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The robust correlation between the performance of thin-film composite (TFC) reverse osmosis membranes and the polyamide (PA) active layer determines the necessity of precise design of the PA layer, and this regulation primarily involves the surface morphology and internal characteristics of the PA layer. In this study, we fabricated honeycomb Turing structure or nanovoid-rich TFC series membranes using polar/nonpolar organic phase additives. Characterization and simulation results confirmed that the enhancement of membrane performance relied more on the abundant nanovoids within the PA layer rather than the ordered honeycomb lattice surface. Notably, the TFC-nDCE membrane with multilayer nanovoids exhibited an approximately 89 % improvement in water permeability while maintaining satisfactory salt rejection (98.29 %). We emphasized the significant role of nanovoids in the diffusion process of amine monomers and investigated the potential relationship between nanovoids and the degree of surface cross-linking. Building upon this, a new insight into the formation of nanovoids induced by PA anisotropic growth was presented through a careful analysis of the amine monomer diffusion rate and the morphological evolution of nanovoids. The structure-property relationship between internal structures, surface morphologies, and performances was systematically and thoroughly investigated, pointing out the direction for the rational design of TFC membranes. [Display omitted] • Revealed effects of nanovoids on the water/salt flow in honeycomb Turing PA layer. • Impacts of nanovoids on the physicochemical structure of PA layer were emphasized. • New insights on the anisotropic growth of PA were provided. [ABSTRACT FROM AUTHOR]

The separation performance of current organic solvent nanofiltration (OSN) membranes are still not satisfied. In this work, an ultra-thin TpHz covalent organic frameworks (COFs) interlayer was in situ constructed in advance on polyimide substrate, then an ultra-thin polyamide separation layer incorporated with amino-functionalized graphene quantum dots (af-GQDs) was constructed via interfacial polymerization (IP). A high performance interlayered thin-film nanocomposite (iTFN) OSN membrane with integrally covalent bonding structure, ultra-thin and ultra-smooth surface was obtained after post crosslinking and activation. The effect of ultra-low concentrations for the polyamide reaction monomers, the COFs monomer Tp and the doped af-GQDs nanoparticle reveals that they could help to form a very thin (7–8 nm in thickness) and defect-free skin layer with very smooth surface (about 2.7 nm in roughness). The iTFN OSN membrane shows excellent solvent permeance and solute selectivity, with an ethanol permeance reaching 97.6 L m−2 h−1 MPa−1 and an RDB rejection higher than 99%. After a 180 h long-term filtration with 100 mg L−1 RB/DMF solution, it remained an RB rejection of higher than 99%, demonstrating its superior resistance to strong polar solvent. Our work paves a unique way for the fabrication of novel OSN membrane with both in situ constructed nanomaterials interlayer and nanomaterials incorporated in skin layer. [Display omitted] • Integrally covalent iTFN OSN membrane has COFs interlayer and af-GQDs incorporated. • Ultra-thin TpHz COFs layer constructed in situ with ultra-low content of Tp and Hz. • Ultra-thin polyamide skin formed using ultra-low content for MPD, TMC and af-GQDs. • Ethanol permeance reaches 97.6 L m−2 h−1 MPa−1 with RDB rejection of above 99%. • The integrally covalent iTFN OSN membrane achieves superior solvent resistance. [ABSTRACT FROM AUTHOR]

We successfully fabricated a kind of novel sandwich-like thin-film nanocomposite (TFN) polyamide (PA) membranes via interfacial polymerization (IP) method on polyimide (PI) support surface which was modified by a layer of nanosized amine-modified zeolitic imidazolate framework - 8 (mZIF-8) nanoparticles for organic solvent nanofiltration (OSN). Uniform distribution of the nanoparticles was obtained via directly immersing the PI support membrane in aqueous mZIF-8 suspension prior to the IP. A post-IP cross-linking procedure was conducted to enhance further the solvent resistance of the fabricated TFN OSN membranes. Ultra-smooth (average surface roughness of 13.7 nm) and ultra-thin (average thickness of about 33 nm) skin layer was achieved, together with high Rhodamine B (RDB, 479 Da) rejection (99.1%) and reasonable ethanol permeance (~28 L m−2 h−1 MPa−1), as well as nearly unchanged RDB rejection after being submerged in DMF at high temperature (80 °C) for 120 h, indicating their very good resistance in very harsh strong polar solvent circumstance and the promising aspect of their industrial application. • The OSN membrane was fabricated with covalent bonding between layers. • The mZIF-8 interlayer helped to form an ultra-smooth and ultra-thin skin layer. • OSN membrane permeance was effectively increased without sacrificing rejection. • The OSN membrane kept super stability in DMF at 80 °C for 120 h. [ABSTRACT FROM AUTHOR]