Structure–property relationships of reduced graphene oxide membranes intercalated with polycyclic aromatics

Abstract Graphene oxide (GO) membranes intercalated with various organic moieties have shown excellent potential for a range of water processing applications. However, microstructure–functional property relationships in these structurally disordered membranes are not well understood. We demonstrate a practical methodology for developing such relationships for GO membranes intercalated with molecular species, with polycyclic aromatic toluidine blue O (TBO) as an example functional intercalant. We use solid‐state UV–vis absorbance and fluorescence measurements to quantitatively track the arrangements of TBO in a series of TBO‐loaded reduced GO (rGO) membranes. This study reveals the evolution of diverse arrangements including TBO monomers, lateral and stacked dimers, and other aggregates, as a function of overall TBO loading. These microstructures are then correlated to changes in overall properties such as interlayer d ‐spacings, permeate fluxes, and solute rejections. The characterization of these different intercalant microstructures explains non‐intuitive flux and rejection trends, which can circumvent flux and solute rejection trade‐offs.