Effect of surface roughness on methane adsorption in shale organic nanopores from the perspective of molecular simulations

•CH4 adsorption in rough graphene nano-slits is studied via molecular simulations.•The heterogeneity of the adsorption layer along the rough topology is clarified.•Surface wrinkles enhance the adsorption by increasing adsorption area and capacity.•A mathematical method for evaluating gas reserves in rough nanopores is provided.•The answer to the debate may lies in the distinct roles of basal and edge surfaces. Understanding the shale gas adsorption behavior within organic nanopores is crucial for its development. The pore surfaces commonly exhibit random inherent roughness, which can significantly impact gas adsorption, while it’s still in debate about whether the roughness could enhance the gas adsorption or not. To clarify the underlying mechanisms of the effect of surface roughness, in this study, the Grand Canonical Monte Carlo and Molecular Dynamic simulations are used to investigate the methane adsorption in wrinkled graphene nanochannels with various roughness. The heterogeneity of the adsorption layer along the rough topology is described in detail. The adsorption is enhanced near the concave region and weakened near the convex region. Additionally, increased surface roughness shifts the gas molecules’ aggregation modes in the concave region from a gradual gradient to oscillatory “adsorption points”. We observe that wall roughness due to the wrinkle can enhance the adsorption amount overall, attributed to the increased surface area and the increased unit adsorption capacity due to potential energy overlap. However, the contributions of both factors differ under various pressure and roughness conditions. Then a new mathematical method to estimate the gas adsorption amounts is provided and aligns well with molecular simulation results for a wide range of pressure and roughness conditions. And a potential answer the current debate about the positive or negative impact of adsorption due to roughness is promoted. The key may lie in the dominant role of the co-existed roughness caused by the fragment basal or edge surface. Our work could shed light on the underlying effect of surface roughness on the gas adsorption in shale, and have significant implications for the reserve estimation of shale gas formations.