Injecting CO2/N2 into marine sediments to form gas hydrates for CO2 storage is an emerging Carbon Capture and Storage (CCS) technology, holds the potential to significantly reduce the costs of CCS while simultaneously enhancing environmental persistence. However, there is currently a lack of comprehensive investigation into the critical parameters and stability evaluations of CO2/N2 mixed hydrates (Mix-H) formation. This study delves into the impact of gas-liquid ratios, pressure–temperature gradients, and hydrate formation degree on the phase equilibrium, formation kinetics, and thermodynamic stability of Mix-H. Experimental findings elucidate the excess water significantly enhances CO2 dissolution, increasing the thermodynamic barrier for Mix-H formation. Consequently, this leads to weakened kinetics and reduced total CO2 composition within the Mix-H (54.2%–96.4%). Raman spectroscopy confirmed varying heterogeneous compositions and thermodynamic stability of hydrate crystals within the bulk Mix-H. The heterogeneity is quantitatively assessed using a novel test – stepwise depressurization, which revealed increased heterogeneity with decreasing initial pressure–temperature as well as increasing gas-liquid ratios and hydrate formation degree. The heterogeneity of Mix-H significantly impacts the CO2 capture efficiency and long–term stability of CO2 sequestration under environmental disturbances. The results also pave the way for evaluating the performance of mixed hydrate applications in hydrate–based chemical engineering and CCS technology.
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