Geological sequestration of carbon dioxide (CO2) in solid hydrate state beneath seafloor is an attractive option for mitigating global warming. However, as a representative geological factor in marine sediment, clay mineral still plays an ambiguous role in hydrate depositional behaviors and reservoir structural evolution, which provides an obstacle to accurately assessing the potential and security of marine CO2 sequestration. In this work, spatiotemporal hydrate distribution and sedimentary structure evolution in the presence of two typical clay minerals with different structures and properties were investigated by low-field nuclear magnetic resonance (LNMR) technique. There was an inextricable interaction between clay-fluid migration and hydrate phase transition in porous sediments. Pore plugging owing to migration, agglomeration, and redeposition of unstable kaolinite (KIT) particles weakened final CO2 storage capacity by 10.3% and exacerbated heterogeneous hydrate distribution. CO2 storage capacity in montmorillonite (MMT) system was significantly improved with a water conversion of 82.7% for the high interaction potential between clay particles and favorable mass transfer conditions within the reservoir. However, clay minerals accelerated CO2 hydrate destabilization and disrupted the initial water distribution and pore structure. Migration of MMT fluid with high viscosity and gel property during hydrate phase transition resulted in a complex pore evolution and irreversible sedimentary skeleton deformation, providing an effective warning for field implementation of geological carbon sequestration. The findings expand the understanding of pore-scale interaction between clay minerals and gas hydrates, and provide valuable support for stratigraphic adaptability evaluation of CO2 sequestration in marine sediments.
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