Laminated graphene oxide and hydrotalcite membranes via alternating spray-deposition with stable desalting performance

Laminated graphene oxide (GO) membrane has great potential for desalination, but achieving good stability in salt retention and water permeation is still a challenge. The “compact” sieving structure and the “loose” permeating structure of the GO membranes offer synergetic effects for high-performance desalination. Here, a composite desalination membrane involving two two-dimensional layered nanomaterials with opposite charges has been reported. The multi-layered GO (MLGO) and hydrotalcite (HT) were then alternated in a spray-coating on a PDA-modified substrate to construct multiple structures. Different assembly regions were identified by in-situ morphology monitoring, which showed that MLGO and HT were connected by electrostatic attractions. Also, the composite membrane showed high salt retention, permeability and long-term performance stability. The water flux of the composite membrane increased from 2.8 L m−2 h−1 bar−1 to 3.6–5.2 L m−2 h−1, which was due to the increases in the interlayer spacing distances and the introduction of new permeable spaces. After a 400 h continuous filtration test, the Na2SO4 retention remained stable. The water fluxes were in the range of 2.0–3.0 L m−2 h−1 bar−1, which corresponded to an increase by 42.9 %–114.3 % in comparison with the pure MLGO membrane. As compared with the MLGO membrane, molecular dynamics (MD) simulations revealed that more water molecules passed through the MLGO-HT membrane with a shorter pathway length and higher speed than MLGO membrane. The present study demonstrated the potential of a composite with 2D materials for desalination applications.