Microstructural design of crown nanopores in graphene membrane for efficient desalination process

Abstract

Designing a membrane with simultaneous high water permeability and desalination rate to overcome the trade-off presents a persistent and substantial challenge. In this paper, we employed molecular dynamics simulations to design the structure of the graphene crown ether reverse osmosis membrane and elucidate the relationship between the membrane's microscopic separation mechanism and its structure-activity.The results show that the water permeability through crown graphene nanopores exceeded that of the original graphene nanopores by an order of magnitude, and hundreds of times greater than that of the traditional reverse osmosis membrane. Additionally, the water permeation in multilayer crown graphene nanopores also surpassed that in monolayer original graphene nanopores. The water permeability exceeds 46.73 L/cm2/day/Mpa with 100 % salt rejection. Furthermore, the various sizes and shapes of graphene nanopores significantly influence water permeation. Within crown graphene nanopores, a narrow pore enables superior water permeation and salt rejection compared to a circular shape, unlike original graphene nanopores. Observed from MD simulation trajectories,this highly water permeation is caused by the hydrogen bonding between crown ether graphene and water molecules. First-principle calculations further confirm that water transport in graphene crown ether is energetically more favorable than in original graphene nanopores. Our findings support crown graphene membranes as promising candidates for seawater desalination.