alone did not guarantee nucleation. Four typical types of hydrate formation were observed, including the most favorable form, i.e., instantaneously formed self-settling hydrate clusters. Furthermore, high-speed close-up imaging revealed multi-site, millisecond-scale nucleation mechanisms and a three-stage clustering process. These findings demonstrate that liquid CO₂ jet injection can rapidly form self-settling hydrates in the positive- buoyancy zone, providing a promising pathway for hydrate-based oceanic CO₂ sequestration and contributing to global carbon neutrality.

Graphical abstract

Keywords

CO₂ hydrate / Liquid CO₂ jet / Marine carbon sequestration / Positive buoyancy zone / Carbon neutrality

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