High performance mixed-dimensional assembled MXene composite membranes for molecular sieving

Two-dimensional (2D) separation membranes have proved their superiorities in addressing global water scarcity and recycling resources. However, current 2D membranes usually suffer from swelling and irregular stacking issues, which result in poor separation performance. Herein, we developed novel mix-dimensional assembled MXene composite membranes with high permeability and selectivity by intercalating 1D carboxylated cellulose nanofibers (CNFs) into 2D lamellar MXene nanosheets. The effects of chain length of CNFs and MXene/CNFs mass ratios on the morphologies, physicochemical properties, and separation performances of composite membranes were systematically investigated. The optimized MXC-3-L membrane exhibited superior rejection to Congo red (CR, >99%) and remarkable separation efficiency of dye/salt. The separation factors for the CR/NaCl and CR/Na2SO4 mixtures were 512.0 and 517.2, respectively. Moreover, the MXC-3-L membrane showed distinct rejections to perfluoroalkyl substances (PFAS) (>95%) with a nearly 8-fold increase of permeance in comparison with the commercial polyamide membrane. The 2D X-ray diffraction analysis verified that the intercalation of 1D CNFs into 2D MXene nanosheets via strong hydrogen bonding can regulate the nanochannel into more stable and regularly stacking lamellar structures, which plays a key role in high permeance and excellent molecular separation efficiency. In addition, 1D CNFs play an essential role as "threading" and "stitching", shielding the defects between adjacent MXene nanosheets and improving the separation efficiencies. Our work provides new insights into design of defect-free and highly selective 2D materials-based membranes for enhanced wastewater treatment and molecular sieving.