Ionic transport through a bilayer nanoporous graphene with cationic and anionic functionalization

Understanding the ionic transport through multilayer nanoporous graphene (NPG) holds great promise for the design of novel nanofluidic devices. Bilayer NPG with different structures, such as nanopore offset and interlayer space, should be the most simple but representative multilayer NPG. In this work, we use molecular dynamics simulations to systematically investigate the ionic transport through a functionalized bilayer NPG, focusing on the effect of pore functionalization, offset, applied pressure and interlayer distance. For a small interlayer space, the fluxes of water and ions exhibit a sudden reduction to zero with the increase in offset that indicates an excellent on-off gate, which can be deciphered by the increasing potential of mean force barriers. With the increase in pressure, the fluxes increase almost linearly for small offsets while always maintain zero for large offsets. Finally, with the increase in interlayer distance, the fluxes increase drastically, resulting in the reduction in ion rejection. Notably, for a specific interlayer distance with monolayer water structure, the ion rejection maintains high levels (almost 100% for coions) with considerable water flux, which could be the best choice for desalination purpose. The dynamics of water and ions also exhibit an obvious bifurcation for cationic and anionic functionalization. Our work comprehensively addresses the ionic transport through a bilayer NPG and provides a route toward the design of novel desalination devices.