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Gas hydrate-based CO₂ capture processes have attracted considerable attention due to their potentials for energy-efficient pre-combustion CO₂ capture. Recent investigations have explored the use of tailored-wettability porous silica gels, highlighting benefits in thermodynamic and kinetic efficiencies, specifically characterized by low energy requirements and rapid formation. However, achieving high purity levels for both H₂ and CO₂ is crucial for practical implementation. Consequently, identifying and optimizing an effective separation route becomes imperative. In this study, we examined the thermodynamic stability, gas uptake, and separation factors of THF (5.56 mol%) + H₂ + CO₂ hydrates with varying compositions (H₂:CO₂ = 80:20, 60:40, 30:70, or 20:80 mol%) in C0 and C1 silica gel (functionalized by monofunctional alkylsilanes (X-(CH₃)₂-Si-C_n)) systems with SDS (0 or 500 ppm). Pressure-composition …