Integrated transport-reaction nanomeshes in HGO/CoP membranes for high-flux emulsion separation and catalytic antifouling

Two-dimensional lamellar membranes are promising for emulsion separation, but their practical use is limited by tortuous transport pathways and irreversible organic fouling. Herein, we report pathway-engineered holey graphene oxide/cobalt phosphide (HGO/CoP) nanomesh membranes that integrate in-plane HGO nanopores, CoP nanomesh pores, and HGO/CoP interfacial transport regions into a coupled transport-reaction architecture. The porous CoP nanosheets provide additional transport regions and catalytic reaction nodes within the HGO framework while enabling membrane-mediated peroxymonosulfate (PMS) activation. The optimized HGO/CoP-8 membrane delivered a high emulsion permeance of 283.6 L m −2  h −1 bar −1 with oil rejection above 99.5%, together with underwater superoleophobicity and low oil adhesion. More importantly, PMS-assisted regeneration restored the flux recovery ratio to 98.9%, which remained above 95% over five successive emulsion filtration-regeneration cycles, demonstrating effective catalytic antifouling and membrane regeneration. Electron paramagnetic resonance spectroscopy and scavenging experiments using two 1 O 2 quenchers indicated coexisting radical and non-radical oxidation pathways, with singlet oxygen as a major contributor. This work demonstrates a transport-reaction pathway engineering strategy for designing high-permeance antifouling membranes for oily emulsion treatment.