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To achieve greater separation performance and antifouling properties in a thin-film composite (TFC) nanofiltration membrane, cellulose nanocrystals (CNCs) were incorporated into the polyamide layer of a TFC membrane for the first time. The results of Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy (XPS) confirmed the successful formation of the CNC-polyamide composite layer. Surface characterization results revealed differences in the morphologies of the CNC-TFC membranes compared with a control membrane (CNC-TFC-0). Streaming potential measurements and molecular weight cutoff (MWCO) characterizations showed that the CNC-TFC membranes exhibited a greater negative surface charge and a smaller MWCO as the CNC content increased. The CNC-TFC membranes showed enhanced hydrophilicity and increased permeability. With the incorporation of only 0.020 wt % CNCs, the permeability of the CNC-TFC membrane increased by 60.0% over that of the polyamide TFC without CNC. Rejection of NaSO and MgSO by the CNC-TFC membranes was similar to that observed for the CNC-TFC-0 membrane, at values of approximately 98.7% and 98.8%, respectively, indicating that divalent salt rejection was not sacrificed. The monovalent ion rejection tended to increase as the CNC content increased. In addition, the CNC-TFC membranes exhibited enhanced antifouling properties due to their increased hydrophilicity and more negatively charged surfaces.

Traditional polyamide-based interfacial polymerized nanofiltration (NF) membranes exhibit upper bound features between water permeance and salt selectivity. Breaking the limits of the permeability and rejections of these composite NF membranes are highly desirable for water desalination. Herein, a high-performance NF membrane (TFC-P) was fabricated via interfacial polymerization on the poly­(vinyl alcohol) (PVA) interlayered poly­(ether sulfone) (PES) ultrafiltration support. Owing to the large surface area, great hydrophilicity, and high porosity of the PES–PVA support, a highly cross-linked polyamide separating layer was formed with a thickness of 9.6 nm, which was almost 90% thinner than that of the control membrane (TFC-C). In addition, the TFC-P possessed lower ζ-potential, smaller pore size, and greater surface area compared to that of the TFC-C, achieving an ultrahigh water permeance of 31.4 L m–2 h–1 bar–1 and a 99.4% Na2SO4 rejection. Importantly, the PVA interlayer strategy was further applied to a pilot NF production line and the fabricated membranes presented stable water flux and salt rejections as comparable to the lab-scaled membranes. The outstanding properties of the PVA-interlayered NF membranes highlight the feasibility of the fabrication method for practical applications, which provides a new avenue to develop robust polyamide-based NF desalination membranes for environmental water treatment.

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