“Ion-cage” structure of graphene oxide membranes with stable interlayer spacings towards efficient desalination

Multilayered graphene oxide (GO) membrane with sub-nanometer channels is an ideal candidate for desalination. However, excluding small ions using GO-based membranes in the pressured filtration processes remains a great challenge due to the tortuous transport paths of laminates and their water-swelling characteristic. In our previous work, we developed the cation-controlled theory to precisely regulate the interlayer spacing of GO membranes in aqueous solutions. In this work, we proposed an "ion-cage" strategy to enhance the stability (anti-swelling) of the K-controlled GO (icGO-K) membrane for achieving efficient desalination. The icGO-K membrane, coated with positively charged polyethyleneimine (PEI) on its upper and lower surfaces, immobilized intercalated cation K+ between the laminates by electrostatic repulsion to maintain the stability of the confined interlayer spacing. The icGO-K membrane demonstrated superior rejection of 95.3 %, 83.2 %, 81.8 %, and 70.7 % for MgCl2, MgSO4, NaCl, and Na2SO4 while maintaining competitive permeance of ∼ 3.5 L m-2h−1 bar−1 in the desalination process. More importantly, the icGO-K membrane exhibited ultra-long desalination stability up to 720 h. The enhanced performance can be attributed to the synergistic effect of the confined interlayer spacing and surface electrostatic repulsion. Overall, this work provides attractive strategy to fabricate fine-tuning 2D laminate nanochannels for high efficiency of desalination application.