Hydrate technology with high gas storage capacity and excellent safety features has attracted much attention for capturing CO2 from biogas to produce purified CH4. When considering operational efficiency, it is desirable to overcome technical barriers such as slow hydrate generation and low separation efficiency. Therefore, based on the properties of surfactant-enhanced hydrate generation kinetics, this work first systematically evaluated the performance of 500 ppm SDS on the separation efficiency of 40 mol% CO2 and 60 mol% CH4 simulated biogas. The experimental results show a significant increase in gas capture at higher driving forces, with the rise being dominated by the CH4 component, indicating that larger driving forces reduce hydrate selectivity to CO2-CH4 and weaken gas separation efficiency, with a maximum CO2 recovery of 84.24 ± 1.19% at 275.15 K and 8 MPa. Interestingly, hydrate growth mainly occurred in the liquid phase, leading to the separation factor being positively correlated with the induction time with sufficient CO2 dissolution. In comparison, the gas capture per unit volume of solution could be improved by more than a factor of 2 at higher gas–liquid ratios. The best separation factor of 7.84 ± 0.73 was achieved, and separation factors in general gradually decreased with increasing gas–liquid ratio; however, there was high-pressure failure behavior. Furthermore, the impact of the defoamer on separation efficiency was deeply investigated for SDS decomposition foaming, with results showing that the defoamer would alleviate hydrate decomposition foaming behaviour while having no significant effect on hydrate generation kinetics and separation efficiency.
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