Superhydrophilic and oleophobic membrane functionalized with heterogeneously tailored two-dimensional layered double hydroxide nanosheets for antifouling

Fouling is a common challenge to all membrane-based separation technologies. The current study demonstrated an antifouling membrane with a superhydrophilic but oleophobic (in air) characteristic, which was achieved through covalently tethering heterogeneously tailored two-dimensional layered double hydroxide (LDH) nanosheets to a polyvinylidene fluoride membrane surface. The nanosheets were in situ grafted with alternately arranged sodium 1-dodecanesulfonate (SDS) and 3-aminopropyltriethoxysilane (APTS) chains during preparation. Poly(methacrylic acid) (PMAA) was previously grafted on the membrane via plasma induced graft copolymerization as anchor sites for nanosheet binding. With a simple dip-coating operation, the surface-tailored LDH nanosheets could be bound to the membrane via cross-linking between the amine groups of APTS and carboxyl groups of PMAA. Ultimately, the long hydrophobic SDS and short hydrophilic APTS chains on the nanosheets formed a heterogeneous and infiltration selective (due to steric exclusion) surface on the membrane. As a result, the hydrophilic moieties on the membrane surface were much more accessible to water than to liquids of larger molecular size, thereby bringing about the superhydrophilic but oleophobic characteristic. The functionalization gave rise to both significantly enhanced wettability and hydrophilicity of the membrane, mainly owing to the increase of the electron donor component of surface energy (gamma(AB-)). Additionally, the functionalized membrane obtained a greater permeability without compromising its selectivity. Furthermore, as verified in both filtration tests with synthetic and practical foulant solutions, the superhydrophilic and oleophobic characteristic endowed the functionalized membrane with conspicuously greater cleaning efficiency and excellent capability in resisting irreversible fouling, suggesting promising applications in various fields.