Hydrogen adsorption and diffusion behavior in kaolinite slit for underground hydrogen storage: A hybrid GCMC-MD simulation study

Abstract

Underground hydrogen storage (UHS) in reservoirs offers the opportunity for large-scale and long-term storage of hydrogen. In order to understand the fundamental mechanisms of hydrogen storage and transportation, it is crucial to study the adsorption and diffusion behavior of hydrogen in reservoirs. By utilizing a hybrid GCMC and MD simulation procedure, we investigated the adsorption and diffusion behavior of hydrogen in kaolinite slit with pore sizes ranging from 1 to 20 nm at pressures up to 30 MPa and temperatures ranging from 303 to 423 K. Hydrogen distribution, excess adsorption, diffusion coefficient, and gas–solid interaction energy were analyzed in relation to pore size, temperature, pressure, and mineralogy. When pores are larger than 5 nm, most of the hydrogen is located in the bulk phase, resulting in insignificant hydrogen loss due to adsorption. Therefore, reservoirs with pores larger than 5 nm are suitable for UHS. Reservoirs with low temperatures and high hydrogen pressures are conducive to UHS, but the hydrogen mobility is reduced. The mineralogy of the formation results in pore surfaces with different charge properties, which significantly affects hydrogen storage. Although van der Waals interaction dominates the gas–solid interaction, Coulomb interaction remains important. The negatively charged pore surface mitigates the gas–solid Coulomb interaction, thereby preventing hydrogen loss through adsorption. This study enhances our understanding of hydrogen storage mechanisms in subsurface porous media and elucidates the influence of various factors. Consequently, it provides a theoretical framework for selecting UHS sites.