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Thin-film nanocomposite (TFN) membrane based on polyamide (PA) chemistry was widely applied for water purification and desalination process due to the improved water permeance. It remains a great challenge to significantly enhance rejection because of the non-selective defects caused by the aggregation of nanomaterials in the PA layer. Novel interlayer-based TFN (iTFN) membrane containing nanomaterial interlayer between the porous substrate and PA layer is the promising candidate to improve PA integrity and thus overcome the ubiquitous trade-off between permeability and selectivity. The nanomaterial interlayer not only promotes the subsequent interfacial polymerization (IP) but also provides improved pathways for water transport, which leads to simultaneous improvement in membrane permeability and selectivity. This review systematically categorizes nanomaterial interlayers into three types according to construction methods, namely, direct deposition, in situ growth and functional group-anchored in situ assembly (FAISA). The mechanism of interlayer modulating IP process and PA structure, as well as the effects on water transport, are comprehensively analyzed. Encouraging results reveal that using MOFs interlayer prepared by FAISA is the most promising way to break the trade-off in manufacturing reverse osmosis membranes. Finally, challenges and future efforts are presented for advancing iTFN membranes. [Display omitted] • Recent advances in the porous nanomaterial interlayer enhanced iTFN membranes have been summarized. • Nanomaterial interlayers are categorized into three types according to the construction methods. • The effects of nanomaterial interlayer on interfacial polymerization and separation performance have been explored. • Functional group-anchored in situ assembly MOFs interlayer is a promising candidate to overcome the trade-off between membrane permeability and selectivity. • Challenges and future efforts of promoting nanomaterial interlayer-based iTFN membranes are proposed. [ABSTRACT FROM AUTHOR]

Nanofiltration (NF) membrane is of great significance for desalination of light brine and purification of drinking water. Although the development of novel preparation methods and membrane materials has improved the separation performance, it is still a major challenge to promote NF membrane toward industrial production with simpler and more controllable process. Herein, the polyphenol intermediate layer was designed by 5,5′,6,6′-tetrahydroxy-3,3,3′,3′-tetramethyl-1,1′-spirobisindane (TTSBI) with twist structure and polyethyleneimine (PEI) co-deposition to increase the surface hydrophilicity and electropositivity of the polysulfone ultrafiltration substrate. Subsequently interfacial polymerization (IP) was carried out on the polyphenol intermediate layer to assemble a polyamide ultrathin selective layer using trimesoyl chloride and piperazine monomer. Through adjusting the co-deposition time of TTSB and PEI, a unique nano-pleated structure was successfully formed on the thin-film composite membrane surface. The water permeance of the membrane was determined as 23.7 L m−2 h−1 bar−1 with 99.4% Na 2 SO 4 rejection, which was almost triple fold of the flux of the controller membrane without the intermediate layer. Our results provide an efficient and convenient way to fabricate the advanced NF membrane with higher divalent/monovalent ion selectivity and water permeance simultaneously, which will provide advices for the gas separation and pervaporation membranes with the IP method. • Novel TTSBI-PEI interlayer-based polyamide membrane was fabricated by interfacial polymerization. • The nano-pleated structure on the selective layer improved the water flux without deterioration of Na 2 SO 4 rejection. • The novel nanofiltration membrane exhibited excellent long-term stability. [ABSTRACT FROM AUTHOR]