4.7 Article

Macroscale insights into heterogeneous hydrate formation and decomposition behaviors in porous media

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 475, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2023.146215

Keywords

Hydrate; Hydrocarbon; Heterogeneity; Phase transition; Porous media

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This study achieved the controllable process of heterogeneous hydrate phase transition at a macroscale and successfully realized different distribution patterns of hydrates. The observations revealed that water and gas transfer in pores governed the kinetic of heterogeneous hydrate phase transition. A new sequence of nucleation-growth-migration driven by water migration for heterogeneous hydrate formation was proposed, and it was found that the phase transition rates between heterogeneous and homogeneous hydrate differed by 2 to 3 times due to mass migration. These findings are important for explaining the enrichment of methane hydrate in marine sediment and developing targeted approaches to natural gas hydrate production, as well as indicating the feasibility of hydrocarbon capture, storage, and transport using hydrate-based technologies.
Hydrocarbon fuels are distributed unevenly in the earth, known as heterogeneity. How to harness the nature of heterogeneity for sustainable development of energy sources is the key issue. Herein, the controllable process of heterogeneous hydrate phase transition is firstly realized at macroscale, and three typical hydrate distribution patterns (dispersed, massive, and layered) with the same hydrate saturation are successfully achieved. Macroscale observations revealed the kinetic of heterogeneous hydrate phase transition governed by water and gas transfer in pores. Specifically, a new sequence of nucleation-growth-migration driven by water migration for heterogeneous hydrate formation in porous media is proposed. In contrast, gas transportation capacity and reformation probability determine the heterogeneous hydrate decomposition efficiency. Significantly, the phase transition rates between heterogeneous and homogeneous hydrate differs by 2 to 3 times due to mass migration. These results suggest that the porous sediments with facilitated water migration under strong capillary effect are preferable for heterogeneous distribution of hydrocarbon fuels, providing explanations for the enrichment of methane hydrate in marine coarse-grained sandy sediment. Nevertheless, the distribution heterogeneity could be challenging to efficient and economic gas production, raising the demand for targeted approaches to develop natural gas hydrate with different distribution patterns. More significantly, the enhanced hydrate formation rate in porous media by controllable heterogeneous hydrate formation method offered by this work also indicates the feasibility in hydrocarbon capture, storage and transport via hydrate-based technologies.

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