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Coupled thermo‐hydro‐mechanical‐chemical modelling has attracted attention in past decades due to many contemporary geotechnical engineering applications (e.g., waste disposal, carbon capture and storage). However, molecular‐scale interactions within geomaterials (e.g., swelling and dissolution/precipitation) have a significant influence on the mechanical behaviour, yet are rarely incorporated into existing Thermal‐Hydro‐Mechanical‐Chemical (THMC) frameworks. This paper presents a new coupled hydro‐mechanical‐chemical constitutive model to bridge molecular‐scale interactions with macro‐physical deformation by combining the swelling and dissolution/precipitation through an extension of the new mixture‐coupling theory. Entropy analysis of the geomaterial system provides dissipation energy, and Helmholtz free energy gives the relationship between solids and fluids. Numerical simulation is used to compare with the selected recognized models, which demonstrates that the swelling and dissolution/precipitation processes may have a significant influence on the mechanical deformation of the geomaterials.

This paper presents the development of a discrete fracture model of fully coupled compressible fluid flow, adsorption and geomechanics to investigate the dynamic behaviour of fractures in coal. The model is applied in the study of geological carbon dioxide sequestration and differs from the dual porosity model developed in our previous work, with fractures now represented explicitly using lower‐dimensional interface elements. The model consists of the fracture‐matrix fluid transport model, the matrix deformation model and the stress‐strain model for fracture deformation. A sequential implicit numerical method based on Galerkin finite element is employed to numerically solve the coupled governing equations, and verification is completed using published solutions as benchmarks. To explore the dynamic behaviour of fractures for understanding the process of carbon sequestration in coal, the model is used to investigate the effects of gas injection pressure and composition, adsorption and matrix permeability on the dynamic behaviour of fractures. The numerical results indicate that injecting nonadsorbing gas causes a monotonic increase in fracture aperture; however, the evolution of fracture aperture due to gas adsorption is complex due to the swelling‐induced transition from local swelling to macro swelling. The change of fracture aperture is mainly controlled by the normal stress acting on the fracture surface. The fracture aperture initially increases for smaller matrix permeability and then declines after reaching a maximum value. When the local swelling becomes global, fracture aperture starts to rebound. However, when the matrix permeability is larger, the fracture aperture decreases before recovering to a higher value and remaining constant. Gas mixtures containing more carbon dioxide lead to larger closure of fracture aperture compared with those containing more nitrogen.