Realizing small-flake graphene oxide membranes for ultrafast size-dependent organic solvent nanofiltration

Membranes for organic solvent nanofiltration (OSN) or solvent-resistant nanofiltration (SRNF) offer unprecedented opportunities for highly efficient and cost-competitive solvent recovery in the pharmaceutical industry. Here, we describe small-flake graphene oxide (SFGO) membranes for high-performance OSN applications. Our strategy exploits lateral dimension control to engineer shorter and less tortuous transport pathways for solvent molecules. By using La³⁺ as a cross-linker and spacer for intercalation, the SFGO membrane selective layer was stabilized, and size-dependent ultrafast selective molecular transport was achieved. The methanol permeance was up to 2.9-fold higher than its large-flake GO (LFGO) counterpart, with high selectivity toward three organic dyes. More importantly, the SFGO-La³⁺ membrane demonstrated robust stability for at least 24 hours under hydrodynamic stresses that are representative of realistic OSN operating conditions. These desirable attributes stem from the La³⁺ cross-linking, which forms uniquely strong coordination bonds with oxygen-containing functional groups of SFGO. Other cations were found to be ineffective.