Surface Wettability Governs CO 2 Hydrate Formation Dynamics: Insights from In Situ NMR Studies

作者：Yanhui Dong, Qian Zhang, Shimin Liu, Liheng Wang, Guang‐Jun Guo, Shouding Li, Derek Elsworth · 发表于：Energy & Fuels · 年份：2025 · DOI：10.1021/acs.energyfuels.5c04104 · 被引用次数：2 · 研究领域：Methane Hydrates and Related Phenomena、Hydrocarbon exploration and reservoir analysis、CO2 Sequestration and Geologic Interactions

Surface wettability in geological sediments critically influences gas hydrate formation, yet the combined effects of wettability on gas migration and hydrate growth remain poorly understood. This study examines how surface wettability governs the dynamics of CO 2 hydrate formation constrained through in situ nuclear magnetic resonance (NMR) spectroscopy and imaging across a spectrum of hydrophilic to hydrophobic conditions. Our experiments reveal that distinct hydrate formation patterns vary systematically with pore surface wettability. In hydrophobic pores, a hydrate shell forms rapidly at gas–water interfaces and restricts the diffusion of CO 2, ultimately limiting the final hydrate saturation. Conversely, hydrophilic pores exhibit extended induction times, enabling sustained CO 2 dissolution and, consequently, higher hydrate saturation. Time-resolved T 2 relaxation profiles reveal greater heterogeneity in gas–water–hydrate distribution within hydrophobic samples, where hydrates preferentially develop in a pore-filling morphology, while in hydrophilic samples, they predominantly exhibit a grain-coating morphology. These wettability-dependent formation patterns substantially influence sediment permeability, with hydrophobic pores showing a more pronounced reduction compared with hydrophilic conditions. We propose a conceptual model that explains these observations through the dynamic interplay among surface wettability, gas–water interface distribution, and subsequent hydrat...