Gas permeation through double-layer graphene oxide membranes: The role of interlayer distance and pore offset

Abstract Hierarchically stacked graphene oxide (GO) membranes have sparked considerable interest due to their prominent separation performance; however, the underlying separation mechanisms remain elusive. In this study, we conducted molecular dynamics (MD) simulations to explore the role of interlayer distance and pore offset in gas (H2, CH4, N2 and CO2) permeation through double-layer GO membranes. Gas permeance is found to increase with the interlayer distance and pore offset until the interlayer distance exceeds a critical value. With elongating the interlayer distance and pore offset, a sieving effect occurs to overcome preferential adsorption and dominates the transport in mixed H2/CO2, resulting in selective permeation shifting from CO2 to H2. This simulation study provides mechanistic insight into gas permeation through layered GO membranes, and would facilitate the design of new GO membranes for high-performance gas separation.