Existing polyamide (PA) membrane synthesis protocols are underpinned by controlling diffusion-dominant liquid-phase reactions that yield subpar spatial architectures and ionization behavior. We report an ice-confined interfacial polymerization strategy to enable the effective kinetic control of the interfacial reaction and thermodynamic manipulation of the hexagonal polytype ( Ih ) ice phase containing monomers to rationally synthesize a three-dimensional quasilayered PA membrane for nanofiltration. Experiments and molecular simulations confirmed the underlying membrane formation mechanism. Our ice-confined PA nanofiltration membrane features high-density ionized structure and exceptional transport channels, realizing superior water permeance and excellent ion selectivity.
Although covalent organic frameworks (COFs) demonstrate notable potential for developing advanced separation membranes, contemporary COF membranes still lack controlled stacking and highly efficient sieving. Here, Turing-architecture COF membranes were constructed by engineering a reaction-diffusion assembly process via heterogeneous nucleation synthesis with tannic acid (TA). TA covalently binds with amine monomers to form a composite precursor with increased reactivity and decreased diffusivity. This altered the pathway of Schiff base reactions with aldehyde monomers, fulfilling suitable reaction-diffusion conditions, and ultimately formed the labyrinthine stripe or spot-patterned Turing COF film with controlled stacking and uniform pore structure. This endows our COF membrane with highly efficient molecule sieving ability for organic solvent nanofiltration while exhibiting a flux that is 621% greater than that of commercial membranes. Thus, this study provides a paradigm for the in situ synthesis of highly efficient COF membranes for diversely sustainable separations.
Nanofiltration membranes with confined nanopores are vital for energy-efficient molecular and ionic sieving towards sustainable ecosystems. However, the production of contemporary nanofiltration membranes still relies on hazardous petrochemical-based chemicals, raising serious water contamination concerns and complicating after-usage disposal. This phenomenon contradicts the sustainability of membranes derived from green chemistry principles, emphasizing not only their eco-friendly application but also their preparation and end of life. Here we report the synthesis of a sustainable nanofiltration membrane (SNFM) with superior performance for water treatment and an inherent natural soil degradation mechanism through a safer approach utilizing integrated low-hazard chemicals. Experiments and simulations confirmed that our SNFM can be fabricated in an environmentally friendly manner and decomposed by natural soil microorganisms, contributing to its distinctive eco-friendliness. Notably, the SNFM demonstrated both exceptional water permeance and molecular and ionic sieving capability, outperforming commercial and state-of-the-art membranes. This approach establishes a new paradigm for next-generation water recycling and sustainable chemical processes.