Solvent dehydration with structurally engineered nanoporous graphene oxide membranes.

Pervaporation provides a selective route to high purity solvents that are indispensable for high precision industry. Here, we introduce structurally engineered nanoporous graphene oxide membranes (N-GOm), obtained by heterogeneous co-assembly of nanoporous graphene oxide (NPGO) and GO nanosheets. The NPGO nanosheet characterized by nanoporous sp3 carbon domains and oxygen functionalized groups, synergistically increases water affinity, effectively elevating the water adsorption energies (Eads). The N-GOm integrates defective sp3/sp2 heterogeneous stacked cavity to facilitate water transport, effectively improve the solution self-diffusion coefficient (D), thereby improve diffusion activation energy (ED) indirectly, while graphitic sp2-stacked regions ensure stable structure and enable precise molecular sieving. Here, the thermal crosslinking rN-GOm achieves a remarkable flux of 18.4 kg·m-2·h-1, highlighting the potential for industrial solvent dehydration. These complementary structural properties enable rapid and highly selective transport via densely packed sieving channels and interconnected internal pathways, providing atomistic insight into how carbon microenvironment and stacking structure regulate adsorption and diffusion in ultrathin two-dimensional membranes.