Water and Solute Transport Governed by Tunable Pore Size Distributions in Nanoporous Graphene Membranes

Nanoporous graphene has the potential to advance membrane separations by offering high selectivity with minimal resistance to flow, but how mass transport depends on the structure of pores in this atomically thin membrane is poorly understood. Here, we investigate the relationship between tunable pore creation using ion bombardment and oxygen plasma etching, the resulting pore size distributions, and the consequent water and solute transport. Through tuning of the pore creation process, we demonstrate nanofiltration membranes that reject small molecules but offer high permeance to water or monovalent ions. Theoretical multiscale modeling of transport across the membranes reveals a disproportionate contribution of large pores to osmotic water flux and diffusive solute transport and captures the observed trends in transport measurements except for the smallest pores. This work provides insights into the effects of graphene pore size distribution and support layer on transport and presents a framework for designing atomically thin membranes.